Leer 3
Leer 3
Leer 3
controlled by a coherent driving field which acts on each resonance frequencies (Fig. 1(b)). In particular, we ac-
of the molecules with a coupling amplitude h`i = −µi ·Ei , count for the fluorescence spectrum measured for the pair
and a frequency ωL . The light-matter interaction Hamil- of coupled molecules reported in Ref. [22].
(i) (i)
tonian ĤL = h`(i) (σ− eiωL t + σ+ e−iωL t ), where µi is the Our calculations are performed in the standard two-
i-th transition dipole moment and Ei is the amplitude of qubit computational basis {|00i, |01i, |10i, |11i} (|iji ≡
the coherent driving acting on molecule i (at ri ). |i1 i ⊗ |j2 i), and the corresponding dimer density matrix
The dimer dissipative dynamics is appropriately de- elements are denoted as ρij,kl , with associated popula-
scribed within the Born-Markov formalism, with Ĥ = tions ρij,ij (density matrix elements |ijihij|), i, j = 0, 1.
ĤS + ĤL , by the quantum master equation The calculations here presented are amenable to experi-
mental verification in a dimer molecular set-up where the
i task of optically resolving the single molecules by means
ρ̇ˆ = − Ĥ, ρ̂ + L(ρ̂),
(1)
~ of laser spectroscopy techniques is possible. This kind of
experiment has been performed, for instance, by Hettich
with dissipative Lindblad super-operator given by [24] et al. [22], and the detection and measurement of cou-
pled single terrylene molecules embedded in an organic
Γ1 (1) (1) (1) (1) (1) (1)
(para-terphenyl) crystal (thickness of about 250 nm) has
L(ρ̂) = − ρ̂σ+ σ− + σ+ σ− ρ̂ − 2σ− ρ̂σ+ (2)
2 been reported. There the detection was carried out by
Γ2
(2) (2) (2) (2) (2) (2)
means of fluorescence excitation spectroscopy at a tem-
− ρ̂σ+ σ− + σ+ σ− ρ̂ − 2σ− ρ̂σ+
2 perature ∼ 1.4 K. Such a recorded fluorescence spectra,
Γ12 (1) (2) (1) (2) (1) (2)
at high excitation laser intensity, exhibits the appearance
− ρ̂σ+ σ− + σ+ σ− ρ̂ − 2σ− ρ̂σ+
2 of an ‘additional’ peak between those associated to the
Γ21 (2) (1) (2) (1) (2) (1)
individual transition frequencies ν1 , and ν2 , which is the
− ρ̂σ+ σ− + σ+ σ− ρ̂ − 2σ− ρ̂σ+ , experimental evidence of the dipole-dipole coupling V12
2
between the qubits.
where Γii ≡ Γi = nA12;i /2 = nωi3 kµk2 /(30 hc3 ) are the The continuous curves shown in Fig. 1(a) are in perfect
spontaneous emission rates (A12;i , i = 1, 2 are the Ein- agreement with the experimental results reported in [22],
stein vacuum coefficients), n is the refraction index of the for the same set of implemented physical parameters:
dispersive medium in which the molecules are embed- difference in dipole transition frequencies ∆− = 2320
ded (for example, a paraterphenyl crystal in [22]), and MHz, dipolar coupling strength V12 = 950 MHz, indi-
Γ12 = Γ∗21 are the collective spontaneous emission rates, vidual and collective decay rates Γ1 = Γ2 = 2π × 50
arising from the coupling between the molecules through MHz, Γ12 = 2π × 9 MHz; with ∆e = −160 MHz, for a
(i) (i)
the vacuum field [24]; σ+ = |1i ih0i |, and σ− = |0i ih1i | laser coupling `i = 200 MHz. Here, we have calculated,
are the raising and lowering Pauli operators acting on directly from Eq. (1), the steady state occupation prob-
molecule i. abilities for the states |01i, |10i, and |11i as a function of
In particular, in the near field approximation (r12 the laser detuning. We can also see from Fig. 1(a), the
λL ) theh d-d interaction energy is given i by hV12 = effect due to a different dipolar coupling, as shown by the
√
3h Γ1 Γ2
µ̂1 · µ̂2 − 3(µ̂1 · r̂12 )(µ̂2 · r̂12 ) , and Γ12 = dashed curves, for V12 = 50 MHz. Since this implies a
8πz 3
√ change in the relative position of the coupled dipoles, this
Γ1 Γ2 µ̂1 · µ̂2 : the maximum (minimum) interaction is reflected in a shift of the resonant peaks at frequencies
strengths V12 are obtained for parallel (perpendicular) ν1 , and ν2 , and a decreasing of the signal intensity com-
dipole moments [33]. z ≡ nk0 r12 ; µ̂i , and r̂12 are unit ing from the two-photon emission process (intermediate
vectors along the transition dipole moments and along peak) due to the weaker dipolar coupling.
the relative separation between the molecules. The case of molecules with equal transition frequen-
We stress that Eq. (1) is more general than that used cies (∆− = 0) is illustrated by the continuous curves in
in [11, 15] in the sense that it accounts for qubit-qubit Fig. 1(b), for V12 = 950 MHz. As expected, only two
coupling, coherent external driving, and nonlocal fluctu- peaks appear: one associated to the resonance condition
ations due to radiative corrections [24]. ν1 = ν2 , and the intermediate one, associated to the dipo-
lar coupling. By bringing the dipoles into resonance, a
clear increment in the two-photon resonance signal, in
III. RESONANCE FLUORESCENCE comparison to the experimentally measured spectra [22]
(calculated as the dashed curve in Fig. 1(b)) is observed,
To evaluate the system’s physical observables, we per- thus indicating a stronger dipole-dipole coupling.
form the calculation of the occupation probabilities in The resonance fluorescence spectrum reported in [22]
the steady state. We compute this for several different can be theoretically reproduced by plotting the steady
experimental conditions realizable in the laboratory, as state quantity ρ01,01 + ρ10,10 + 2ρ11,11 , as shown in Fig.
shown in Fig. 1. These involve weak and strong coherent 1(c). This shows the appearance of the two-photon reso-
laser driving (e.g., Fig. 1(c)), different dipole interaction nance as the laser excitation intensity is increased. This
strengths (Figs. 1(a), and 1(d)), and different dimer’s peak is shifted from the laser detuning ∆+ = 0 due to the
3
FIG. 1: Steady state occupation probabilities for the dimer system. The detunings ∆− ≡ ν1 − ν2 , and ∆+ /2 ≡ (ν1 + ν2 )/2 − νL .
a) Populations ρij,ij for two different dipolar couplings, ∆− = 2320 MHz. b) Probabilities for a fixed dipolar coupling, = 950
MHz, and different molecular resonance conditions. In both cases, Γ1 = Γ2 = 2π ×50 MHz, Γ12 = 2π ×9 MHz, ∆e = −160 MHz
and `i = 200 MHz. c) Fluorescence spectrum given in terms of the occupation probabilities, as a function of the laser coupling
strength and the laser detuning ∆+ /2. In MHz, Γi = 18π, Γ12 = 9π, ∆− = 2320, and ∆e = −160. d) Zoom of the two photon
(intermediate) resonance for `i = 100 MHz.
the vacuum fluctuation noise, an effective shift that has as this allows the initialization of a broad class of en-
been experimentally [22] and theoretically [23] estimated tangled states [11, 14]. In the standard two-qubit com-
at around −160 MHz. The calculations here presented putational basis, the maximally entangled Bell state
have been done for the independent and collective de- |ψ + i = √12 (|01i + |10i) is obtained for a = w = d = 0;
cay rates Γi = 18π MHz, Γ12 = 9π MHz. Figure 1(d) b = c = z = 1/2. All the other states of the Bell basis,
shows a zoom of the intermediate resonance of Fig. 1(c), as well as the Werner mixed state [14] can be produced
for a laser coupling `i = 100 MHz, and different dipolar in a similar manner.
couplings. This shows a clear increment in the size of
the resonance as the qubit coupling is increased. If this
graph were to be calculated for `i = 10 MHz (not shown), A. Coherent control dynamics
the probability of simultaneous excitation ρ11,11 appears
multiplied by the scale factor 10−5 . Hence, the resonance We consider
signal can be tailored according to designed structural √ the dynamics
√ of the initial entangled state
|ψ
√0 (α)i =
√ α|01i + β|10i, where α is a real number,
molecular parameters. The difference in the half-width β = | β|eiφ is a complex number of phase φ, and
of the reported peaks has its origin in the constructive α + |β| = 1. This choice follows the identification of
and destructive interference of the different possible re- the eigenstates of the system’s Hamiltonian ĤS , in the
laxation pathways [25]. absence of external driving. If no cooperative phenomena
due to V12 (decay rate Γ12 ) take place (for example, due
to a long separation between the molecules, V12 ∼ 0),
IV. DIMER ENTANGLEMENT EVOLUTION in the absence of laser driving, the entanglement of this
type of state has a natural asymptotic time decay due to
As a norm for the entanglement quantification of the the emission rates Γii ≡ Γi of the individual molecules.
dipole-coupled molecules, we use Wootter’s concurrence The numerical solution of the master equation (1) al-
C(ρ) = max{0, λ1 − λ2 − λ3 − λ4 }, where the λi ’s are lows the quantification of the dimer entanglement dy-
the square roots of the eigenvalues of the non-hermitian namics, as shown in Fig. 2, where the external field
(1)
matrix ρeρ, arranged in decreasing order, with ρe = σy ⊗ has been used to produce a coherent control of entangle-
(2) ∗ (1) (2)
σy ρ σy ⊗σy [26]. We consider the initial state density ment. Figure 2(a) shows that for a strong laser coupling
matrix (`i = 500 MHz) the concurrence abruptly decays to zero
for a time less than tΓ , where tΓ ≡ 1/Γ is the time asso-
a 0 0 w ciated to the decay rates Γi ≡ Γ for all the initial state
0 b z 0 configurations (all α). In this work, ∆+ , ∆− , ∆e , V12 ,
ρ(0) = , (3)
0 z∗ c 0 and `i are given in frequency (ν ≡ ω/2π) units, whereas
∗ and Γij appear divided by a 2π-factor to consistently give
w 0 0 d
4
√ √ √ √
FIG. 5: Initial state preparation of product states |Ψ0 (γ)i = ( γ|0i + δ|1i) ⊗ ( ζ|0i + η|1i), for a) ζ = 0, b) ζ = 1/2, c)
ζ = 1. ∆− = 2320 MHz, ∆+ = 0. The decay rates Γi = 100π MHz, Γ12 = 18π MHz. `i = 100 MHz, ∆e = −160 MHz, and
V12 = 950 MHz.
FIG. 6: Initial product states |Ψ0 (γ)i (Eq. (5)), in the absence of qubit-qubit interaction and collective decay (V12 = 0, Γ12 = 0),
for a) ζ = 0, b) ζ = 1/2, c) ζ = 1. ∆− = 2320 MHz, ∆+ = 2638 MHz. Γi = 10π MHz, `i = 200 MHz, ∆e = −160 MHz.
∆e –the Lamb shift experienced by the molecular dou- coupling strength for which maximum stationary entan-
bly excited state, and to the external driving field. The glement is generated. Away from this optimal value, the
results are clearly different from those of Fig. 5; even stationary entanglement decreases monotonically until it
though the qubits start from a separable state, they en- reaches a certain intensity from which any entanglement
tangle due to the radiative corrections and the external correlation is washed away and the concurrence goes to
field. The concurrence exhibits a similar behavior for the zero after a few oscillations. This indicates that the laser
conditions a) ζ = 0, and c) ζ = 1, for which there is a can be used to tune and maximize stationary entangle-
maximum amount of generated entanglement, and ESD ment production, given an initial condition.
and collapse-revival behavior are present as a function
of the initial qubit preparation. The scenario ζ = 1/2
(graph 6(b)) does exhibit a different type of decay, and
unlike the previous cases, there are not two “islands” of
entanglement, and the oscillations persist the most for
γ 7→ 1. Notice that the time scale for such oscillations is
much longer than those of the graphs previously shown.
1. Laser coupling
FIG. 7: Concurrence dynamics as a function of the laser inten-
We address the entanglement effects due to the molec- sity `i ≡ `, for the initial condition |Ψ0 (γ)i, with γ = ζ = 1/2.
ular coupling to the laser field, for the initial condition a) V12 = 950 MHz, b) V12 = 50 MHz. ∆− = 2320 MHz,
given by Eq. (5). Figure 7 shows the entanglement evo- ∆+ = 0, Γ = 100π MHz, Γ12 = 18π MHz, ∆e = −160 MHz.
lution as a function of the laser field coupling strength `.
In the figure, γ = ζ = 1/2, and the other parameters are In Fig. 7(b) we have decreased V12 to 50 MHz. In con-
given as in Fig. 5, for a) V12 = 950 MHz, and b) V12 = 50 trast to the previous case, for low laser coupling strength,
MHz. Figure 7(a) shows that for the considered initial there are no entanglement oscillations before the con-
product state of superpositions there is an optimal laser currence reaches its minimum value: the concurrence
7
exhibits an island whose height depends on the laser is in contrast to the revival of entanglement reported in
strength. Unlike the previous case, here the maximum [30], where such a behavior is critically dependent on the
entanglement occurs at low intensity, due to the fact the collective decay. As is shown in our case, the revival phe-
qubit-qubit interaction is smaller than ∆e , which domi- nomenon is strictly induced by the external laser control
nates the dynamics. The entanglement rapidly vanishes and the quantum noise fluctuations given by the Lamb
as the laser intensity increases, with the two-particle state shift [23].
becoming separable during a period whose length in-
creases with the laser intensity. It then starts to build up
towards a stationary degree of entanglement, for which
there is also a maximum value which is directly depen-
dent on the intensity of the laser. After this, the entan-
glement gradually decays as the laser intensity is further
increased (not shown) and eventually vanishes following
a similar pattern to that of Fig. 7(a).
the relevant dynamical decay. An analytical expression for the concurrence, for the
molecular input values of the inset of Fig. 10, follows
from the calculation of the non trivial density matrix
elements found for the solution of the master equation:
ρ00,00 = 1 + (1 − α)e−2Γt 1 − 2eΓt ,
ρ11,11 = (1 − α)e−2Γt ,
p
ρ00,11 = ρ∗11,00 = (1 − α)α eit(2π∆e +iΓ+4π∆+ ) . (6)
The concurrence C(ρ) = 2 max {0, |ρ00,11 | − ρ01,01 }.
Thus, the ESD time can be directly obtained from the
condition |ρ00,11 | − ρ01,01 ≤ 0; for any α < 1/2, this reads
1 1−α
t̃α = ln √ . (7)
Γ 1−α− α−α 2
FIG. 10: Comparison between the effects due to the laser and
the vacuum fluctuations over the entanglement dynamics. In For α ≥ 1/2 there exists no solution with physical mean-
the main graph, the solid curve exhibits collapses and revivals; ing for t̃α , in agreement with what is shown in the inset
`i = 200 MHz, ∆e = −160 MHz. The long dashed curve of Fig. 10. An experimental study on the engineering
exhibits ESD; `i = 200 MHz, ∆e = 0. The short dashed
and modification of the molecules decay rates has already
curve corresponds to `i = 1 MHz, and ∆e = −160 MHz. The
initial state is |ψ0 (1/2)i. The remaining parameters used in been reported [32]; this could facilitate the observation
the simulations are of the effects reported in Figs. 9 and 10.
√ the same √ as in Fig. 9. By switching to
the initial state α|00i + β|11i, the inset shows the ESD
sensitivity to the initial condition; ∆+ = 20000 MHz, ∆e =
−160 MHz, and `i = 0; the other parameters are as in Fig. 9. V. CONCLUSIONS
We have plotted, in Fig. 10, the dynamics of the con- We summarize the major findings of the present work
currence for the initial entangled state |ψ0 (α = 1/2)i, on dimer entanglement dynamics. We have shown how
to show the interplay between the laser driving and the entanglement evolution, which includes ESD, ESB,
the shift experienced by the doubly excited state due and collapse-revival dynamics, can be precisely controlled
to background noise fluctuations. The concurrence de- by means of an external driving field, and an appropriate
cays asymptotically when the laser coupling is absent, in qubit initialization. In addition, the light-matter inter-
agreement with our previous results. action can be used to produce transitions between the
The main graph of Fig. 10 also shows sudden dis- system states in such a way that a reliable production of
entanglement (but not revival) when the laser coupling steady state entanglement is favored. There are entan-
is strong and there is no contribution arising from the glement dynamics corrections due to the radiative shift of
vacuum noise (long dashed curve). This behavior is also the doubly-excited molecular state arising from the vac-
observed uum fluctuations: in the scenario where the qubits do not
√in the inset
√ of Fig. 10, for a different initial con-
dition, α|00i + β|11i: the ESD is more pronounced experience collective coupling effects (only independent
when α tends to zero, and it vanishes for α > 1/2. This interaction with the environment), the entanglement ex-
is because in our density matrix configuration, ρ00,00 cor- hibits a collapse-revival behavior. On the other hand, by
responds to the lowest system eigenstate in the standard considering different type of initial conditions, an ESD
basis, and hence, for α → 1, the system has a higher dynamics can also be induced due to the energy shift.
probability of decaying to the ground state and the in- We have shown that it is crucial, for a correct character-
teresting quantum effects are lost. ization of entanglement dynamics, to take into account
The sensitivity of the ESD dynamics to the initial con- the radiative corrections induced by the electromagnetic
ditions is shown in the inset of Fig. 10. In the main fig- vacuum field, as such shifts or energy corrections perma-
ure, the entanglement decays asymptotically (uppermost nently affect the evolution of entanglement.
√ √
curve, ` = 1) for the initial conditions α|01i + β|10i
(for all α), and hence ESD never takes place. However,
the VI. ACKNOWLEDGEMENTS
√ inset of √ Fig. 10 shows that for the initial condition
α|00i + β|11i, and absence of laser driving, the en-
tanglement decays abruptly for values of α close to zero, This work was partially supported by Colciencias
and hence ESD is reinforced at very early times t̃. This Grant 1106-452-21296, and the DAAD-Colciencias ex-
clearly indicates that different types of initial entangled change (PROCOL) program. We acknowledge the hos-
states experience different input noise from the environ- pitality of the Freiburg Institute for Advanced Stud-
ment. ies, and the Max Planck Institute for the Science of
9
Light Erlangen, where parts of this work were com- Award (A/09/0851). We would like to acknowledge L. L.
pleted. JHR is grateful to the DAAD for a Research Stay Sánchez-Soto for a critical reading of the manuscript.