Ultrafast Laser Physics!

Ursula Keller / Lukas Gallmann

ETH Zurich, Physics Department, Switzerland

www.ulp.ethz.ch

Chapter 10: Ultrafast Measurements

Ultrafast Laser ETH Zurich

Physics
Ultrafast laser physics (ULP)

Time

1as!

1 picosecond = 1 ps = 10–12 s
1 femtosecond = 1 fs = 10–15 s
1 attosecond = 1 as = 10–18 s

Length

1am!
 Measurement with !s time resolution

Harold E. Edgerton, MIT"

1903-1990"
!

Flash photography: !
Flash lights driven by
electronics !

triggered flash lights "

#µs time resolution "
(already available 1935)"
limited by flash duration "
(„light pulse duration“)!
 The problem
•$ Straightforward: Measure
slow event with fast event

•$ However, all detectors are

time-integrating on these
time scales
E. Muybridge: Animal Locomotion (1887)

•$ Solution: Map dynamics/

time axis to static
observable!
 The solution
•$ The classical pump-probe approach:

2"x
•$ Map time to translation in space: ! = # "x
c
•$ Therefore S(!x) " S(# )
•$ 1 nm resolution in !x yields 7 as resolution in !
•$ Delay is equivalent to real time if duration of probe pulse is
negligible and process is perfectly reproducible
•$ This idea can be generalized to other mappings of time to
time-independent quantities
Pump-Probe Measurement

!t

!z = 1 µm " !t # 2 $ 3.3 fs
2
!z = c!t!
 Ultrafast Pump-Probe Techniques
Differential Transmission Spectroscopy
probe device
under test
photo
detector
pump (PD)
Laser
beam chopper "t
splitter
!c
JPD noise of probe

signal
signal = [T("t, Ipump) – T(Ipump = 0)] Iprobe

!c !
Transmission of device under test with
• Why a chopper?
pump on pump off
• Why not the chopper in the probe pulse?
• Why do you use a lock-in amplifier?
 Ultrafast Pump-probe Techniques
Differential Transmission Spectroscopy
probe device
under test
photo
detector
pump (PD)
Laser
beam chopper "t
splitter
!c
JPD noise of probe

signal
signal = [T("t, Ipump) – T(Ipump = 0)] Iprobe

!c !
Transmission of device under test with
pump on pump off

Ultrafast measurements need some kind of nonlinearities in the

measurement system (i.e. intensity dependent transmission)
 Different arrangements

•$ Noncollinear degenerate pump-probe

measurements
•$ Collinear degenerate pump-probe
measurements
 Noncollinear degenerate pump-probe

CHOPPER "Langsamer" Detektor

LINSE (zeitlich gemittelt)
PUMP
k1

PROBE k2
!t
SAMPLE
Polarisation

Noncollinear: pump and probe beam not collinear

good for signal-to-noise because pump power is not on detector

Degenerate: pump and probe pulse have the same central wavelength
 Collinear degenerate pump-probe

Polarisation LOCK-IN
VERSTÄRKER
PROBE PUMP bei f1
CHOPPER
bei f1 PBS
PUMP

!t
PBS
SAMPLE
PROBE
LINSE

What is the reason for the PBS (polarizing beam splitters) in the set-up?
 Collinear degenerate pump-probe
Polarisation LOCK-IN
VERSTÄRKER
PROBE PUMP bei f1
CHOPPER
bei f1 PBS
PUMP

!t
PBS
SAMPLE
PROBE
LINSE

LOCK-IN
Polarisation VERSTÄRKER
PROBE PUMP bei f1œ
- f2
CHOPPER
bei f1 STRAHL-
TEILER
PUMP

!t
SAMPLE
CHOPPER
bei f2 LINSE

PROBE

Potential problem? Detector can be saturated by strong pump beam.

 Degenerate four-wave mixing
"Langsamer" Detektor
E1

PUMP

k1

E2 k2
SAMPLE
PROBE

Polarisation => Beugungsgitter

Why is this set-up a degenerate four-wave mixing experiment?

 Degenerate four-wave mixing
"Langsamer" Detektor
E1

PUMP

k1

E2 k2
SAMPLE
PROBE

Polarisation => Beugungsgitter

Parallel polarization creates a transient diffraction grating inside the sample.

This grating exists as long as there is a coherent excitation (i.e. within the
dephasing time)
Review articles: K.-H. Pantke und J. M. Hvam, "Nonlinear quantum beat spectroscopy in semiconductors,"
Int. J. of Modern Physics B, 8, 73-120, 1994
E. O. Göbel, "Ultrafast Spectroscopy of Semiconductors," Festkörperprobleme, Advances in Solid State Physics,
30, S. 269-294, 1990
J. Shah, "Ultrafast Spectroscopy of Semiconductors," Springer-Verlag
Degenerate four-wave mixing
"Langsamer" Detektor
E1

PUMP

k1

E2 k2
SAMPLE
PROBE

Polarisation => Beugungsgitter

LINSE
PUMP SAMPLE
k1

PROBE
k2
!t
Polarisation 2k 2 - k 1

"Langsamer" Detektor
 Optical Gating

NICHTLINEARER
SIGNAL KRISTALL
k1

PROBE
k2
!t
LINSE
LANGSAMER
DETEKTOR

Application: time resolved femtosecond luminescence measurement

T. C. Damen and J. Shah, "Femtosecond luminescence spectroscopy with 60 fs compressed pulses,"
Applied Phys. Lett. 52, 1291, 1988
J. Shah, "Ultrafast Luminescence Spectroscopy using sum frequency generation,"
IEEE JQE, 24, 276-288, 1988
 Optical Gating: Time-of-flight imaging
Laserpuls Starke
Streuung durchgelassener
Laserpuls

Abtasten Lichtanteil mit

Biologisches wenig Streuung
Gewebe => Abbildung

NICHTLINEARER
SIGNAL KRISTALL
k1

PROBE
k2
!t
LINSE
LANGSAMER
DETEKTOR
Application of optical gating for “time-of-flight” imaging
M. R. Hee, J. A. Izatt, J. M. Jacobson, J. G. Fujimoto, "Femtosecond transillumination optical
coherence tomography," Optics Lett., vol. 18, pp. 950-952, 1993
 Optical coherence tomography (OCT)

Science, 254, 1178, 1991!

How does this work?

Optical coherence tomography (OCT)

Michelson Interferometer

Interference only within

coherence length

Science, 254, 1178, 1991!

 Optical coherence tomography (OCT)

30 fs pulse duration -> 10 µm axial resoluton "

10 fs pulse duration -> 3 µm axial resolution "

Prof. J. G. Fujimoto, MIT, USA"

 Time resolved four-wave-mixing

LINSE
PUMP SAMPLE
k1

PROBE
k2
!t
Polarisation 2k 2 - k 1

"Langsamer" Detektor

How do you do time resolved four-wave mixing?

 Time resolved four-wave-mixing

Polarisation LINSE
PUMP SAMPLE
k1

PROBE #1
k2
!t1
2k 2 - k 1 NICHTLINEARER
KRISTALL

PROBE #2
!t2
LINSE
LANGSAMER
DETEKTOR
 Photoconductive Switching

Laserpuls

Output

Photoconductive switch or Auston switch:

D. H. Auston, "Picosecond optoelectronic switching and gating in silicon,"
Appl. Phys. Lett., vol. 26, pp. 101-103, 1975
D. H. Auston, P. Lavallard, N. Sol, D. Kaplan, "An amorphous silicon photodetector for picosecond pulses,"
Appl. Phys. Lett., vol. 36, pp. 66-68, 1980
 Photoconductive Switching
+V
I (t)

Z0 Z0

I (t + !)

OUT

Photoconductive sampling gate

D. H. Auston, A. M. Johnson, P. R. Smith, J. C. Bean,
"Picosecond optoelectronic detection, sampling, and correlation measurements in amorphous semiconductors"
Appl. Phys. Lett., vol. 37, pp. 371, 1980
 High-order harmonic generation in gases
Spectrum of harmonics
Log(Strength)

Plateau
Cutoff

Harmonic order P. B. Corkum, Phys. Rev. Lett. 71, 1994 (1993)

Classical electron-trajectories
! Multiple trajectories with same recombination energy but different excursion time exist

HHG
tr
+
ti !1 !2
Short Long
trajectory trajectory
 HHG and attosecond science
Laser-based Intense ultrafast Ti:sapphire CPA (!800 nm, > 300"J)
pulse repetition rate: "1 kHz (moving towards 10 kHz)
HHG pulse energy center: up to 100 eV
pulse energy of attosecond pulses: < nJ
pulse duration: "100 as

Laser-based HHG: “a success story”

Femtosecond domain:
nJ pulses at 100 MHz
100 mW average power

Attosecond domain:
nJ pulses at 1 kHz
1 !W average power

Challenges/Problems of laser based HHG:

Low pulse repetition rates and low pulse energy!
limits signal-to-noise ("5 orders of magnitude reduction)
 Streaking techniques instead of pump-probe
attosecond resolved measurements strongly signal-to-noise limited
use phase sensitive techniques instead:
energy streaking: mapping time to energy
angular streaking: mapping time to angular momentum
attosecond pulse synchronized with strong infrared field
strong infrared field can be used for streaking
energy streaking: mapping time to energy (linear polarized streaking field)
[1] R. Kienberger et al., Science, 207, 1144 (2002)
[2] R. Kienberger et al., Nature, 427, 817 (2006)
[3] E. Goulielmakis et al., Science, 305, 1267 (2004)
 Attosecond streak camera
•$ Most versatile and most successful technique to date:
Attosecond streak camera Hentschel et al., Nature 414, 509 (2001)
1.$ The attosecond pulse and an intense, short infrared pulse are overlapped in/on
a medium being studied – they can be delayed with respect to each other
2.$ The attosecond pulse ionizes the medium
3.$ The vector potential of the infrared pulse shifts the resulting electron spectrum
in energy as a function of the relative delay

Measured at ETH, 2012

 Streaking techniques instead of pump-probe
attosecond resolved measurements strongly signal-to-noise limited
use phase sensitive techniques instead:
energy streaking: mapping time to energy
angular streaking: mapping time to angular momentum
attosecond pulse synchronized with strong infrared field
strong infrared field can be used for streaking
angular streaking: mapping time to angular momentum (circular polarized)

time measurement
=
angle measurement

no as pulses!
5 fs

P. Eckle, A. Pfeiffer, C. Cirelli, A. Staudte, R. Dörner, H.-G. Muller, M. Büttiker, U. Keller,

Science 322, 1525, 2008
 Delay in tunnel ionization
How long does it take for an electron to traverse the
tunneling barrier in tunnel-ionization of helium?

A. S. Landsman, M. Weger, J. Maurer, R. Boge, A. Ludwig, S. Heuser, C. Cirelli, L. Gallmann, U. Keller

Optica 322, 1525 (2008)
30!
and much more ….