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Ceramic Lasers 1st Edition Akio Ikesue Digital Instant
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Author(s): Akio Ikesue, Yan Lin Aung, Voicu Lupei
ISBN(s): 9780521114080, 052111408X
Edition: 1
File Details: PDF, 21.57 MB
Year: 2013
Language: english
more information - www.cambridge.org/9780521114080
CERAMIC LASERS

Until recently, ceramic materials were considered unsuitable for optics due to the numerous
scattering sources, such as grain boundaries and residual pores. However, in the 1990s the
technology to generate a coherent beam from ceramic materials was developed, and highly
efficient laser oscillation was realized. In the future, the technology derived from the
development of the ceramic laser could be used to develop new functional passive and
active optics.
Co-authored by one of the pioneers of this field, the book describes the fabrication tech-
nology and theoretical characterization of ceramic material properties. It describes novel
types of solid lasers and other optics using ceramic materials to demonstrate the application
of ceramic gain media in the generation of coherent beams and light amplification. This
is an invaluable guide for physicists, materials scientists and engineers working on laser
ceramics.

akio ikesue is the President of World-Lab. Co., Ltd. He is also an executive scientist at
SCHOTT AG, Germany, and an invited professor at ENSCP (Ecole Nationale Supérieure
de Chimie de Paris).
yan lin aung is a Senior Researcher at World-Lab. Co., Ltd. His research focuses on
opto-ceramics.
voicu lupei is a Professor at the National Institute for Laser, Plasma and Radiation
Physics in Bucharest, Romania. His research interests are in photonic materials, quantum
electronics processes in doped laser materials, and applications of solid-state lasers.
CERAMIC LASERS

A K I O IK E S U E
World-Lab. Co., Ltd, Japan

YA N L IN AUNG
World-Lab. Co., Ltd, Japan

VO I C U L U P E I
National Institute for Laser, Plasma and Radiation Physics,
Romania
cambridge university press
Cambridge, New York, Melbourne, Madrid, Cape Town,
Singapore, São Paulo, Delhi, Mexico City
Cambridge University Press
The Edinburgh Building, Cambridge CB2 8RU, UK
Published in the United States of America by Cambridge University Press, New York

www.cambridge.org
Information on this title: www.cambridge.org/9780521114080


c A. Ikesue, Y. L. Aung, V. Lupei 2013

This publication is in copyright. Subject to statutory exception


and to the provisions of relevant collective licensing agreements,
no reproduction of any part may take place without the written
permission of Cambridge University Press.

First published 2013

Printed and bound in the United Kingdom by the MPG Books Group

A catalog record for this publication is available from the British Library

Library of Congress Cataloging in Publication data


Ikesue, Akio, 1958–
Ceramic laser materials / authors, Akio Ikesue, Yan Lin Aung, Voicu Lupei.
pages cm
Includes index.
ISBN 978-0-521-11408-0 (hardback)
1. Laser materials. 2. Ceramic materials. I. Title.
TA1677.I44 2013
621.36 6 – dc23 2012042974

ISBN 978-0-521-11408-0 Hardback

Cambridge University Press has no responsibility for the persistence or


accuracy of URLs for external or third-party internet websites referred to
in this publication, and does not guarantee that any content on such
websites is, or will remain, accurate or appropriate.
Contents

Preface page ix
Acknowledgement xii
1 Introduction 1
1.1 Research background 1
1.2 Technical problems of melt-growth single crystals 2
1.3 Technical problems of ceramics 7
1.4 Purpose of this research 11
1.5 Outline of the book 12
References 16
2 Solid-state laser processes and active materials 18
2.1 Interaction of quantum systems with electromagnetic radiation
(radiation absorption and emission processes in quantum systems) 18
2.2 Solid-state lasers 25
2.3 The flow of excitation inside the laser material 63
2.4 Laser emission processes 67
2.5 The spatial distribution of the de-excitation processes 82
2.6 Thermal field inside the pumped laser material and thermal effects 85
2.7 Performance scaling of solid-state lasers 91
2.8 The laser material 93
References 115
3 Experimental technique: powder characteristics and the synthesis of optical
grade ceramics, effects of sintering aids 121
3.1 Introduction 121
3.2 Microstructure and optical characteristics of Nd:YAG processed by HIP
(hot isostatic pressing) 142
References 158
4 Synthesis of polycrystalline ceramic lasers (RE-doped sesquioxides) 160
4.1 Current status of single crystal technology 160
4.2 Requirements for sesquioxide ceramic lasers 162

v
vi Contents

4.3 Synthesis of optical grade sesquioxide ceramics 169


4.4 Optical quality and laser performance 176
References 185
5 Synthesis of RE (Nd) heavily doped YAG ceramics 187
5.1 Production of heavily doped Nd:YAG and lasing characteristics 188
5.2 Effect of impurity (Si) on Nd solid-melt in YAG ceramics 204
References 218
6 Optical scattering centers in polycrystalline ceramics 219
6.1 Introduction 219
6.2 Experimental procedure 220
6.3 Results 223
6.4 Discussion 234
6.5 Summary 239
References 240
7 Advanced technologies in ceramics (composite, fiber, single crystal by
sintering method, etc.) 241
7.1 Composite technology 243
7.2 Ceramic fiber laser 252
7.3 Single crystal ceramics produced by sintering 255
7.4 Summary 265
References 265
8 Current R&D status of ceramic lasers worldwide 267
8.1 Garnet system materials 268
8.2 Perovskite system materials 273
8.3 Non-oxide system (II–VI compound) materials 275
8.4 Fluoride system materials 277
8.5 Applications in the fields of biotechnology and medical technology 279
8.6 High intensity lasers for engine ignition 282
8.7 Investigation of solid-state lasers as solar pump lasers 285
References 288
9 The future of ceramic technology 290
References 298
10 High resolution optical spectroscopy and emission decay of laser ceramics 300
10.1 Structural characterization of doped ceramics by optical spectroscopy 301
10.2 The quantum states of the doping ions 321
10.3 Radiative and non-radiative de-excitation processes 345
10.4 Distribution of the doping ions in ceramics 358
10.5 Conversion of excitation in doped ceramics 360
10.6 Conclusions from high resolution optical spectroscopy of laser ceramics 370
References 372
Contents vii

11 Ceramic lasers 386


11.1 Pumping schemes 386
11.2 Radiative and non-radiative processes in ceramics 392
11.3 Ceramic laser materials and components 401
11.4 Ceramic lasers 403
11.5 Concluding remarks: the state of the art and directions of development
of ceramic lasers 424
References 427
Index 442
Preface

Research and development on various types of solid-state laser has been carried out since
the creation of the first ruby laser by Dr. T. H. Maiman in 1960 [1]. Examples of laser
technologies include continuous wave (CW) lasers using Nd:YAG (neodymium-doped
yttrium aluminum garnet) single crystals at room temperature developed by Dr. Geusic
in 1964 [2], and tunable and ultra-short pulse lasers using Ti:sapphire single crystals
developed by P. F. Moulton in 1982 [3]. These lasers are still being applied in industrial
applications.
On the other hand, it is said that people started to use porcelain (ceramic ware) as standard
tableware in the days before Christ. In the USA, modernization of ceramic technology
started in the 1950s. Ceramics have now become an essential part of technologies that
support industries such as electronics and engineering etc., and their industrial use has
expanded greatly from year to year.
The interaction of ceramics with optics originated from the success that was achieved by
Dr. R. L. Coble of MIT (Massachusetts Institute of Technology) in the late 1950s [4]. He
succeeded in fabricating alumina ceramics including fewer residual pores by controlling the
microstructure. This material exhibited translucency (i.e., diffused transmission, not in-line
transmission throughout the specimen), and was applied as a discharge tube in a high-
pressure sodium vapor lamp, thus contributing to the advancement of lighting technology.
Research and development of various types of translucent and transparent ceramics then
occurred around the world, but the optical quality of the translucent ceramics was much
inferior to that of commercial single crystal and glass materials. In addition, there were no
practical applications of these ceramics at that time, and most of the translucent ceramics
were only of interest for laboratory research.
The development of transparent ceramic materials for applications in laser oscillation
is an ultimate aim of materials technology. It is also a dream of materials scientists in
the field of ceramics to develop ceramic (polycrystalline) materials which can be used
for laser oscillation with a performance equal to or better than that of conventional single
crystal materials. The first two attempts were from the USA, where laser oscillation using
Dy:CaF2 ceramics under cryostatic conditions was reported in 1964 [5], and pulse laser
oscillation using Nd:ThO2 –Y2 O3 ceramics was reported in 1973 [6]. Both succeeded in
producing laser oscillation using ceramic materials, but the laser performance was very

ix
x Preface

poor even though the ceramic samples were fabricated using the most advanced technology
at that time. Almost two decades passed until the next attempt was made in 1995 (by
the author) to produce efficient laser oscillation using ceramic materials [7], selecting
Nd:YAG, which is a technologically and industrially important material in the field of
solid-state lasers. It was demonstrated that polycrystalline Nd:YAG ceramics can be used
for CW laser generation with an efficiency comparable to that of commercial single crystal
lasers. Microchip lasers [8] and single mode laser oscillation [9] were achieved using
heavily doped Nd:YAG ceramic, and the excellent performance of ceramic lasers was
demonstrated. The importance of ceramic lasers began to achieve recognition worldwide
from 2000, and nowadays research and development of ceramic lasers is being carried
out around the world. Moreover, the development of new optical materials in addition to
Nd:YAG ceramics was initiated by applying the technology to make highly transparent
ceramics.
The ceramic laser changed completely the common concept of the conventional solid-
state laser. It was possible to fabricate polycrystalline ceramic laser gain media with
extremely low scattering and optical homogeneity, which cannot be obtained with commer-
cial single crystals. In addition, ceramic technology permits the fabrication of composite
laser elements with extremely complicated structures to improve the laser performance
[10], and the fabrication of fiber laser elements to generate high beam quality lasers. In this
sense, ceramic lasers can provide a broad range of design flexibility for the enhancement of
laser performance compared to traditional single crystal lasers. New laser materials, which
are difficult to obtain using the conventional melt-growth technology, such as Sc2 O3 and
Y2 O3 , can be fabricated by advanced ceramic processing, and high laser performance from
such sesquioxide ceramics has been confirmed [11]. It is predicted that ceramic lasers will
play a major role in solid-state lasers in the future, and will have applications in many
industrial fields.
It is interesting that the author successfully produced a highly efficient ceramic laser
even though he was not an expert in the field of ceramics or lasers at that time, but was
engaged in the research and development of refractory materials. The readers may question
(1) why the author focused on the development of ceramic lasers and (2) how the author
managed to achieve technological success. Regarding the first question, it is normally the
dream of a researcher to make a breakthrough in the development of the most difficult
materials theoretically and technologically, and this was the best opportunity for the author
to realize a contribution to ceramic technology. Regarding the second question, to be
honest, at that time the author did not actually know about the special (strict) requirements
(demand characteristics) of laser materials, and that is why he could perform such a reckless
exploration of laser generation using ceramic materials. Therefore, even an engineer who
does not know the materials technology may well open the door to new technologies if he
or she has a challenging spirit and can keep the dream alive as an engineer. “Challenging
nothing for fear of failure might be the biggest risk for a scientist.”
In this preface, the development of ceramic lasers has been described briefly. In this
book, a wide range of topics is described, from the fabrication technologies of ceramic
Preface xi

lasers, which are expected to be used in the development of future solid-state lasers, to their
performance.

References
[1] T. H. Maiman, Stimulated optical radiation in ruby, Nature (London) 187 (1960)
493–494.
[2] J. E. Geusic, H. M. Marcos, and L. G. van Uitert, Appl. Phys. Lett. 4 (10) (1964)
182–184.
[3] P. F. Moulton, Opt. News 8 (6) (1982) 9.
[4] R. L. Coble, Am. Ceram. Soc. Bull. 38 (10) (1959) 501.
[5] S. E. Hatch, W. F. Parson, and R. J. Weagley, Appl. Phys. Lett. 5 (1964) 153.
[6] C. Greskovich and J. P. Chernoch, J. Appl. Phys. 44 (10) (1973) 4599–4605.
[7] A. Ikesue, T. Kinoshita, K. Kamata, and K. Yoshida, J. Am. Ceram. Soc. 78 (4) (1995)
1033–1040.
[8] I. Shoji, Y. Sato, T. Taira, A. Ikesue, and K. Yoshida, Highly Nd3+ -doped YAG
ceramic for high power microchip, CGCT-1, 2000/Abstract Book, T-C-05 (2000),
pp. 345–355.
[9] A. Ikesue, Yan Lin Aung, T. Taira, T. Kamimura, K. Yoshida, and G. L. Messing,
Progress in ceramic lasers, Mater. Res. Annu. Rev. 36 (2006) 397–429.
[10] A. Ikesue and Yan Lin Aung, Synthesis and performance of advanced ceramic lasers,
J. Am. Ceram. Soc. 89 (6) (2006) 1936–1944.
[11] A. Ikesue, K. Kamata, and K. Yoshida. Synthesis of transparent Nd-doped HfO2 –Y2 O3
ceramics using HIP, J. Am. Ceram. Soc. 79 (2) (1996) 359–364.
Acknowledgement

This research and development effort was started when the author was working in a refrac-
tory manufacturing industry (Kurosaki Harima Corporation) as an engineer. Support from
the members of Kurosaki Harima Co. for research up to the present date is greatly appre-
ciated. The authors are very thankful to collaborators around the world for their supportive
collaboration: Professor Y. Iwamoto (Nagoya Institute of Technology), Associate Profes-
sor T. Kamimura (Osaka Institute of Technology), Associate Professor T. Taira (Institute
of Molecular Science) and Associate Professor T. Yamamoto (Tokyo University) from
Japan, and Dr. A. Lupei (Romania) and Dr. Yvonne Menke (SCHOTT AG, Germany) from
Europe, and Dr. R. Shori (UCLA), Dr. J. Sanghera (Naval Research Laboratory) and Dr. M.
Dubinsky (Army Research Laboratory) from the USA. Also, the authors greatly appreciate
support and useful advice from Dr. Joan Fuller, Dr. K. Jata and Dr. K. Goretta of AFOSR
(Air Force Office of Scientific Research)/AOARD (Asian Office of Aerospace Research
and Development) for the development of the “high power density laser.”

xii
1
Introduction

1.1 Research background


There are many scientific, military, medical and commercial laser applications which have
been developed since the invention of the laser in the 1960s [1–11]. It is clear that the laser
is essential for optical communication, nowadays part of the optoelectronics industry. This
industry is growing continuously and rapidly in scale and is comparable to the automobile,
electronics, and the semiconductor industries. Lasers can be classified generally into four
groups depending upon the type of gain medium: (1) semiconductor lasers, (2) gas lasers,
(3) liquid (dye) lasers, and (4) solid-state lasers. (1) Semiconductor lasers are used as
optical sources for optical communication, and read/write systems in recording media
(optical disks, magneto-optical disks etc.). (2) One gas laser is the He–Ne laser which
is used as an optical source for measurements in basic research because of its low cost.
Excimer lasers are used as optical sources for etching in CVD (chemical vapor deposition),
and for lithography. CO2 lasers have many industrial applications such as laser cutting and
welding. (3) Dye lasers use an organic dye as the gain medium. The wide gain spectrum of
available dyes allows these lasers to be highly tunable, or to produce very short duration
pulses on the order of a few femtoseconds. (4) Typical solid-state lasers are the glass lasers
applied in nuclear fusion reactors, and YAG lasers used in mechanical processing and
medical applications etc.
The discoveries of the ruby laser by Maiman in 1960 [1, 12] and of the YAG laser by
Guesic et al. in 1964 [2] led materials scientists to develop a variety of solid-state laser
materials including crystalline and non-crystalline materials. For instance, garnet materials
such as GGG (Gd3 Ga5 O12 ), GSGG (Gd3 Sc2 Ga3 O12 ) and YSGG (Y3 Sc2 Ga3 O12 ) [13–20],
fluoride materials such as CaF2 and MgF2 [21], alexandrite materials [22–24], synthetic
forsterite materials, and YVO4 [25–29], and amorphous materials such as silicate glasses
containing Rb, K and B [30, 31] were successfully developed. The basic requirements of
the physical properties of solid-state laser materials are a high thermal conductivity, high
chemical stability, and excellent machining properties. In addition, the laser gain materials
must have a large cross-section of stimulated emission (σ ) and long fluorescence lifetime
(τ ). Moreover, the laser threshold of the materials must be as low as possible, and stable
laser oscillation in CW (continuous wave) or pulsed mode must be obtainable with a high

1
2 Introduction

energy conversion efficiency. The material that satisfies these demand characteristics is
YAG, which occupies the majority of the solid-state laser market. It is not likely that there
will be new materials in the future that can exceed the performance of YAG materials in
terms of physical properties and laser characteristics. However, almost all of the materials
used for solid-state lasers, including YAG, are single crystals produced by the melt-growth
process. Initially, single crystals were produced by the Verneuil process, also called flame
fusion [2], but because of quality issues in terms of laser amplification efficiency and
laser beam quality, crystals grown by the Cz (Czochralski) process are now being used
in industrial applications [32]. However, it takes about one month to grow an undoped
YAG single crystal with a relatively large diameter, and it takes longer to grow an Nd:YAG
single crystal. In addition, the optically homogeneous portion of the single crystal ingot
which is suitable for laser oscillation is very limited because of the intrinsic core and facets.
Therefore, the productivity and output characteristics are still unsatisfied from an industrial
point of view.
Therefore, it was considered that if it were possible to produce YAG laser materials using
ceramic technology, the above technical issues of single crystal YAG materials could be
solved, but a weak point was that the grain boundaries in ceramics can disturb the efficient
amplification of the coherence beam in the materials. This weak point was reflected in
the results achieved from Dy:CaF2 ceramics in 1964 and from Nd:ThO2 –Y2 O3 ceramics
in 1974. Although laser oscillation was demonstrated using these ceramic materials, the
resulting beam quality and lasing efficiency were not sufficient for the development of
ceramic materials as laser gain media in the future. However, this negative opinion changed
abruptly with the successful demonstration of a highly efficient polycrystalline Nd:YAG
ceramic laser at room temperature by the author in 1995. The author demonstrated that
ceramic materials can show laser performance equivalent to that demonstrated for single
crystal laser gain media and, moreover, ceramic lasers have potential which cannot be
realized with conventional single crystal lasers. Nowadays, the optical quality of polycrys-
talline ceramic laser gain media is comparable to that of the high quality commercial single
crystal counterparts, and further technological progress is expected in the future.

1.2 Technical problems of melt-growth single crystals


As described above, single crystal YAG materials are mainly used in solid-state lasers
and almost all of the YAG laser gain media are produced by the Cz method (melt-growth
process). Transition metal elements (Cr, Ti etc.) or lanthanide rare earth elements (Nd,
Tm, Ho etc.) are doped as laser active ions in the YAG host material. Among these laser
active ions, Nd is a four-level laser system, with narrow spectral width and high quantum
efficiency. Therefore, Nd-doped YAG has become the most important laser material.
Figure 1.1 shows the principle of laser action in the Nd3+ ion. The Nd3+ ion has three
fluorescent emissions: (1) 0.9 µm (4 F3/2 → 4 I9/2 ), (2) 1.06 µm (4 F3/2 → 4 I11/2 ) and (3)
1.3 µm (4 F3/2 → 4 I13/2 ), and the radiative transition possibilities of each state are 0.25,
0.60 and 0.15, respectively [33, 34]. Emission (2) has the highest energy efficiency, and
1.2 Technical problems of melt-growth single crystals 3

20

Exciting Level
16

R2
11502cm-1 Upper Level
Energy [×103 cm-1]

4F
3/2 11414
4F R1
4F 5/2 Laser Transition
12 3/2

1.6 μm 4I ~6000
Laser Transition 15/2

8
4I ~4000
4I 13/2
15/2
2526
4I 2473
4 13/2 4I 2146
11/2 2111
2029 Lower Level
4I 2001
11/2

4I 848
9/2 4I
0 Ground Level 9/2 311
197
134
0

Figure 1.1 Energy diagram for Nd3+ ions in YAG crystal.

normally Nd:YAG crystals are used for 1.06 µm generation. To obtain laser action in
Nd:YAG materials, first the electrons of Nd ions in the ground state are excited with a
xenon or krypton lamp (white light source from a discharge flashlamp) so that the electrons
are pumped up to energy levels higher than 4 F3/2 . More recently, a semiconductor laser (LD,
laser diode) with a certain wavelength has been used to pump the ground state electrons
directly to the 4 F5/2 band. Accordingly, these excited electrons which are in the upper levels
decay rapidly to the 4 F3/2 level (non-radiative transition), and then when these electrons are
transferred to 4 F13/2 , 4 F11/2 and 4 F9/2 , three fluorescent emissions (radiative transitions) (λ =
0.9, 1.06 and 1.3 µm) occur. Then the fluorescent emission is amplified in a set of mirrors
(the resonator), and finally an intensified light with a single wavelength (monochromatic
light) is emitted. In the Nd system, when electron transitions occur from the upper levels
to the 4 F3/2 level on exciting with a lamp source, the transitions are non-radiative and the
energy is released as heat. Therefore, effective laser oscillation cannot be achieved using
a lamp excitation system. (However, a high output power can be achieved using a lamp
excitation system because the lamp can provide very high input power to the laser gain
medium.) In the LD excitation system, laser diodes of wavelengths 808 nm or 885 nm
are used which can pump the ground state electrons directly to upper levels, 4 F5/2 or 4 H3/2
levels. Therefore, there are no excited electrons which undergo non-radiative transitions as
seen in the lamp excitation system, and efficient laser oscillation can be achieved. However,
4 Introduction

Gas

Seed Crystal :<111> YAG

Ir Crucible

Induction Coil
Melted YAG

Zirconia Refractory

Zirconia Powder

Figure 1.2 Schematic diagram of a YAG single crystal grown by the Czochralski method.

it was difficult to obtain high power LDs, and low power models were also very expensive.
Therefore, the lamp excitation system was common for solid-state lasers. In the twenty-first
century, the price of high performance LDs is becoming more reasonable, and recently a
highly effective compact and high power (kilowatt range) Nd:YAG laser system with LD
pumping has been commercialized. But, a technical issue of the LD excitation source is
that the wavelength of the LD is shifted when its temperature is increased during laser
operation. It is necessary to control the temperature of the main body of the LD and the
spectral width of the emission band of the LD.
As described in Section 1.1, the Cz method is commonly used to produce YAG single
crystals (see Figure 1.2). High purity raw materials (over 4N, 99.99 mass%) of Y2 O3 , Al2 O3
and Nd2 O3 are used. They are weighed in the YAG stoichiometric ratio, and blended. Then
the blended powders are pressed into powder compacts and sintered. This relatively dense
Nd:YAG sintered body is put into an Ir (iridium) crucible, and melted by high frequency
induction heating at over 1950 ◦ C. Then a YAG seed crystal is placed on top of the YAG
melt, and the growing crystal is continuously pulled very slowly at a rate of 0.2 mm h−1 with
a rotation speed of 10–30 rpm. Normally, a YAG seed crystal with an orientation of 111
is used because it has the largest surface energy, but in some cases, 110 and 100 seeds
are also used. When Nd ions are doped into a YAG crystal, Nd replaces Y sites in the garnet
structure. However, the ionic radius of the Nd ion is much larger than that of the Y ion, and it
is well known that Nd hardly dissolves in YAG crystal. The segregation coefficient of the Nd
ion in YAG crystal (the ratio of the Nd concentration in the crystal to the Nd concentration
in the melt) is very small, about 0.2 [35]. Therefore, a highly doped Nd:YAG sintered body
is prepared in advance to produce a YAG melt with 2–3 times higher Nd concentration
than the target Nd concentration. (For instance, suppose the target composition is 1 at.%
1.2 Technical problems of melt-growth single crystals 5

Nd:YAG, then sintered bodies of 2 or 3 at.% Nd:YAG are prepared in advance, and they
are melted and grown to obtain a crystal of 1 at.% Nd:YAG.) Although, high concentration
Nd:YAG melts are prepared in advance, it is not certain that the grown crystal will have a
high Nd concentration with homogeneous doping. When the Nd concentration in YAG is
higher than 1 at.%, many inclusions (light scattering sources) are generated in the crystal,
and it cannot be used as a laser crystal. Therefore, the concentration of Nd ions is limited
to 1 at.% in YAG single crystals for laser applications. Even a 1 at.% Nd:YAG crystal
ingot includes optically inhomogeneous parts such as the core and (211) facets from the
pulling axis towards the rim area [35]. Accordingly, only a part (the optically homogeneous
part) of the grown crystal can be used as a laser gain medium. Another technical issue
with melt-growth crystals is that the Nd concentration varies slightly in the longitudinal
direction of the ingot. This is because when the crystal is pulled, the concentration of Nd
ions in the grown crystal is significantly lower than that in the melt. Thus, Nd ions are
concentrated in the melt as the crystal growth progresses. Therefore, the Nd concentration
in the grown crystal at the early stage of crystal growth (near the seed crystal) is slightly
lower compared to the middle stage and terminal stage (the end of the ingot) along the
longitudinal direction of the crystal ingot. As a result, this process produces a crystal rod
which has a change in refractive index at each end. This is the technical limitation of the
conventional melt-growth method.
A polarized image of approximately 1 at.% Nd:YAG single crystal (ingot), a Schlieren
image and X-ray tomography image are shown in Figure 1.3(a), (b) and (c), respectively
[35]. All of the images (especially the cross-sectional images) show crystal defects (such
as core and facets) in the crystal ingot. A commercial Nd:YAG slab and polarized images
(cross-nicol) are shown in Figure 1.3(d) and (e, f ), respectively. The commercial Nd:YAG
single crystal has very high transparency, and it looks optically very homogeneous to the
naked eye (under natural light). However, when it is observed under a polarizer, lamella
shaped facets can be seen across the length direction of the slab, suggesting that even the
commercial high quality single crystal materials include such optically inhomogeneous
components.
Any optical defects remaining in a laser gain medium can significantly reduce the light
amplification efficiency and beam quality. Therefore, the demand characteristics for laser
materials are necessarily very strict. Regarding quality control in commercial single crystal
production, the thermal stress and refractive index distribution of the grown Nd:YAG ingot
are inspected using a polarizer and interferometry. Optically homogeneous parts of the
ingot are cut off and polished, and then the numbers of optical scattering centers in the
samples are detected using a laser system. Finally, the most optically homogeneous part is
selected as a high quality laser gain medium.
The optical loss of commercial high quality Nd:YAG single crystal is in the region of
0.2% cm−1 , and the quality has improved significantly compared with the crystal grown
by the Bernoulli process in 1964. In fact, the melt-growth single crystal technology has
reached its limits, and it is extremely difficult to improve further the quality of current
single crystal materials.
6 Introduction

(a) (b) (c)

(d)

(e) (f)

Figure 1.3 Cross-section of an Nd:YAG single crystal imaged by (a) polarizing light, (b) the Schlieren
method (interferometry image), and (c) X-ray tomography. (d) Appearance of a commercial single
crystal Nd:YAG slab, and (e, f ) polarized images (open and cross-nicol) under a polarizer.

To grow a YAG crystal, a very expensive Ir crucible and growth unit is necessary. What
is worse is that the growth rate is very slow. Normally it takes about one month to grow
an ingot. Other economic issues are the very high initial costs of the fabrication equipment
and running costs for a long delivery time (electricity, and recovery costs for the Ir crucible
etc.). In addition, the yield percentage of high quality laser crystal is very low. There are
also technological issues. Only a small cross-section rod can be achieved. The diameter
of the ingot is limited to 5–6 inches, and a laser rod with approximately 10 mm diameter
by 150 mm length or a laser slab of approximately 6 × 20 × 150 mm3 can be removed
1.3 Technical problems of ceramics 7

from the ingot. Therefore, large gain media for the future development of high power lasers
cannot be produced by the current melt-growth crystal technology.
As described above, generally YAG has many advantages compared to other laser mate-
rials. However, the most important part in the laser system is the Nd:YAG material, and
there are still many unsolved economic issues (including yield percentage) and technolog-
ical issues. It is technologically almost impossible to achieve a breakthrough in the current
single crystal growth process, and even a partial solution to the problems appears far
away.

1.3 Technical problems of ceramics


Regarding translucent ceramics, Dr. R. L. Coble first developed translucent alumina ceram-
ics in 1959 [4, 36], and then this material was used as a discharge tube in a high pres-
sure sodium vapor lamp. Polycrystalline ceramics were thought to be opaque until Coble
demonstrated experimentally that ceramics can transmit light when the bulk density is
increased to very near the theoretical density by reducing the number of residual pores
during the sintering process. Later, by controlling the purity, particle size and homogeneity
of the starting raw materials, and by improving the traditional sintering process according
to sintering theory, it was possible to manufacture high purity and high density ceramics
with controlled microstructure. With a history of over 20 years, translucent and transparent
ceramics composed of simple oxides such as MgO, Y2 O3 and ZnO and multiple oxides
such as ZrO2 –Y2 O3 and spinel (MgO–Al2 O3 ) and recently PLZT ((PbLa)(ZrTi)O3 ), SBN
((SrBa)Nb2 O6 ) using the electro-optical effect, Gd2 O2 S:Pr and (YGd)O3 :Eu for X-ray scin-
tillators and highly thermally conductive ceramics (AlN) have been developed [37–42], and
some of them have been commercialized.
However, up to now translucent ceramics have been developed for applications requiring
only thin shapes, and have not been produced for high optical quality applications. There-
fore, there was no published account of an optical ceramic with high optical quality until the
transparent polycrystalline Nd:YAG ceramics developed by the author in 1995. In fact, the
optical quality of conventional high quality translucent ceramics, which include many grain
boundaries, was significantly inferior to that of commercial single crystals. For that reason,
most of the published papers discussed mainly the optical quality and applications of thin
transparent ceramics. For instance, in the case of alumina, which belongs to the hexagonal
crystal system, the transmittance of 1 mm thick normal sintered ceramic is considerably
lower than that of hot-pressed translucent alumina ceramic or single crystal sapphire (see
Figure 1.4) [43]. Since the thickness of all materials was set at 1 mm in this experiment,
when the transmittance is plotted with the thickness of each sample in accordance with
the Lambert–Beer law, it can be seen that the slopes of the lines for single crystal and
polycrystalline ceramics are considerably different, i.e., the scattering characteristics of
the materials are different. The slope of the lines gives the optical attenuation coefficient
(optical loss). This value was significantly larger even in the cases of transparent MgO or
spinel ceramics which belong to the cubic crystal system. For these reasons, translucent
8 Introduction

100
Al2O3 single crystal

80

Transmittance (%)
60
Al2O3 ceramics (Hot press)

40

Al2O3 ceramics
20

0
0.4 0.6 0.8 1.0 1.5 2.0 2.5
Wavelength (m)
Figure 1.4 Relationship between measured wavelength and in-line transmittance for sapphire single
crystal, hot-pressed Al2 O3 ceramic, and Al2 O3 ceramic produced by normal pressure sintering.

Figure 1.5 Illustration of optical scattering in polycrystalline ceramics due to various microstructural
defects: (a) grain boundary, (b) residual pore, (c) secondary phase, (d) birefringence, and (e) surface
roughness.

ceramics were mainly used for applications requiring a thin slice shape in the technology
of the twentieth century.
Figure 1.5 illustrates the microstructure and scattering sources of normal translucent
ceramics [44]. The ceramic is composed of many fine grains (crystallites) with randomized
crystal orientations. Scattering sources in normal ceramics are (a) grain boundaries,
(b) residual pores, (c) inclusions and secondary phases, (d) birefringence and double
reflections, and (e) surface roughness. However, the fundamental differences in microstruc-
ture between single crystal materials and ceramic materials which affect the scattering
1.3 Technical problems of ceramics 9

Nd:YAG rod

Flashlamp Rod holder

Heat sink for O ring


laser rod
Slit for lamp
Cop of laser head

Cooling pipe for lamp

Window
Chamber (water cooling)
Reflection mirror (upper)
Reflection mirror (lower)

Figure 1.6 Schematic diagram of a commercial laser oscillator using a single crystal gain medium
and flashlamp excitation.

characteristics are (a) the present of grain boundaries, and (b) the quantity by volume
of residual pores. Accordingly, it is considered that these scattering sources significantly
influence the optical quality of ceramic materials.
On the other hand, it is true that laser crystals with very low scattering loss can have a
very high laser amplification efficiency. In fact, ultra low loss single crystals still cannot be
produced using the current crystal technology. The optical loss of high quality commercial
single crystals is around 0.3–0.2% cm−1 (some latest data show less than 0.2% cm−1 ), and
this quality can offer relatively efficient laser generation from commercial single crystals.
A schematic diagram of a commercial laser oscillator using a single crystal gain medium
and flashlamp excitation is shown in Figure 1.6 [45]. External energy (from a flashlamp
or semiconductor laser) is input into the laser gain medium (doped with fluorescent ions)
in order to excite the electrons continuously from the ground state to laser levels. Then,
the emitted fluorescent beams are reflected and amplified between two mirrors. The laser
beam quality and amplification efficiency are severely affected by the numbers of scattering
sources in the laser gain medium.
Previously reported papers on translucent ceramics have discussed few details of the
optical characteristics (optical constant), and there have been almost no reported papers
which have described the scattering loss, condition of double refraction and homogeneity
of the refractive index in ceramic materials. It can be considered that the scattering loss of
the translucent or transparent ceramics developed in the past was very high, and they could
not meet the requirements of laser materials.
However, one researcher, Dr. Greskovich of GE Co., developed a transparent Nd-
doped 10%ThO2 –Y2 O3 ceramic, and succeeded in producing laser oscillation at room
10 Introduction

Figure 1.7 Picture of Dr. C. D. Greskovich and microstructure of Nd:ThO2 –Y2 O3 ceramic.

temperature for the first time using a polycrystalline ceramic gain medium in 1973. (About
10 years before this, successful laser oscillation was achieved using Dy:CaF2 ceramic
under cryostatic conditions, but the details of the physical properties of the materials
were not described.) Dr. Greskovich succeeded in fabricating transparent Nd:ThO2 –Y2 O3
ceramic by sintering low sinterability Y2 O3 powder, with 10% ThO2 as a sintering aid, at
2200 ◦ C for about 100 hours.
Figure 1.7 shows reflection microscopy and transmission microscopy images of the 1%
Nd:ThO2 –Y2 O3 ceramic together with a picture of Dr. Greskovich [6, 46, 47]. Although
only a few residual pores are observed on the surface in the reflection micrograph, many
internal defects (such as voids and grain boundary phases) can be observed in the transmis-
sion micrograph. An optically inhomogeneous structure, called an “orange peel” structure,
can be seen with the naked eye. Although it was reported that the number of residual pores
in the Nd:ThO2 –Y2 O3 ceramic reached 10−5 –10−7 (10–0.1 ppm) in 1973, the optical loss
of the material was lower than several percent per centimeter. Because of this optical qual-
ity, pulse laser oscillation could be produced by flashlamp excitation at room temperature,
but the slope efficiency was as low as 0.1%. This technology was the best achieved in the
1.4 Purpose of this research 11

1970s, and the success of Dr. Greskovich encouraged materials scientists. However, there
was no challenger who could compete with this achievement for about 20 years.
Compared to normal optics for active and passive applications, the optical quality of the
single crystals required for laser application is significantly higher because light amplifi-
cation occurs in the gain medium, and the amplified light is passed repeatedly through the
gain medium. Therefore, even a small amount of optical loss of the material may have a
significant effect on laser oscillation. In the past, various types of translucent or transparent
ceramic materials have been developed. But it can be assumed that the scattering losses
of those materials were very large compared to the materials reported by Dr. Greskovich.
It was difficult to produce single crystal material with optical quality sufficient for laser
applications, and it was far too difficult to produce conventional translucent ceramics, which
include many crystal defects such as grain boundaries, residual pores and inclusions etc.,
which could meet the requirements for laser applications. For that reason, conventionally
it was doubted that ceramic materials could be used as laser gain media in the future of
solid-state lasers. If a technology existed which could remove microstructural defects per-
fectly (except grain boundaries) from ceramics, perhaps ceramic materials could be used as
optical materials in laser applications. This problem was not solved until the author demon-
strated high efficiency laser oscillation from a polycrystalline ceramic material. Details of
this development are described in this book.

1.4 Purpose of this research


Normally the output power of a solid-state laser is comparable to that of a gas laser (e.g.,
CO2 laser), and solid-state laser oscillators are very compact compared to gas lasers. There
are many disadvantages to using gas lasers. For instance, no waveguide system is available
in CO2 gas lasers. However, in the case of Nd:YAG lasers, the oscillation wavelength is
about 1 µm, and they can be used for optical fiber transmission systems. In addition, a high
output power can be achieved from a compact solid-state laser system.
The most important material for solid-state lasers is Nd:YAG, and the optical quality
of the Nd:YAG single crystal must be as high as possible, as mentioned before. In the
case of ceramic processing, powders (the powder composition is very close to or the
same as the target composition) prepared by a wet process such as the alkoxide method,
co-precipitation method, or homogeneous precipitation method etc. have generally been
used to obtain high performance ceramic materials. Using such wet processed powders,
there are many reports of advanced ceramics with very high homogeneity and density or
with transparent quality. However, the fabrication process is very complicated, and even the
ceramics prepared from wet processed powders did not have optical quality comparable to
that of the single crystal counterparts. The wet process was invented to overcome the
problems generally seen in the solid-state reactive sintering process, for example, the
formation of microstructural defects due to inhomogeneous blending of the powders,
remaining unreacted phases, compositional variation among grains, and lack of uniformity
of the grains. In the wet process, homogenization of the raw powder materials is performed
12 Introduction

at the formation of the host composition (e.g., garnet) step and calcination, in advance of
the sintering process. In principle, therefore, it is very effective for improving homogeneity
during the sintering process.
However, from another technical point of view, it can be considered that the wet process
was invented to avoid the above described problems of the dry process because the properties
of raw powder materials for the conventional dry process (solid-state reaction method) were
not good enough for the production of optical quality ceramics. Whether this speculation is
true or not hinges upon the fact that high optical quality ceramics can be produced by the dry
process, using good quality raw powder materials. In this research, therefore, we focused
on the solid-state reaction method without using synthesized raw powders prepared by the
wet process. If the dry process can overcome the above mentioned general technical issues,
it will become a very important industrial process for the economic production of optical
ceramics because the powder preparation process is very simple and the preparation of
powders with various compositions is very easy. Accordingly, the dry process was selected
for this study. The main objectives of this study are as follows:

(1) to produce a transparent polycrystalline Nd:YAG ceramic of optical quality by the


solid-state reaction method;
(2) to evaluate the optical quality of the ceramics produced, especially the laser oscillation
characteristics;
(3) to clarify the effect of the microstructure of the ceramics on the laser performance;
(4) to explore new functionalities unique to ceramics (technologies that cannot be obtained
using conventional single crystals);
(5) to figure out the technical problems involved in the fabrication of laser ceramics and to
provide a means for solving the problems.

1.5 Outline of the book


This study is based on the above five objectives, and comprises eleven chapters. Outlines
of the chapters are given here.
Chapter 2 introduces the main principles of solid-state lasers. After a brief description
of the interaction of electromagnetic radiation with quantum systems and of laser emission,
the three major components of the laser, the active laser material, the pumping system and
the laser resonator, are presented, with emphasis on their roles and characteristics. The
flow of excitation inside the pumped laser material is examined and it is shown that the
competition of laser emission with other de-excitation processes, such as luminescence
and non-radiative processes that generate heat, is determined by specific characteristics of
these three parts of the laser. It is thus determined that the development of solid-state lasers,
including optimization of the efficiency, use of new wavelength ranges, diversification of
the temporal regime of emission, and scaling to very high power or energy, requires specific
qualities of the laser material. From examination of the actual state of the art it is concluded
that the traditional laser materials, based on doped crystals or glasses, cannot support the
necessary development of lasers and new solutions must be looked for. Polycrystalline
1.5 Outline of the book 13

materials produced by ceramics techniques could be very promising in this development.


The ceramic laser materials combine some of the advantages of glasses (large size, high
optical uniformity and so on) with the qualities of crystals, adding new features such as
enhanced compositional versatility, enhanced doping concentrations, tight control of the
doping profile, possibility of producing composite materials and so on. Various classes of
ceramic materials are described and the main directions of research are outlined.
In Chapter 3, the sintering behavior of raw powder materials, Y2 O3 and Al2 O3 powders
prepared for this study and corresponding commercial powders used as starting materials
for the synthesis of transparent YAG ceramics, are compared. In addition, YAG sintered
bodies were prepared using these powder sources and their sintering behaviors were also
investigated. Based on these results, the reasons why transparent ceramics were not pro-
duced successfully by the conventional dry process are investigated. Because a normal
sintered body includes many residual pores which cause severe internal scattering, it is
necessary to reduce the amount of residual pores to an extremely low level. To produce
pore-free ceramics, it is necessary to use raw powder materials with good sinterability in the
dry process. One more important point is the processing technology, especially the process
of making the powder compact. This chapter describes a powder granulation method and
the properties of the granulated powders for the fabrication of laser ceramics. A method for
determining the packing condition of the granulated powders in the powder compacts and
the packing condition in relation to the compacting pressure is described.
The HIP process has become important for the production of high optical quality YAG
ceramics and large scale laser gain media. In this study, a HIP machine was used to reduce
the porosity, one of the optical scattering factors in ceramics. Argon gas was used as a
pressure medium. The applied pressure ranged from 9.8 to 196 MPa, and the treatment
temperature ranged from 1500 to 1700 ◦ C. The results achieved by a capsule-free HIP
treatment are described. Argon gas, the pressure medium, was introduced into the Nd:YAG
ceramics via grain boundaries, and the formation of pores due to argon gas was observed
in HIP samples. As a result, the number of residual pores increased after HIP treatment.
The disadvantages of the HIP process were determined qualitatively and quantitatively.
Approaches to solving the problem of pore formation in the sintered body and a fabrication
technology for optical ceramics with extremely low scattering are described.
Chapter 4 describes sesquioxides such as Sc2 O3 , Y2 O3 , and Lu2 O3 etc. which are
promising new materials for laser gain media. However, their melting points are higher
than 2400 ◦ C, and a phase transition point exists just below the melting point. For these
reasons, it is very difficult to produce sesquioxide laser crystals by the conventional melt-
growth process. In the ceramic process, it is possible to produce transparent sesquioxide
materials because sintering occurs at temperatures very much below the melting point and
phase transition point. In addition, ceramic technology allows the fabrication of large scale
media, composite gain media, and advanced gain media with controlled absorption and
emission spectral linewidth. Therefore, it is possible to create new functionalities such as
wavelength-tunable lasers and short pulse lasers. These materials are unique to the ceramic
technology, and there are many new functionalities to be discovered.
14 Introduction

Chapter 5 describes the synthesis of Nd:YAG ceramics heavily doped with 0.3–4.8 at.%
Nd ions, their optical characteristics and their laser performance. Generally, only about
1 at.% Nd ions can be dissolved homogeneously in YAG single crystal grown by the Cz
method. If the doping concentration of Nd ions exceeds 1 at.%, segregation of Nd occurs,
the optical quality decreases, and the material is not suitable for use as a laser gain medium.
In the case of polycrystalline YAG ceramics, it was confirmed that a greater amount of Nd
ions dissolved homogeneously compared to the melt-growth Nd:YAG single crystals. From
the spectroscopic point of view, heavily doped polycrystalline Nd:YAG ceramic (more than
1 at.% Nd ions) has a new functionality as an advanced laser material. One of its applications
is as a microchip laser and its laser performance (slope efficiency) was better than that of
commercial Nd:YAG single crystals. In addition, single longitudinal mode laser oscillation
was realized without using an etalon, mode selector, from a microchip ceramic laser.
In this chapter, the effect of impurities (Si added as a sintering aid) on the dissolution
of Nd ions in YAG ceramics is described, and we discuss why a large amount of Nd ions
can be dissolved homogeneously in YAG ceramics compared with single crystal YAG.
The main difference between single crystals and ceramics in terms of microstructure is the
presence or absence of grain boundaries, but a small amount of Si is also added in Nd:YAG
ceramics. It was identified for the first time that the addition of a small amount of Si leads
to more homogeneous dissolution of Nd ions in the YAG ceramics. The traditional theory
says that Nd can hardly replace Y in the YAG lattice because of the large difference in ionic
radius of the atoms. In this study, it was assumed that the lattice distortion, occurring when
Nd3+ replaces Y3+ in the YAG lattice, was compensated for by the addition of Si, and as
a result, a large amount of Nd could be doped homogeneously into the YAG lattice. In an
actual experiment, it was confirmed that 7.2 at.% Nd was doped homogeneously into YAG
ceramic using Si as a sintering additive.
In Chapter 6 we investigate the sources of optical scattering in polycrystalline ceramics,
and summarize the results of fabrication techniques for very reliable high quality Nd:YAG
ceramics. Single crystals have been utilized traditionally as the laser gain medium because
they do not have the problem of grain boundary scattering. This advantage has led to the
use of single crystals for optical applications. In this chapter, we focus on the pore volume
of Nd:YAG ceramics and the amount of grain boundaries, and evaluate the amount of
optical scattering quantitatively. In addition, the correlation between laser characteristics
and optical scattering was investigated. It was verified that the number of residual pores
and grain boundary phases greatly affects the laser oscillation characteristics. It was also
realized that the laser oscillation characteristics do not depend upon the number of grain
boundaries. Recent data demonstrated that the scattering coefficient of high quality laser
ceramics at the laser oscillation wavelength regions is lower than that of commercial laser
single crystals, and a breakthrough occurred in the optical performance of ceramics. The
laser performance of ceramics with extremely low scattering has reached very close to the
quantum oscillation efficiency, and ceramic materials have almost reached the ideal state
for application in optics. In addition, using laser tomography, the scattering conditions of
ceramics and commercial laser single crystals were investigated. Results of laser damage
tests, which can be used in the future development of high power lasers, are also described.
1.5 Outline of the book 15

In Chapter 7, the design flexibility of the ceramic technology is demonstrated with


examples of different shapes of laser gain media such as composites and fibers. The laser
performances are also described. Recently, a new type of composite consisting of two
or more crystals having the same crystal structure but different compositions has been
developed using a diffusion bonding technology in the USA. However, it has been pointed
out that the composite is very weak and shows a lack of long-term durability attributable to
the thermomechanical problems of the bonded interface of the composite. In this chapter,
the problems of conventional bonding technology are described, along with approaches to
solving those problems with the help of ceramic technology. Moreover, recently the author
has succeeded in fabricating single crystals using a solid-state sintering process. Using this
process, with a seed crystal, it is possible to fabricate bulky crystals as well as spherical
single crystals several tens of micrometers in diameter. This technique is expected to find
application in quantum devices using microsphere resonators. This chapter describes the
composite formation technology which is essential for the creation of new functionalities
in laser technology, and the fabrication of single crystals by sintering which can produce
laser materials with ideal optical performance.
In Chapter 8, the current status of ceramic lasers is summarized. Nowadays this area
is of great technological value, and research and development of ceramic lasers is very
active not only in Japan but also in Asia, especially China, America and Europe, and it is
expected that ceramics will become major materials for solid-state lasers in the future. The
development of the Dy:CaF2 ceramic in 1964 and of the Nd:Y2 O3 –ThO2 ceramic in the
USA led the way to the development of polycrystalline ceramic materials for application
as solid-state lasers. However, the laser oscillation was a pulse laser operation produced
under cryogenic conditions which was technologically and theoretically demanding. The
oscillation efficiencies were extremely low, clouding the future of ceramic gain media for
solid-state lasers. Since the successful development of high performance Nd:YAG ceramic
lasers, the potential functionalities of ceramic laser materials, which cannot be produced
using conventional melt-growth technology, have been realized successfully, and nowa-
days ceramic laser materials form a technological paradigm for solid-state lasers. Japan
has led the way in ceramic laser technology from 1995 until today, but successful laser
oscillations using ceramic gain media have also been reported from the USA, Europe and
China. Thanks to the successful development of ceramic laser gain media, the development
of high performance optical ceramics has become popular, and new types of transparent
ceramic materials have been reported: for example, high refractive index materials such
as zirconia and BNZT for ceramic lenses, Pr- or Ce-doped LuAG materials for radiation
(X-rays or gamma-rays) detecting scintillators, and spinel ceramic materials for ultravio-
let, infrared and visible light transmission windows. Nowadays, the development of high
level optical ceramics is taking place worldwide because of their high marketability. This
chapter explains the development of optical ceramics on a world scale, including ceramic
lasers.
In Chapter 9, the technology and science described in Chapters 1–7 are brought together.
Moreover, the role and the future of ceramics in laser technology are described. The
fundamental idea of the ceramic laser is based on the fabrication of an ideal ceramic with
16 Introduction

defect-free microstructure. This basic idea will be applicable in other technological fields
(e.g., electronic materials and structural materials etc.). Application technologies developed
by the author, and their possible development in the future, are also described in this chapter.
Chapter 10 describes the main results in the spectroscopic investigation of doped trans-
parent ceramics. It is shown that spectroscopic investigation has a double role, as a structural
method for describing the variety, nature and structure of the various structural centers of
the doping ions and the distribution of the doping ions in these centers, and as a method
of characterizing the optical processes that determine laser emission. Thus, spectroscopic
investigation provides the necessary information on the energy level structure and transition
probabilities to enable mathematical modeling of the laser process and selection of suitable
parameters for the laser material, pumping system and resonator design. Data on a large
variety of spectroscopic studies on doped ceramics are presented and their implication in
the structural properties of the ceramic and in modeling of the laser processes is discussed.
Chapter 11 describes the main factors that influence laser emission and heat generation
in doped ceramics. It is shown that a proper exploitation of the properties of laser ceramics
requires optimization of the pumping scheme for optimum utilization of the assorted exci-
tations for laser emission and for a reduction of heat generation. The structure–properties–
functionality relation for ceramic material is discussed and modalities to upgrade traditional
laser materials or to tailor new materials are discussed, together with new schemes for power
and energy scaling.

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[31] E. Snitzer, Oyo Butsuri (Bull. Appl. Phys. Jpn.) 34 (3) (1965) 164–175.
[32] M. Umino and M. Abe, Optronics Mag. 40 (1985) 93–97.
[33] L. G. DeShazer and L. G. Komai, J. Am. Opt. Soc. 55 (1965) 940.
[34] T. Kushida, H. M. Marcos, and J. E. Geusic, Phys. Rev. 167 (1967) 289.
[35] G. Adachi, K. Shibayama, and T. Minami, New Technology for Advanced Materials,
Kagaku-Dojin, Kyoto (1987), p. 1830.
[36] R. L. Coble, U.S. Patent 3026210 (1962).
[37] G. D. Miles, R. A. J. Sambell, J. Rutherford, and G. W. Stephenson, Trans. Br. Ceram.
Soc. 60 (1967) 619.
[38] R. W. Rice, J. Am. Ceram. Soc. 54 (1971) 205.
[39] F. W. Valdiek, J. Less-Common Met. 13 (1967) 530.
[40] K. Nagata, Y. Yamamoto, H. Igarashi, and K. Okazaki, Powder and Powder Metallurgy
Society of Japan, Proceedings of Spring Meeting (1982), p. 120.
[41] C. Greskovich and K. N. Wood, GE Rep., No.72CRD (1972), p. 243.
[42] C. Grescovich, D. Cusano, D. Hoffman, and R. Rinder, Bull. Am. Ceram. Soc. 71 (7)
(1992) 1120–1130.
[43] K. Nakano, Electronics, February (1985).
[44] K. Miyauchi and G. Toda, Opto-ceramics, Gihodo, Tokyo (1984).
[45] T. Hirai, Jitsuyo-Laser-Gijyutsu (Practical Laser Technology), Kyoritsu, Tokyo
(1987).
[46] C. Greskovich and K. N. Woods, Ceram. Bull. 52 (5) (1973) 473–478.
[47] C. Greskovich and J. P. Chernoch, J. Appl. Phys. 45 (10) (1974) 4495–4502.
2
Solid-state laser processes and active materials

Lasers constitute the main component (the optical range) of quantum electronics, the science
of generation, amplification, the control of the properties (wavelength, temporal regime,
power range) of radiation by the processes of interaction of electromagnetic radiation with
quantum systems. The word LASER is an acronym standing for Light Amplification by
Stimulated Emission of Radiation. The driving mechanism that determines the amplifica-
tion of radiation in a laser is the stimulated emission in an ensemble of identical quantum
systems (the active medium) with inversion of populations between a high energy level
and a lower energy level that act as emitting and terminal energy levels for the emission,
in a resonator that grants the necessary conditions for amplification and extraction of the
amplified radiation beam and gives it a modal structure. A very important class of lasers
is the solid-state lasers, where the quantum systems are embedded in a transparent solid
material. The first laser was a solid-state laser based on the ruby crystal [1] and during their
longer than fifty years history lasers have undergone tremendous scientific and technolog-
ical development. Many textbooks discuss the basic physical properties and processes that
determine the characteristics of laser materials and processes and the physics and engineer-
ing of solid-state lasers [2–20]. They contain extensive lists of relevant literature which will
not be repeated here. Based on these books and on other relevant literature, this chapter
discusses some of the major characteristics of laser materials and processes based on doped
transparent polycrystalline materials produced by ceramic techniques.

2.1 Interaction of quantum systems with electromagnetic radiation


(radiation absorption and emission processes in quantum systems)
2.1.1 Elementary processes
According to the analysis of Einstein [21], when interacting with an ensemble of identical
quantum systems (of density n0 ) with two energy levels E1 and E2 > E1 , an electromagnetic
radiation of quantum hν = E2 − E1 can induce two types of processes, absorption from the
level E1 to E2 and stimulated emission from E2 to E1 , which compete with the spontaneous
emission from E2 . These processes are shown schematically in Figure 2.1. In the absence
of this interaction the densities of the populations of the two levels at temperature T are

18
2.1 Interaction of quantum systems with radiation 19

E2, n2 E2, n2 E2, n2

B12 ρ(ν) B21 ρ(ν)


A12

E1, n1 E1, n1 E1, n1


(a) (b) (c)

Figure 2.1 Absorption and emission processes in a two-level quantum system: (a) stimulated absorp-
tion, (b) stimulated emission and (c) spontaneous emission.

related by the Boltzmann distribution law n2 /n1 = (g2 /g1 ) exp[−(E2 − E1 )/kT ], where g1
and g2 are the degeneracies of the two energy levels. Interaction with the electromagnetic
field induces variation of the population densities described by the rate equation
dn2 dn1 (st) (sp)
=− = W12 n1 − W21 n2 − W21 n2 , (2.1)
dt dt
such that at any moment of time the sum of the populations remains equal to the total
(st) (sp)
population n0 , i.e. n1 + n2 = n0 . In Eq. (2.1), W12 , W21 and W21 denote the rates of
absorption, stimulated emission and spontaneous emission, respectively. If the action of
the external electromagnetic field is suddenly stopped, the variation of the population n2
is determined by the spontaneous emission only and is described by an exponential decay
law with the spontaneous radiative emission (luminescence) lifetime τrad = (W21 )−1 ,
(sp)

i.e.

n2 (t) = n2 (0) exp(−t/τrad ). (2.2)

The rates of the stimulated (induced) processes depend on the energy density ρ(ν) of the
(st)
electromagnetic field, W12 = B12 ρ(ν) and W21 = B21 ρ(ν), while the rate of spontaneous
emission W21 = A21 is constant and τrad = (A21 )−1 . The Einstein coefficients A21 , B12
(sp)

and B21 are related by


8π ν 2 hν g1
A21 = B21 and B21 = B12 .
c3 g2
Whereas in the spontaneous emission there is no phase relation between the quanta emitted
by the various individual excited quantum systems of the ensemble, in the case of stimulated
emission the emitted quantum of each member of the ensemble is in phase with the quantum
that stimulates its emission. Stimulated emission can be induced both by photons of the
incident resonant electromagnetic field and by photons already emitted in the spontaneous
and stimulated emission processes. When the exciting electromagnetic field is coherent, the
beam of stimulated emission quanta from the various members of the ensemble preserves
20 Solid-state laser processes and active materials

the coherence; however, if the incident beam is non-coherent, the beam of stimulated
photons will have a very low degree of coherence.
At low incident energy density ρ(ν) the de-excitation of the level E2 by spontaneous
emission (luminescence) dominates completely the stimulated emission. The spontaneous
emission lines of the isolated quantum systems have small but finite width ν determined
by the lifetime broadening (the natural linewidth), such that τrad ν = (2π )−1 , which influ-
ences uniformly all the identical quantum systems from the ensemble and the lines have
Lorentzian shape. However, in reality these quantum systems are not completely free and
isolated and thus their quantum states are influenced by additional interactions that induce
broadening of the lines. The broadening of the lines can be homogeneous, when it influences
all the quantum systems from the ensemble identically, or it can be inhomogeneous, when
these additional interactions induce different shifts of the energy levels of the various quan-
tum systems. If these shifts are not resolved spectrally, they result in broadening of the lines,
although large perturbations could induce resolved effects. The homogeneously broadened
optical lines (absorption and emission) are symmetric around the central frequency ν0 and
have Lorentz shapes
 −1
2 4(ν − ν0 )2
gL (ν) = 1+ , (2.3)
π ν (ν)2

where ν is the full width at half maximum (FWHM). In the case of inhomogeneous
broadening the lines can be symmetric, with Gaussian shapes
   
ln 2 1 4(ν − ν0 )2
gG (ν) = 2 exp − ln 2 , (2.4)
π ν (ν)2

or asymmetric. Generally these two broadening mechanisms act together and sometimes
symmetric broadening combining the Lorentzian and Gaussian shapes (Voight profiles)
can be observed. Since the lineshapes are normalized, the linewidth ν and the peak value
g(ν0 ) are related, gL (ν0 )ν = 2/π ≈ 0.637, and gG (ν0 )ν = 2(ln 2/π )1/2 ≈ 0.939. Under
the action of narrow-band radiation all members of the ensembles with homogeneously
broadened lines respond identically, whereas in the case of absorption lines with dominant
inhomogeneous broadening the excitation is selective and involves systems whose peak
frequency is near the exciting frequency and are confined in the spectral region delineated
by the homogeneous broadening.
In real systems the characteristics of transitions are determined by the quantum states
(energy levels, wave functions) and by interaction with the electromagnetic field (selection
rules and transition probabilities for the various components – electric multipole and mag-
netic dipole – of the field). The optical transitions are investigated experimentally by static
(absorption, emission spectra) or dynamic (emission decay) or combined (time-resolved
spectroscopy) spectroscopic methods. The Einstein coefficients are seldom used in practice,
and parameters more relevant to collection or interpretation of the experimental results are
employed.
2.1 Interaction of quantum systems with radiation 21

r The line strength S characterizes the intensity of the spectral lines and is related to the
transitions between the quantum states for the various components i of the electromag-
netic field (electric dipole, electric quadrupole, magnetic dipole),

S= |ϕ1 |Pi |ϕ2 |2 , (2.5)
i

where ϕi are the wavefunctions of the states 1 and 2, and Pi is the operator of interaction.
The line strength can be measured directly from the experimental absorption spectrum.
r The oscillator strength f is a dimensionless parameter that establishes the relation
between the strength of transitions in a quantum system and the theoretical strength
of a single electron in a harmonic oscillator model and is related to the line strength by
8π 2 me ν
f12 = S12 , (2.6)
3e2 hg1
where me and e are the electron mass and charge and ν is the frequency of transi-
tion. The oscillator strengths for the downward and upward transitions are related by
f21 = (g1 /g2 )f12 . The line strength and oscillator strength can be related to the Einstein
coefficients,
8π 2 e2 ν 2 (8π 2 )2 ν 3
A21 = 3
f12 = S12 . (2.7)
mc 3hc3 g1
r The cross-section expresses the ability of an individual quantum system to absorb or
emit radiation and its dimension is that of an area (usually cm2 ) per quantum system.
The cross-section reflects the spectral composition of the optical process, σ (ν, ν0 ) =
σ0 g(ν, ν0 ), where the peak cross-sectionσ0 corresponds to the maximum (ν = ν0 ) of line
and, since the lineshape is normalized, σ (ν, ν0 )dν = σ0 . The absorption and emission
cross-sections are connected to the Einstein coefficients by the Fuchtbauer–Ladenburg
relations
1
σa ≡ σ12 (ν, ν0 ) = hνB12 g(ν, ν0 ) (2.8)
c
1 c2 c2
σe ≡ σ21 (ν, ν0 ) = hνB21 g(ν, ν0 ) = A21 g(ν, ν0 ) = g(ν, ν0 ) (2.9)
c 8π ν 2 8π ν 2 τrad
and a relation of reciprocity between these two cross-section holds,
 
σ12 (ν, ν0 )dν = (g2 /g1 ) σ21 (ν, ν0 )dν. (2.10)

The emission cross-sections corresponding to the center of the emission line (the peak
cross-sections) are related to the characteristics of the line and to the radiation lifetime: for
the Lorentz lineshapes
c2 c2 1
σ21 (ν0 , ν0 ) = 2 2
A21 = 2 2
, (2.11)
4π ν0 ν 4π ν0 ν τrad
22 Solid-state laser processes and active materials

whereas for Gaussian lines


 1/2  1/2
c2 ln 2 c2 ln 2 1
σ21 (ν0 , ν0 ) = A21 = . (2.12)
4π ν02 ν π 4π ν02 ν π τrad

2.1.2 The absorption of radiation


By traveling through the ensemble of quantum systems (the active medium) the energy
density of a resonant electromagnetic beam will be modified by these interactions. The
evolution of energy density ρ(νe ) after traveling a distance x inside this medium, neglecting
the effects of spontaneous emission, is described by the equation
 
dρ(νe ) g1
= −ρ(νe )B12 hνe n1 − n2 , (2.13)
dx g2
for which the solution is
   
g1 x
ρ(νe , x) = ρ0 (νe ) exp −hνe B12 n1 − n2 . (2.14)
g2 c
In the case of weak incident energy density n2 ≈ 0, and there is a net attenuation of the
beam by absorption. Equation (2.14) then takes the known Beer–Lambert form
ρ(νe , x) = ρ0 (νe ) exp[−α(νe )x], (2.15)
where α(νe ) is the absorption coefficient,
hνB12 n1
α(ν) = = n1 σ12 (ν). (2.16)
c
For a broadened absorption line of shape g(ν, ν0 ) the peak absorption cross-section (νe = ν0 )
can be related to the linewidth of the absorption line,
σ12 (ν0 , ν0 ) ∝ 1/ν. (2.17)

2.1.3 Amplification of radiation by stimulated emission


According to this picture, the absorption from the external electromagnetic field resonant
with the difference between the two energy levels induces its attenuation, whereas the
stimulated emission amplifies this field and the balance between these two processes at any
moment of time is determined by the instantaneous populations of the levels on which the
transitions originate: the population of the lower level for absorption and that of the upper
level for stimulated emission. Under the action of the external resonant field on the two-level
system, the population of the upper level cannot be larger than that of the lower level, and
the absorption dominates the stimulated emission. As a consequence, no net amplification
of the incident electromagnetic field can be obtained. Moreover, as mentioned above, if the
incident electromagnetic radiation is non-coherent, then the stimulated emission radiation
will have a very low degree of coherence.
2.1 Interaction of quantum systems with radiation 23

E3(Ep ) E4(Ep )

E2(Eem ) E3(Eem )

Pump

Pump
Laser

Laser
E2(Et)

E1(Et = Eg ) E1(Eg )
(a) (b)

Figure 2.2 The three-level (a) and four-level (b) laser schemes.

However, inversion of populations between levels E2 and E1 can be obtained under


the action of an external electromagnetic field by de-coupling the absorption from this
field and the stimulated emission in three-level systems. In such systems the strong external
electromagnetic radiation is absorbed efficiently into an upper level E3 (Ep ) from which the
excitation decays rapidly to the level E2 (Eem ) that gives stimulated emission terminating on
the ground level E1 (Et ≡ Eg ), as shown schematically in Figure 2.2(a). If the external field
is strong enough, the population of the excited level E2 can be larger than that of the ground
level E1 . This modality for creating inversion is called pumping. In the three-level (3L)
scheme a spontaneous emission quantum between the levels E2 and E1 can be amplified by
stimulated emission in an avalanche process and this grants a very high degree of coherence
to the amplified beam since all the photons from the amplified beam have identical phase
and propagate in the same direction. In order to dominate the global spontaneous emission,
conditions for efficient amplification of the stimulated emission must be created, i.e. a
long path for amplification, and this can be obtained by placing the quantum system in a
resonator that recirculates the largest part of the stimulated emission radiation through the
active medium and outcouples the rest of this beam. In the case of optical transitions, a
Fabry–Perot interferometer consisting of two parallel mirrors, one fully reflecting (the end
mirror, R2 ∼= 1), the other with a small transmission T = −ln R1 ≈ 1 − R1 (the exit mirror)
at the wavelength of emission, can serve as resonator. Moreover, by its mode structure, the
resonator determines the spectral characteristics of the laser radiation, the beam divergence,
diameter and transverse energy distribution.
Since in the three-level quantum generators the stimulated emission transition terminates
on the ground level, inversion of the population is difficult to achieve and very high
pumping rates are necessary. This shortcoming can be avoided in an alternative approach,
the four-level (4L) scheme (Figure 2.2(b)), in which the terminal level Et of the stimulated
emission is placed well above the ground level Eg such that Et − Eg kT , and its thermal
population is negligible. Additionally, the excitation reaching this level must decay very
fast to the ground level in order to avoid self-saturation of the laser emission. Intermediate
cases, when the terminal level is close to the ground level (Et − Eg of the order of kT )
and its thermal population causes partial reabsorption of emission can also exist: these
24 Solid-state laser processes and active materials

are called quasi-three-level (Q3L) schemes due to the partial reabsorption of emission,
although several authors prefer the name quasi-four-level (Q4L) scheme since the terminal
level is not the ground state. In order to avoid stimulated emission on other transitions, in
all these schemes the reflectivities of the laser mirrors must correspond to the wavelength
of the desired laser emission.
A quantum generator of radiation using stimulated emission is then composed of three
major parts: (i) the active material that contains the ensemble of quantum systems whose
quantum properties determine the ability to create inversion of the population and to
amplify the stimulated emission, as well as the major characteristics of this emission
(wavelength, gain spectrum and so on); (ii) the system which produces the inversion of
population between the emitting and the terminal energy levels (the pumping system);
(iii) the resonator which provides the conditions for feedback and outcouples part of the
beam of radiation amplified by stimulated emission. It is obvious that the starting point
in designing a quantum generator is the active material. The other two parts, the pumping
system and the laser resonator, must enable the most efficient exploitation of the properties
of this material; moreover, optimization of the quantum generator of the radiation will
require correlated optimization of these three parts. Fundamentals and engineering of laser
emission are described in many textbooks, such as [2–11]; these textbooks also provide
lists of the relevant literature, which will not be repeated here.
The stimulated emission can be considered as a negative absorption that increases when
the beam travels repeatedly inside the pumped laser material due to the reflections on the
mirrors with reflectivity R2 ∼ = 1 and R1 < 1. In order to reach gain at any given geometrical
point inside the pumped laser material placed in the resonator, the stimulated emission beam
must travel a round trip in the resonator. During this round trip the coherent radiation is
amplified with a gain dependent on the length of the laser rod according to exp(2glrod ).
However, taking into account that part of the laser beam is outcoupled through the mirror
R1 , the global round-trip gain is reduced to G = R1 exp(2glrod ). Similar to the absorption
coefficient α, the emission coefficient equals n2 σe ; however, taking into account the possible
reabsorption of the amplified beam due to a residual population of the terminal level, the net
effect on the amplified beam can be characterized by an effective gain coefficient g = nσe
with n = n2 − n1 .
The laser material and the resonator can introduce additional losses at the wavelength
of laser radiation, such as parasitic absorption, scattering, diffraction, residual Fresnel
reflection and so on, and these are coined in a loss coefficient L. The amplified beam
becomes intense enough to overcome the residual losses and the outcoupling loss when
R1 exp(2gl − L) ≥ 1; (2.18)
the strict equality in this equation defines a threshold condition for laser emission,
2gl = −ln R1 + L; (2.19)
usually the reflectivity R1 is large enough and ln R1 = ln(1 − T ) ≈ −T where T is the
transmission of the exit mirror, and
2gl ≈ T + L. (2.20)
2.2 Solid-state lasers 25

Below the threshold, the losses block the stimulated emission flux and a small-signal
gain coefficient g0 can be defined; immediately above the threshold, the stimulated emission
is amplified according to the gain g0 but for higher excitation the amplification of the light
beam continues until the gain saturates for the inversion of the population determined by
the actual pump intensity. The value of the saturated gain is determined by the pumping
conditions and by the characteristics of the laser material and the design of the resonator
and thus Eq. (2.18) establishes the connection between the output and input power by
taking into account all these characteristics. The gain threshold condition defines the pop-
ulation inversion and the emission cross-section necessary to overcome the actual losses
of the resonator: a larger emission cross-section determines a smaller threshold population
inversion and thus the laser starts to oscillate for frequencies around the central value ν0 of
the function g(ν, ν0 ) and the gain profile will be considerably narrower than the width of
this function. Nevertheless, pumping high above the threshold determines a broader gain
profile. Since the peak value g(ν0 , ν0 ) of the function g(ν, ν0 ) is inversely proportional to
the linewidth ν, and the Einstein coefficient A21 is inversely proportional to the emission
lifetime, the quantum systems with narrow emission lines and long lifetime will show a
lower laser threshold.
Although the first laser was a three-level system, the ruby laser [1], very soon the advan-
tages of four-level lasers became evident. The quantum systems with discrete energy levels
able to give emission in the optical range (ultraviolet, visible, infrared) with wavelengths
from hundreds of nanometers to tens of micrometers can be free atoms (such as in the
He–Ne laser) or ions (such as Ar+ ), free molecules (CO2 , CO, N2 and so on), excimer
noble gas halide molecules (ArF, KrF, XeF, KrCl, XeCl), ions of elements from the transi-
tional groups (elements with incomplete inner electronic shells) doped in transparent solids,
optically active defects in solids (color centers), solutions of organic molecules (dyes), and
a special category is the semiconductors, where the optical transitions take place between
collective electronic states (the conduction and valence bands). Efficient laser emission
was demonstrated in all types of laser materials; the present book refers to lasers based on
transparent solids doped with laser active ions, called solid-state lasers.
The phase coincidence of the photons in the stimulated emission process gives high
temporal and spatial coherence to the amplified beam: it is monochromatic and propagates
with reduced divergence. These properties open a very broad area of applications, based on
the quality of laser radiation as a carrier of energy or information, as a highly monochromatic
source for excitation or as a frequency etalon, as well as primary radiation for non-linear
optical processes.

2.2 Solid-state lasers


2.2.1 Laser active materials
The solid-state laser material consists of a crystalline or amorphous (glass) transparent
material doped with the laser active ions whose spectroscopic properties enable efficient
excitation and laser emission schemes [18, 19].
26 Solid-state laser processes and active materials

2.2.1.1 Laser active ions


The quantum electronic states of a free multielectron atom are determined by a complex
chain of interactions [12–16] reflected in the Hamiltonian
H = H0 + He−e + Hs−o , (2.21)
where H0 includes the electrostatic interaction between the electrons and nucleus and the
movement of electrons (kinetic part), He−e describes the interactions between the electrons,
and Hs−o describes the coupling of the orbital and spin moments of the electrons. Since
the orders of magnitude of these interactions differ greatly, their effect can be treated by
the perturbation theory. The eigenstates of the central-symmetric part of the Hamiltonian
H0 and of He−e are the electronic configurations consisting of electronic shells that contain
electrons with the same main and orbital quantum numbers n and l. Similar to the hydrogen
atom, the wavefunctions of the electrons can be written as a product between a radial
and an angular part. Each electronic configuration is characterized by a definite energy:
the differences in energy between the various electronic configurations are very large
(typically of the order of 105 cm−1 ) and only the configuration with the lowest energy
(the ground configuration) is populated. The laser active ions used for solid-state lasers
belong mainly to elements of transitional groups, i.e. of groups with incomplete inner
electronic shells of electrons d (single electron orbital quantum number l = 2) or f (l = 3):
the most popular in laser practice are the elements of groups 3d (iron group, n = 3, l = 2)
and 4f (rare earths, RE or lanthanides, n = 4, l = 3). The 3d group contains ten elements
with ground electronic configurations 1s2 2s2 2p6 3s2 3p6 3dn 4s2 , with n running from 1 for
21
Sc to 10 for 30 Zn, whereas the 4f group contains 14 elements with ground configuration
1s2 2s2 2p6 3s2 3p6 3d10 4s2 4p6 4d10 5s2 5p6 4f n 6s2 (for two of these elements a 4f electron
is replaced by a 5d electron), with n running from 1 for 57 La to 14 for 70 Yb. The excited
electronic configurations of these elements are usually placed above the optical range. The
radius of the 3d electronic shell in the 3d elements is smaller than that of the shell 4s;
similarly, in the case of the 4f elements the radius of the 4f shell is smaller than those of
the 5s, 5p and 6s shells, and thus the incomplete electronic shells in the free atoms from
these groups are inner shells.
When introduced in a solid matrix the 3d elements lose the less bound 4s and one or more
3d electrons to form ions of various valence states and thus 3d becomes the outer shell;
the 4f elements lose the 6s electrons and a 4f electron to form the dominant 3+ valence
state, but 4f remains the inner shell, being screened from the exterior by the closed 5s2 and
5p6 shells. In the free ions with weak or moderate spin–orbit interaction (this includes the
3d and 4f elements) the asymmetric part of the electron–electron interaction He−e couples
the individual spin and orbital moments of the electrons from each electronic shell into
the total orbital and spin moments L  and S characterized by the quantum numbers L and
S and determines the splitting of the electronic configurations into new electronic states,
the spectral terms, labeled by 2S+1 L (L takes the label S, P, D, F, G for L = 0, 1, 2, 3, 4
respectively). The L and S quantum numbers of the filled electronic shells are zero and
thus the electronic configurations are not split into terms and transitions are only possible
Exploring the Variety of Random
Documents with Different Content
d’un célibataire et d’une amie de passage, ou encore la visite d’une
parente à un parent momentanément confiné dans son appartement
par l’ordre du médecin.
La comtesse était assise sur l’étroit divan ; le prince lui faisait
face sur une chaise. Il avait, pour la première fois depuis sa
blessure, échangé ses vêtements d’intérieur contre un complet aussi
britannique que le col demi-souple et la cravate de foulard,
nonobstant la légère affectation de « genre artiste » à laquelle il ne
renonçait point. Quant à Stéphanie, sa finesse était trop aiguë et sa
connaissance de Paul trop intime pour n’avoir pas déguisé sous la
plus sobre, mais la plus savante parure sa démarche apostolique.
Tout en noir, comme au couvent, — et dans le fond de son être,
aussi claustrale et spiritualisée que jamais, — elle redevenait par la
magie d’une volonté surtendue celle de qui l’élégance, plus encore
que la beauté, avait désarmé tant d’ennemis lorsqu’elle avait épousé
le prince.
Tandis qu’ils échangeaient des propos d’une indifférence, d’une
banalité qu’on eût dites concertées, tant ils s’entr’adaptaient
aisément, chacun d’eux observait l’autre.
L’altération physique du prince frappait Stéphanie. Osterrek,
pourtant, lui avait ménagé le matin même une entrevue avec le
docteur Burcart, qui avait dit :
— Chaque heure de lit accroît le risque de congestion passive, et
Son Altesse peut à peine quitter le lit deux heures par jour. Alors,
sauf le cas d’un miracle !…
Elle n’en était pas moins émue. Elle le trouvait méconnaissable,
inquiétant surtout par son aspect d’usure et de fragilité.
N’eût-elle pas apporté à cette rencontre des sens définitivement
amortis, le goût instinctif qui l’avait de tout temps portée vers la
santé et la force aurait chassé loin d’elle tout péril de tentation. Elle
pensait, au contraire, avec cette rancune contre la chair, habituelle
aux voluptueuses converties : « Dire que je fus criminelle pour
cela !… » Et elle se plongeait avidement dans le dégoût de l’amour
physique, tandis que, pour ce mourant, le feu de sa charité s’avivait,
comme s’il se fût nourri de la matière renoncée. « Voici enfin, se
disait-elle avec un saint orgueil, l’heure où je l’aime parfaitement ! »
Et lui ?
Lui ne pratiquait ni ne souhaitait aucun renoncement. Ignorant
son état réel, il se jugeait en plein essor de convalescence. Tout à
l’heure, quand il était proche de Madeleine et qu’on était venu lui
dire : « Madame la comtesse attend Son Altesse au salon », il avait
brusquement suspendu son effort de consoler la jeune fille, et il avait
couru, plein de curiosité entreprenante, au tête-à-tête avec
Stéphanie.

Ainsi, dans le même banal appartement d’hôtel, deux épisodes


de la triple aventure se jouaient en même temps, — leurs scènes
séparées uniquement par la chambre vide du prince.
Dans le salon où les glaces avaient reflété naguère l’image de la
danseuse nue, il y avait deux amants un moment dissociés, puis
ramenés aux prises, chacun en arrêt sur sa proie, corps ou âme…
Et dans la chambre de Madeleine, sur le fauteuil où le prince l’avait
laissée, les yeux fixes et secs, la tête douloureuse, les mains
ardentes traînant sur les genoux, il y avait un petit être au grand
cœur, naguère en possession de la paix céleste, l’ayant quittée pour
la folle entreprise de sauver un inconnu, un être à qui cette tâche
allait être arrachée, et qui se sentait au moment d’être précipité dans
le vide.
Elle pensait :
« Il faut que je parte d’ici… avant qu’ils ne reviennent, car ils vont
revenir tous les deux, et cela, non ! Je ne peux pas… J’irai trouver
l’abbé Nervi, le supplier de m’envoyer où il voudra, converse…
servante. Sûrement il m’aidera. Allons !… Il faut se dépêcher ; dans
quelques instants ils vont revenir ensemble. Et je reste là, comme si
j’étais percluse ! Mais qu’est-ce que j’attends ? qu’est-ce que
j’attends ? Oui… J’attends la fin de leur conversation, ce qu’ils vont
décider… »
Sans le savoir, elle attendait autre chose : l’aboutissement d’une
crise intérieure qui avait commencé lorsqu’elle avait appris l’arrivée
de Stéphanie, et qui, depuis, fermentait en elle, évoluant vers son
paroxysme depuis qu’elle les savait ensemble, à vingt pas d’elle,
isolés, enfermés…
Vers ce tête-à-tête invisible se tend une imagination dont la force
et la vivacité furent développées par la culture ascétique. En cet
instant, elle ne peut pas penser à autre chose qu’à Stéphanie et à
Paul, qui furent amants, dont elle a connu, par les aveux de
Stéphanie, la vie d’amants. Ces deux amants dont elle déteste le
péché, elle les admire l’un et l’autre ; ils lui ont appris l’un et l’autre
que l’amour n’est pas nécessairement abject, qu’il change de figure
selon les êtres qu’il unit. Vague réhabilitation dont elle n’a pas eu
conscience jusqu’à présent. Aujourd’hui son imagination transforme
en un tableau animé l’objet de sa méditation, fait vivre devant ses
yeux la rencontre. Qu’ils puissent tenir compte d’elle, chétive et
dédaignée, elle sent bien que non ! Bien sûr, ils ne pensent qu’à eux-
mêmes ; leur péché les ressaisit et ils redeviennent amants. Elle
croit les voir, elle gémit de douleur. Quelque chose d’instinctif, en
elle, proteste, crie : « Moi !… moi !… » Avec le poison de la jalousie
féminine, le poison du désir glisse dans ses veines pour la première
fois, et elle apprend l’amour par la douleur.

Or, si elle avait regardé de ses yeux corporels, au lieu de


l’imaginer, ce qui se passait dans le salon clos, voici ce qu’elle aurait
vu.
Les deux interlocuteurs avaient franchi la première étape. Il
n’était plus question entre eux du confort de l’hôtel, de l’attrait de la
station, de la longueur du voyage entre le couvent et cette station, ni
même des apparences de santé ou de fatigue que montraient leurs
visages. Tout cela s’était volatilisé sans laisser à la conversation le
moindre aliment. Encore moins (quoi qu’imaginât l’innocence
embrasée de Madeleine) pouvait-il s’agir entre eux d’une brusque
reprise de caresses. Paul avait perçu, dès l’abord, une Stéphanie
glacée. D’ailleurs, il ne renonçait à rien, l’ayant jugée désirable, tout
en notant la lourde trace, sur sa beauté, des mois échus en son
absence… Certain vers de Baudelaire (la pêche meurtrie) sillonna
sa mémoire. Mais, jugeant prématurée une offensive, il se
divertissait à n’aider en rien l’adversaire. Il affectait de trouver cette
visite tellement naturelle que nulle explication n’était nécessaire.
« Ce n’est pas moi qui l’ai appelée, donc c’est elle qui est
« demanderesse » ; qu’elle se débrouille… Elle est fort belle,
toujours. » Il la détaillait impudemment, seul des deux à l’aise dans
le silence contraint qui s’appesantissait sur eux. Il fallut bien que
Stéphanie parlât. Fâcheusement pour elle, l’accueil cérémonieux de
Paul l’avait énervée ; elle reconnaissait son procédé pour prendre
l’avantage dans un débat, rien que par l’ironique impassibilité. Elle
aborda de biais l’objet essentiel :
— Osterrek vous l’a dit, n’est-ce pas ? J’ai voulu accourir auprès
de vous dès que j’ai connu votre accident. Je n’ai pas pu.
— Est-ce qu’on vous avait enfermée ? questionna le prince avec
le plus grand sérieux.
— Vous savez ce qui m’a retenue, répliqua Stéphanie sans
accuser le coup. Vous me reconnaissez certainement le droit, dans
le désarroi de ma vie, d’avoir demandé à ma religion un abri… et
une direction.
Paul s’inclina sans rien dire.
— Cette fois, je suis autorisée, reprit-elle, et vous pouvez
disposer de moi.
Comme Paul écoutait toujours, elle dut continuer.
— Mon dévouement pour vous n’a pas fléchi, Paul… Et je crois…
je suis sûre que ma présence ici aura un bon effet sur votre santé
d’abord, et puis… sur l’opinion… Elle vous touche peu, je le sais,
mais le moment est peut-être venu de… ne pas la négliger.
— Je ne comprends pas ? interrompit le Prince que ces derniers
mots seuls avaient égratigné. Me trouvez-vous déjà arrivé à la
minute où il faut préparer un beau départ ?
— Non, bien sûr, fit Stéphanie désarçonnée. Je songe à la famille
royale, à votre pays qui vous aime.
En prononçant ces paroles, elle se gourmandait intérieurement :
« Qu’est-ce que j’ai à être si maladroite ? Je ne sais plus ce que je
dis. »
Le Prince la tira d’embarras en parlant à son tour, parfaitement
libre d’esprit, sauf l’angoisse sensuelle qui pointait en lui : « Voudra-
t-elle ? » Le reste ne lui importait guère. Son égoïsme n’avait aucun
besoin de Stéphanie prolongeant sa présence, puisque Madeleine
était là.
— Ma chère amie, dit-il en lui prenant une main dans les siennes
(la main captive demeura inerte), nous n’en sommes pas à jouer l’un
contre l’autre au plus habile. Parlons franchement : vous n’arrivez
pas de si loin pour me proposer d’être mon infirmière.
— Vous en avez une, fit Stéphanie qui retira sa main.
Il se méprit, lui si délié, à ce geste. « Tiens ! pensa-t-il, elle est
jalouse. » C’était exact, mais d’une jalousie toute spirituelle qu’il ne
pouvait soupçonner.
— Je pense, dit-il assez pauvrement, que vous ne faites pas de
comparaison ?
Elle haussa les épaules, consciente désormais de mener le jeu.
« Il n’a pas changé », pensa-t-elle. La sensation d’être désirée par ce
malade lui fut physiquement pénible. Mais elle dissimula.
« D’ailleurs, pensa-t-elle, Osterrek m’a assuré que je n’ai rien à
craindre. »
Sentant une résistance dont la cause lui échappait, Paul fut prêt
soudain à payer n’importe quel prix pour contenter son envie.
L’instant lui parut propice à la mise en scène qu’il avait méditée à
l’avance.
Il se leva, alla presser le bouton d’une sonnerie.
— Je demande une tasse de thé ?…
— Volontiers.
Madeleine, entendant battre des portes et des pas circuler dans
la chambre, souleva le rideau tendu entre cette chambre et la
sienne, où elle avait fait la nuit. Elle vit, dans le crépuscule de la
pièce vide, passer un maître d’hôtel portant un plateau. La porte du
petit salon fut ouverte. Il était très éclairé ; Madeleine distingua
Stéphanie assise sur le canapé ; puis, le plateau déposé sur le
guéridon et le maître d’hôtel s’effaçant, elle aperçut le prince qui
s’approchait et prenait place à côté d’elle sur le divan. Ensuite la
porte se referma, tirée par le maître d’hôtel, qui repartit les mains
vides. Madeleine poussa un gémissement qui avorta dans sa
gorge… Elle se traîna jusqu’au fauteuil. Ses yeux évoquaient dans la
nuit le torse nu du prince, avec sa coupure sanglante, plus
nettement que ses yeux ne l’avaient jamais vue.
La comtesse, cependant, faisait avec aisance le ménage du
goûter. Paul la regardait et ses narines de chien de chasse la
respiraient d’aussi près qu’il pouvait. Elle s’en aperçut et en fut
incommodée. Ils effleurèrent leurs tasses, s’observant à la dérobée.
A cette minute, Stéphanie comprit qu’elle pouvait faire de lui ce
qu’elle voulait, demander le mariage catholique, demander qu’il la fît
reine et la couvrît d’apanages ; il suffisait d’un abandon. Elle pensa
cette oraison jaculatoire : « Mon Dieu ! ôtez-lui le désir… car, s’il y
cède, moi je ne céderai pas. Et alors tout est perdu. » Les artifices
de sa coquetterie passée ressuscitèrent dans ses gestes, et aussi
dans ses regards et ses paroles. Ainsi s’établit entre eux, pendant
un temps assez long, une convention dont aucun n’était dupe.
Toutefois Paul ne suivait plus le jeu de sa partenaire. « Elle sait bien
qu’elle me tient et elle lâche prise ?… » Il n’était déjà plus capable de
se contenir, car, par un effet assez ordinaire, la maîtresse ancienne,
ranimant par sa présence la mémoire des sens, le bouleversait plus
qu’une nouvelle aventure. Comme le bras de la comtesse atteignant
un citron passait sous ses lèvres, il baisa au vol la place naguère
encerclée par le bracelet des heures. Le recul du poignet fut si
brusque que le citron roula jusqu’au tapis. Elle voulut sourire :
— Voyez ! J’ai perdu l’habitude…
Mais lui ne sourit pas. Il réfléchissait. Il craignait d’avoir compris ;
et sa figure trahissait une angoisse autrement profonde que celle
d’une galanterie rabrouée. Stéphanie perçut le péril et se gourmanda
intérieurement. Ce fut elle qui lui prit les mains, qu’elle sentit
incendiées par la fièvre.
— Paul !…
— Eh bien ?
— Vous avez vu juste. Je ne suis pas venue ici seulement pour
soigner votre corps.
« Voilà qui est plaisant, pensa-t-il (car il ironisait volontiers avec
lui-même). Celle-là aussi veut me convertir ?… »
Mais la raillerie qui transperçait dans ses yeux ne rebuta pas la
missionnaire.
— Paul, reprit-elle d’un ton fervent, j’ai été votre compagne
dévouée, et je vous ai quitté avec désespoir. Je ne suis plus dans le
monde ; je ne suis plus de cette terre. Vous ne pouvez pas m’en
vouloir de chercher à vous posséder au delà de la vie !
Sa déception, qui était amère, le rendit cruel. Il déclama à demi-
voix :
— « C’est peu d’aller au ciel, je veux y conduire. » Polyeucte,
acte IV… Je ne sais plus le numéro de la scène…
Il la détesta un instant, et balança s’il n’allait pas sonner et la
faire reconduire. Mais elle tentait de plus en plus son appétit
sensuel, et chaque obstacle, chaque déconvenue poussaient la
tentation vers son paroxysme. Il vécut alors une de ces minutes où
un homme de son tempérament est prêt à livrer tout pour qu’une
femme dise : Oui !
— Je crois vous comprendre, reprit-il d’un ton volontairement
adouci. Et… tenez !… je vous épargne des précisions qui vous
gênent. Vous désirez d’abord, je suppose, que votre premier
mariage soit rompu à Rome et que le nôtre soit ratifié selon votre
culte ?
— Non ! Non !…
Elle n’avait pas pu se taire, tant la convulsait l’idée de reprendre
la vie conjugale.
— Alors, répliqua Paul dépité, je ne vous comprends plus.
Elle essaya de corriger son imprudence. Penchée sur Paul et lui
tenant la main, elle balbutia :
— Notre mariage ne vous a causé que des déboires, dont je
m’accuse et dont je vous demande pardon. Ne ravivons pas la
curiosité du monde et les soucis de votre famille.
Elle balbutiait péniblement ces paroles confuses, dont elle
déplorait au même instant la misère, quand une sorte d’illumination
intérieure la traversa : elle crut comprendre quel sacrifice
momentané exigeait d’elle le salut de ce mourant.
— Paul, je suis prête à demeurer auprès de vous, afin de vous
conduire à ce rachat de vous-même auquel j’ai voué ma vie.
« Ah ! pensa le prince… Elle y vient ! »
Frémissant d’un émoi dont elle ne sut pas mesurer la violence,
tant la vie claustrale l’avait glacée, il approcha sa bouche de son
oreille et murmura dans un halètement :
— Et ce sera entre nous… comme avant ?
Il commençait de l’enlacer avec ardeur, mais sans brutalité. A ce
contact, elle reconnut enfin le heurt de ce désir viril dont elle se
croyait préservée. Elle parvint à se maîtriser… elle espérait encore.
Mais, comme il cherchait ses lèvres et que la fièvre de cette haleine
l’obsédait, elle se délivra. Debout, hagarde, ses gestes et ses
paroles devinrent la proie de l’instinct. Une seule idée dans sa tête :
écarter l’homme, se sauver de lui. Elle ne freina même pas sa
parole.
— Comme avant !… Cette boue ! cet enfer !… Grâce à Dieu, j’en
suis sortie ! Il ne permettra pas que j’y retombe !
La rudesse du choc laissa un instant le prince abattu sur le divan
comme un mannequin inerte. Puis, de nouveau, il la détesta,
d’autant plus qu’il se méprit sur la cause de sa défaite. Quand il put
cracher son amertume en paroles entrecoupées :
— Voilà votre amour ! dit-il… J’avais oublié votre goût pour les
partenaires solides… Si je n’étais pas le malade que je suis !…
— Paul, implora Stéphanie, ne me meurtrissez pas ! J’ai subi des
déchéances… Elles furent encore de l’amour pour vous.
— Allons ! fit Paul qui récupérait son allure hautaine. Tout ce que
nous dirons ne sert plus à rien, et mieux vaut nous en tenir là.
Alors Stéphanie, dans la terreur d’abandonner sa tâche, de
laisser en perdition cette âme si proche de la mort, montra combien
elle était loin encore, malgré son entraînement mystique, de l’art
subtil d’un Orban ou d’une Madeleine à manœuvrer les âmes.
— Paul, dit-elle, les passions misérables qui vous agitent ne sont
plus de saison. Ignorez-vous la vérité ? Dieu peut faire le miracle de
vous rendre la santé : mais ce sera un miracle. Je vous en conjure,
concevez la gravité de l’heure.
Elle se tut ; leurs yeux, pendant quelques secondes de silence,
ne se quittèrent plus. Elle vit les joues du prince se colorer
brusquement ; puis la pâleur les envahit de nouveau, plus morbide,
plus terreuse. Elle alla vers lui, prête à le secourir :
— Paul…
Il eut la force de se mettre debout, tout seul. Il se recula d’elle,
comme s’il ne voulait plus l’effleurer.
— Écoutez-moi, lui dit-il… Vous venez de me faire plus de mal
que la misérable bête d’amour qui m’a frappé au côté. Votre
compassion me fait horreur… Laissez-moi ! Laissez-moi !
Elle eut encore un mouvement pour protester.
— Je vous dis de me laisser, répéta-t-il.
Il avait sonné, et le valet de chambre était sur le seuil.
— Reconduisez madame la Comtesse.
Elle dut obéir. Derrière le rideau soulevé, Madeleine la vit
traverser la chambre, dont ce domestique ouvrit la porte extérieure
avec une hâte respectueuse, et disparaître.
XVIII

La nuit…
La nuit, lâche ennemie des faibles : elle abuse contre eux de sa
force obscure, insaisissable. Les enfants, les sans-asile, les malades
s’épouvantent à sentir qu’ils sont sa proie désarmée : les malades
surtout, que leur impotence lui livre enchaînés. Alors le monde,
autour de leur lit chétif, s’espace, se vide, les abandonne à leur
souffrance et à leur angoisse. Alors ils pensent : « Nous sommes un
déchet, un rebut ; on nous tolère ; on ne nous achève point ; mais, le
matin venu, le monde ne s’apercevra même pas si nous ne nous
réveillons pas avec lui. »
L’ombre de la nuit passagère rejoint ainsi, pour consommer leur
détresse, la grande ténèbre éternelle.
Heureux, parmi ces désolés, ceux que des mains pleines de
santé retiennent au bord du ravin d’épouvante. Ils se raccrochent à
cette chose vivante, capable de résister à l’ennemi. Par la vue, par le
contact, par l’avide aspiration des paroles et du bruit, des pas qui
rompent le silence hostile, ils s’incorporent à un organisme sain et
fort, ils s’abritent contre la nuit… Les mains de Madeleine, ses yeux
de lumineuse poussière, son visage rayonnant de jeunesse et de
vigueur paysanne, l’articulation lente et sûre des mots qu’elle
prononce : quel bienfait vaudrait celui-là pour le débris humain dont
elle veille l’insomnie… Il l’a appelée au secours dès que l’autre
femme l’a laissé seul après l’avoir frappé au cœur. Sa détresse
égoïste n’a pas eu un mot de repentir ou de pitié pour le mal que
l’humble gardienne a enduré, qu’il sait qu’elle a enduré. Il a dit
brièvement, sèchement :
— Aide-moi à me coucher. Et que personne n’entre, personne…
tu entends ?
Mais, dans la calme tiédeur du lit, sa colère s’est peu à peu
détendue. Il s’est laissé bercer, caresser par l’enfant maternelle,
comme un enfant plus débile. Devant elle, si humble, si discrète,
pourquoi se contraindre ? Il a laissé couler des larmes qui
l’oppressaient et dont le cours l’a soulagé. Il s’est plaint puérilement
du mal qu’il a souffert. Il a confessé la peur atroce qui l’étreint depuis
que des mots irréparables ont été prononcés : la peur de mourir.
Oui, ce même prince Paul qui, dans les combats du front oriental,
s’est fait gourmander et punir par ses chefs pour sa témérité
maladive, la peur de mourir le mue en un chiffon humain. Il s’agrippe
aux poignets de Madeleine.
— Dis-moi la vérité. Pas de dérobades ni de défaites. Est-ce que
je suis perdu ? Je veux savoir !
Ah ! le solide appui, l’efficace réconfort — ce regard, inflexible
sous l’attaque de son regard et la réponse de cette bouche qui ne
peut pas mentir :
— Jamais le médecin ne m’a dit pareille chose. Vous avez été en
danger, alors que vous ne pouviez pas vous lever. Mais quelle
maladie ne comporte pas de danger ? Une des novices de la
Quarantaine est morte à vingt ans sous nos yeux pour une piqûre de
mouche.
Il pense :
« Comme c’est vrai, ce qu’elle dit ! On ne sait rien à l’avance…
J’ai été déjà plus malade que je ne suis, et j’ai guéri. »
— Si tu me soignes bien, fait-il, je ne mourrai pas. J’ai confiance.
— Je vous soignerai de toutes mes forces.
Les mains de l’ange, à force d’être serrées et retenues, sont
presque douloureuses. Et il ne lui permet pas non plus de se taire ; il
veut l’entendre parler, car cette voix l’empêche de penser par lui-
même. S’il était capable, dans sa détresse, de comparer ce qu’elle
dit avec ce qu’a dit Stéphanie, comme il admirerait le don inné, chez
la paysanne inspirée, de l’apostolat consolateur ! Pourtant, elle ose
lui parler de cela même qui l’épouvante, de la Visiteuse suprême
dont il croyait tout à l’heure entendre le pas derrière le seuil. Mais
dans les propos de Madeleine, il ne s’agit plus d’un danger qui le
menace, lui, le malade. Elle raconte avec simplicité comment elle-
même envisage le terme de sa propre vie ; combien il est aisé,
quand le cœur est paisible et net, de vivre amicalement avec une
telle pensée. « Je serais bien malheureuse, dit-elle, si je devais
échapper au sort commun, et voir éternellement les jours et les nuits
se succéder… » Il écoute avidement. Il lui semble que le péril n’est
plus pour lui seul ; que c’est comme au front d’Orient : une menace
confuse, aussi probable pour n’importe qui que pour soi. On ne sait
où l’obus éclatera ; on se fie à sa chance. Et la Visiteuse effrayante
finit par se muer en une compagne douce et pitoyable qui nous suit
tout le long de la vie et se rapproche enfin de vous pour soutenir et
recueillir les derniers pas.
Madeleine sentait mollir peu à peu l’étreinte angoissée de ses
mains et leur fièvre fléchir. Les paupières du malade commencèrent
de battre, puis s’abaissèrent. Cependant Madeleine ne cessa point
de parler, connaissant le pouvoir de sa voix… Mais, peu à peu, au
lieu de l’exhorter, elle murmura simplement des prières. Non pas
uniquement des prières apprises, mais ses prières « à elle », ces
conversations implorantes qu’on ne lui avait jamais enseignées, et
qu’elle n’interrompait guère, à travers les travaux de sa vie… « Ma
chère patronne, je vous supplie de réconcilier ce pécheur, et je
m’offre à être sa rançon. Le Sauveur s’est bien chargé des péchés
du monde : une pauvre petite chose comme moi ne peut-elle pas
être sacrifiée au salut d’une âme ? Ma chère sainte patronne, je
vous en prie, je vous en prie… »
Il reposait à présent. Elle mit silencieusement le lit bien en ordre ;
puis elle traça du pouce droit, sur le front du malade, les deux traits
perpendiculaires de la croix. Ensuite, elle éteignit la lumière des
ampoules, et, à la lueur de la veilleuse, gagna sa couche, où elle
s’étendit, parée à toute alerte.
Le lendemain, au cours de la matinée, il attira contre lui la tête de
la jeune fille et l’étreignit tendrement, sans l’ombre de perversité.
— Hier, lui dit-il, tu m’as fait beaucoup de bien, et moi, je t’avais
fait du mal. Pardonne-moi. Je ne vaux rien… et puis, je suis malade
et persécuté. Je n’ai plus que toi au monde. Je ne veux plus voir que
toi. Ne laisse entrer personne !
Elle eut assez de peine à le convaincre qu’il ne devait pas fermer
sa porte au comte Osterrek.
— Celui-là vous aime à sa manière, mais il vous aime fidèlement.
Maintenant elle le gouvernait. Il consentit à le recevoir quelques
instants, après la visite du médecin : son humeur était adoucie parce
que Burcart, le trouvant en meilleur état, lui avait permis de se lever.
Le prince s’amusa de l’air embarrassé de son camarade. Il
s’obstina à lui parler de tout, sauf de Stéphanie, comme s’il tenait
pour inexistante la rencontre de la veille. Et le comte lui demandant
ses ordres pour la journée :
— Mon vieux, lui dit-il, je veux qu’on me laisse vivre aujourd’hui
une vie végétative ; je ne veux parler à personne ; je ne veux voir
personne que l’ange. Si tu as une communication à me faire,
demande l’ange.
La figure bilieuse du comte se crispait, et son maître vit dans le
coin de ses paupières fripées quelque chose d’humide qui reflétait la
lumière.
— Ne te chagrine pas, vieux camarade, lui dit-il. Je te connais, et
je sais que toi, au moins, tu n’essayeras pas de me faire du mal
exprès.
Il lui serra la main fortement. Le comte sortit sans pouvoir
prononcer un mot.
Ces choses se passaient aux environs de midi. Un brouillard
lucide, mais pourtant impénétrable au regard, s’exhalait du lac et
tendait une gaze claire derrière les vitres. Tout d’un coup cette gaze
se déchira et, par la déchirure jaillit, à la manière des projections de
théâtre, un faisceau de clarté jaune et chaude. Puis le voile entier se
partagea en lambeaux, s’émietta, se volatilisa, et le paysage du lac
redevint éblouissant. Aussitôt le prince voulut se lever. Son valet de
chambre et Madeleine hâtèrent sa toilette. Il avait faim.
— Qu’on serve le lunch dans le petit salon, dit-il. Toi, Madeleine,
tu déjeuneras avec moi. Ah ! pas d’objection, n’est-ce pas ? Tu
déjeuneras avec moi.
Elle y eut moins d’embarras qu’on ne l’aurait supposé : rien ne la
troublait, des événements de la vie matérielle, parce qu’elle ne leur
demandait ni joie ni profit. La gaîté du prince, pendant ce repas tête
à tête, la surprit et la ravit. Gaîté un peu nerveuse, réaction contre la
mortelle angoisse de la veille : on eût dit qu’il prenait sa revanche
sur Stéphanie et voulait se prouver à lui-même qu’il renaissait, qu’il
vivait. Il ordonna à Madeleine de goûter au champagne sec qui était
sa boisson ordinaire et que le médecin lui permettait à doses
modérées ; il s’amusa de la grimace qu’elle fit, buveuse d’eau et de
bière légère depuis l’enfance ; sept ou huit fois dans sa vie (la
dernière au Café franco-suisse) elle avait goûté à du vin rouge…
Mais comment eût-elle résisté au bonheur de voir son malade
rasséréné, et dépouillant pour elle tout ce qu’elle redoutait de lui : la
perversité et l’ironie ? Il était sincère quand il lui dit :
— Je ne vaux rien, et malgré deux rudes coups que j’ai reçus ici,
je n’ai pas changé. On ne change pas !… Si je redeviens solide et
libre, j’ai bien peur de recommencer ma mauvaise vie. Mais j’ai
changé pour toi, et aucune femme n’aura connu l’homme que je suis
avec toi. Je suis désarmé contre toi, comprends-tu ? parce que j’ai
besoin de toi, telle que tu es, petite sainte, et que j’ai une peur
superstitieuse de te défaire… Tu ne peux pas comprendre !
En effet, elle ne comprenait pas : mais les mots qu’elle écoutait la
berçaient, et elle laissait dire. S’il l’attirait contre lui et lui baisait les
yeux et les joues, elle ne résistait pas : elle sentait que d’un mot elle
pouvait l’arrêter. Ces caresses lui étaient douces comme celles d’un
frère chéri ; elle n’en était point troublée. Un contact, une pression de
main, un baiser ne risquaient pas de l’émouvoir : c’était du fond de
son âme, de ce mystérieux inconscient où sa féminité demeurait
tapie, intacte et pressante, que pouvait monter la révélation de
l’amour.
Quand cette dînette, où le prince s’enchanta lui-même à une
façon d’aimer qu’il n’avait plus pratiquée depuis ses sorties de
collégien chez le général Delenca, s’oubliant exprès et cherchant le
bonheur de l’autre, il exigea que l’ange s’étendît sur le divan du petit
salon et se reposât.
— Mais je ne suis point lasse !…
— C’est un ordre. Tu as beau être en acier, on ne résiste pas
indéfiniment à la vie que je te fais mener. Étends-toi ici.
Lui-même traîna près du divan un gros coussin formant tabouret
et s’y assit ; puis il posa sa tête sur la poitrine de la jeune fille. Elle
s’y prêta sans hésitation ni méfiance. Le malade plongea d’ailleurs
tout de suite dans le plus profond repos, corrigeant l’insomnie initiale
de la nuit précédente. Elle, bien qu’elle ne redoutât rien de lui, ne put
s’assoupir, même un instant. Elle était trop heureuse : il lui semblait
que sa jeune santé enveloppait le dormeur, dans cette maternelle
étreinte, et le pénétrait. Le cou du prince, qu’elle entourait de son
bras, s’appuyait à son sein gauche ; elle percevait à la fois le rythme
de leurs deux vies. D’abord l’artère du malade battit en désordre,
tantôt active à l’excès, tantôt presque défaillante, tandis qu’au flanc
de la paysanne les pulsations se succédaient à intervalles courts,
mais égaux. Puis, comme par l’effet d’une mystérieuse endosmose,
les deux rythmes s’harmonisèrent. Vint un moment où l’oreille de
Madeleine n’entendit plus qu’un seul choc géminé. Elle en fut
puérilement joyeuse. Le trésor de maternité que recèle l’âme de
toute vierge sage, elle l’épancha sur ce viveur dont la débilité
douloureuse refaisait un enfant. Furtive et ardente, elle posa ses
lèvres sur sa tempe et les y laissa appuyées, guettant, pour qu’il ne
surprît pas le secret de ce baiser, le plus léger mouvement de celui
qui reposait sur son cœur.
Aussitôt réveillé, le prince exigea qu’on le descendît sur la
terrasse. Il voulait y poursuivre les dernières clartés du jour. A
mesure que déclinait le soleil, son alacrité maladive s’exténuait : le
souvenir de l’atroce soirée de la veille le harcelait, et il s’effarait
devant l’angoisse nocturne. Vainement sa compagne essaya de le
distraire : il lui souriait, il lui parlait avec tendresse : mais elle le
sentait inquiet. Il prolongea sa station sur la terrasse jusqu’à l’heure
où le brouillard montant du lac commença de l’oppresser. Revenu
dans sa chambre, il resta longtemps silencieux. Madeleine avait pris
un ouvrage et travaillait, silencieuse aussi, tout près de lui. Quand
elle levait les yeux sur lui, il souriait encore ; parfois il paraissait sur
le point de lui parler. Finalement, il continuait de se taire. Son lit, où il
avait senti, la veille, perler sur son visage la sueur mortelle, lui faisait
peur ; il refusa de se recoucher selon l’habitude, pour prendre son
repas du soir. Il dîna comme il avait déjeuné, tête à tête avec l’ange,
dans le petit salon. Là, il s’égaya un peu : cette séduction du geste,
de la voix et des mots à laquelle si peu de femmes avaient su
résister, il la déploya pour l’humble fille qui était toute conquise, prête
à lui sacrifier sa vie, et plus que sa vie. Mais il ne disait toujours pas
ce qui le hantait, et Madeleine n’arrivait pas à le deviner. Il se décida
pourtant :
— La nuit dernière, dit-il, si je n’avais pas eu tes mains et ta voix,
je crois que j’aurais étouffé de désespoir. Mais sais-tu le plus grand
bien que tu m’aies fait ?
— Non…
— Eh bien… C’est tantôt… quand tu as mis tes lèvres sur mon
front.
Elle devint pourpre.
— Oh ! vous ne dormiez pas ! c’est mal.
Mais comme elle disait cela, elle sentit poindre en elle un trouble
singulier, où il y avait de l’inquiétude et du bien-être.
D’une voix qui tremblait et se trouait comme celle d’un
adolescent épris, il chuchota, près d’elle :
— Alors ?… Tout le ravage que la souffrance a creusé dans mon
pauvre visage ne t’éloigne pas de moi ?
Elle répondit :
— Bien avant de vous connaître, j’ai aimé votre visage.
Il ne comprit pas : il ne pouvait pas comprendre. Que de paroles
prononcées par cette enfant lui demeuraient inexplicables et dont le
sens mystérieux lui imposait cependant ! Il l’attira contre lui et, de
ses lèvres fermées, effleura sa bouche close ; un grand
frémissement le convulsa. Elle, au contraire, soudain anxieuse,
sentit s’évanouir l’émoi de tout à l’heure.
— Allons, dit-il, appelle pour qu’on me déshabille et qu’on me
couche. Tu ne me quitteras pas ? Tu resteras près de moi comme
hier ?
Elle eut un rire qui l’enchanta, en disant :
— Vous le savez bien !
Depuis que la blessure était cicatrisée, c’était le valet de chambre
qui le dévêtait, aidait à sa toilette et lui passait son pyjama de nuit. Il
fit rappeler Madeleine quand il fut couché. Elle eut la surprise de le
trouver calme ; elle ne se doutait pas qu’elle avait cicatrisé d’un mot,
tout à l’heure, une blessure plus douloureuse que celle du stylet : la
blessure faite au prince par Stéphanie quand, au contact de son
visage, elle avait laissé percer sa répugnance… A présent, le prince
se complaisait à penser : « Un jeune être sain et sincère comme
cette enfant a du plaisir à me regarder, à mettre ses lèvres sur ma
tempe. » Il fut tendre et simple avec elle ; il s’inquiéta de sa fatigue,
et comme, tout en lui tenant les mains, il la voyait fléchir sous le
sommeil, il lui dit :
— Je me sens bien et je suis sûr de m’endormir. J’exige que tu
ailles te reposer dans ta chambre et dans ton lit. Je ne veux pas
abîmer mon ange.
Elle résista, mais il tint bon. Elle le signa de son pouce sur le
front, puis, brisée et comme grisée de fatigue, elle gagna docilement
sa chambre et son lit.
Elle dormit enfin ; elle dormit longtemps. D’abord d’une torpeur
où se dissolvait l’extrême lassitude de son corps, puis d’un sommeil
moins opaque, où transparurent les souvenirs de cette émouvante
journée. Elle revécut le plus doux de tous, quand la tête de son
maître, de son enfant, reposait sur elle. De nouveau, elle osait lui
presser le front de ses lèvres, et son bonheur grandissait à mesure
que leurs deux cœurs s’approchaient de battre d’accord… Quel
sommeil pourrait résister à tant de joie ! Le voile peu à peu s’amincit.
Est-ce qu’elle dort ? Elle a peine à ressaisir la réalité des choses.
Non, elle ne dort plus. Elle est toujours étendue dans son lit, et
pourtant sa bouche est sur le front du maître, et le rythme de leurs
deux vies palpite à l’unisson. Il dit tout bas :
— Si tu m’ordonnes de partir, je partirai.
Elle le serre plus tendrement encore ; il est immobile ; il ne parle
plus… Voici qu’il s’assoupit de nouveau, et qu’elle-même, une douce
torpeur la reprend…
Comment son innocence pourrait-elle pressentir et craindre la
puissance magnétique du sommeil à deux et le déchaînement des
forces de l’amour, alors que la conscience ne les contrôle plus ?

Une des plus étranges désharmonies de l’homme, n’est-elle pas


que, détenant une parcelle du pouvoir de création et de continuité,
— hors de quoi il ne marque sur les choses qu’une empreinte frêle
et caduque, — l’exercice de ce pouvoir formidable soit pour lui un
objet de dévergondage, de vergogne ou d’ironie ? Son exaltation
d’un instant, on dirait qu’il la désavoue : il rougit d’avoir été dieu.
Mais, qu’il y consente ou non, la communion absolue d’un autre être
et de lui, si fortement proclamée dans les écritures, est irrévocable :
ils seront deux dans une seule chair. Communion que les
participants peuvent renier ou rompre. S’ils l’accueillent au contraire
(et c’est le propre de l’amour), elle va bien au delà de la chair, et « ils
sont deux dans un seul esprit ».

Le jour était haut quand le prince Paul rouvrit les yeux. La


chambre de sa gardienne l’environnait. Son premier regard l’aperçut
vêtue de son costume d’infirmière, agenouillée au chevet : on ne
voyait que le haut de son voile blanc d’où les cheveux blonds
débordaient, et un peu de son front. Ses mains se croisaient
étroitement sur sa figure. L’âme du Don Juan meurtri et délaissé
s’imprégnait désormais d’un peu de l’âme de l’ange. Il laissa monter
en lui le flot de tendresse et de pitié. Il dit le nom de l’ange, très bas.
Elle libéra aussitôt son visage de ses mains et leva vers lui des yeux
humides, mais sans tristesse. Quelques instants, ils ne purent se
parler. Ce fut elle qui, devinant son anxiété et soucieuse qu’il ne
souffrît point, lui entoura la tête de ses bras et reposa ses lèvres sur
sa tempe. Au bout de quelques instants, il osa dire :
— Est-ce que tu me pardonnes ?
Elle ne put répondre, mais elle le serra plus étroitement.
Après un silence, il dit encore :
— Je voudrais vivre…
Les lèvres quittèrent son front et juste contre son oreille,
murmurèrent :
— Vous êtes tout près de croire que rien ne peut plus nous
séparer.
— C’est vrai.
Une tendresse, où les sens n’avaient aucune part, les tenait unis
dans un inconcevable apaisement. Ils pensèrent en même temps
qu’une chose s’était accomplie, dans l’ordre des desseins
immuables, qui ne pouvait pas ne pas s’accomplir.
Alors, le prince, se soulevant à demi, dit à voix basse :
— Rien de mon passé ne compte auprès de ce que tu m’as
donné… Mais toi ? Mais toi !…
Elle ne rougit pas, elle ne détourna pas les yeux !
— J’ai connu un bonheur qui n’est pas de la terre… Voilà mon
remords.
De grosses larmes jaillirent de ses yeux, et elle s’abattit en
sanglotant sur le cœur de son ami. Alors le désir éperdu de la
consoler lui suggéra ces paroles :
— Tu sais ce que tu m’as demandé, un jour, de te jurer sur ma
propre tête ?… et je n’ai pas répondu ?
Elle fit signe que oui.
— Eh bien !… dispose de moi selon ton cœur.
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