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Journal of the Optical Society of America B

Exact optical master equations for non-Markovian dephasing in small molecules

W. Vogel

Published Jan 1, 1991• 0 citations
Publisher

Abstract

Generalized optical master equations are derived that describe extremely non-Markovian dephasing phenomena in small, laser-driven molecules. These equations are exact in the sense that no Born approximation or related approximation scheme is applied. Effects of non-Markovian dephasing on the intensity of light scattering are briefly discussed.

DOI
10.1364/josab.8.000129

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Generalized optical master equations are derived that describe extremely non-Markovian dephasing phenomena in small, laser-driven molecules. These equations are exact in the sense that no Born approximation or related approximation scheme is applied. Effects of non-Markovian dephasing on the intensity of light scattering are briefly discussed.
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Non-Markovian master equations describe general open quantum systems when no approximation is made. We provide the exact closed master equation for the class of Gaussian, completely positive, trace preserving, non-Markovian dynamics. This very general result allows us to investigate a vast variety of physical systems. We show that the master equation for non-Markovian quantum Brownian motion is a particular case of our general result. Furthermore, we derive the master equation unraveled by a non-Markovian, dissipative stochastic Schrödinger equation, paving the way for the analysis of dissipative non-Markovian collapse models.
Driven quantum systems subject to non-Markovian noise are typically difficult to model even if the noise is classical. We present a systematic method based on generalized cumulant expansions for deriving a time-local master equation for such systems. This master equation has an intuitive form that directly parallels a standard Lindblad equation, but contains several surprising features: the combination of driving and non-Markovianity results in effective time-dependent dephasing rates that can be negative, and the noise can generate Hamiltonian renormalizations even though it is classical. We analyze in detail the highly relevant case of a Rabi-driven qubit subject to various kinds of non-Markovian noise including 1/f fluctuations, finding an excellent agreement between our master equation and numerically-exact simulations over relevant timescales. The approach outlined here is more accurate than commonly employed phenomenological master equations which ignore the interplay between driving and noise.
We discuss the use of the Born and Markov approximations in describing the dynamics of an atom laser. In particular, we investigate the applicability of the quantum optical Born-Markov master equation for describing output coupling. We derive conditions based on the atomic reservoir, and atom dispersion relations for when the Born-Markov approximations are valid and discuss parameter regimes where these approximations fail in our atom laser model. Differences between the standard optical laser model and the atom laser are due to a combination of factors, including the parameter regimes in which a typical atom laser would operate, the different reservoir state which is appropriate for atoms, and the different dispersion relations between atoms and photons. We present results based on an exact method in the regimes in which the Born-Markov approximation fails. The exact solutions in some experimentally relavent parameter regimes give non-exponential loss of atoms from a cavity.
Non-Markovian quantum evolution of the electronic subsystem in a laser-driven molecule is characterized through the appearance of negative decoherence rates in the canonical form of the electronic master equation. For a driven molecular system described in a bipartite Hilbert space H=Hel⨂Hvib\mathcal{H}={\mathcal{H}}_{el}⨂{\mathcal{H}}_{\mathrm{vib}}H=Hel​⨂Hvib​ of dimension $2\ifmmode\times\else\texttimes\fi{}{N}_{v}$, we derive the canonical form of the electronic master equation, deducing the canonical measures of non-Markovianity and the Bloch volume of accessible states. We find that one of the decoherence rates is always negative, accounting for the inherent non-Markovian character of the electronic evolution in the vibrational environment. Enhanced non-Markovian behavior, characterized by two negative decoherence rates, appears if there is a coupling between the electronic states g,eg,\phantom{\rule{0.16em}{0ex}}eg,e, such that the evolution of the electronic populations obeys d(PgPe)/dt>0d({P}_{g}{P}_{e})/dt>0d(Pg​Pe​)/dt>0. Non-Markovianity of the electronic evolution is analyzed in relation to temporal behaviors of the electronic-vibrational entanglement and electronic coherence, showing that enhanced non-Markovian behavior accompanies entanglement increase. Taking as an example the coupling of two electronic states by a laser pulse in the Cs2{\mathrm{Cs}}_{2}Cs2​ molecule, we analyze non-Markovian dynamics under laser pulses of various strengths, finding that the weaker pulse stimulates the bigger amount of non-Markovianity. Our results show that increase of the electronic-vibrational entanglement over a time interval is correlated to the growth of the total amount of non-Markovianity calculated over the same interval using canonical measures and connected with the increase of the Bloch volume. After the pulse, non-Markovian behavior is correlated to electronic coherence, such that vibrational motion in the electronic potentials which diminishes the nuclear overlap, implicitly increasing the linear entropy of entanglement, brings a memory character to dynamics.
The non-Markovian master equation for open quantum systems is obtained by generalization of the standard Zwanzig-Nakajima (ZN) projection technique. To this end, a coupled chain of equations is written for the reduced density matrices of the bath ϱB(t) and of the system ϱS(t). A formal solution of the equation for ϱB(t) in the 2nd approximation in interaction yields a specific extra term related to the intrinsic bath dynamics. This term is nonlinear in the reduced density matrix ϱS(t), and vanishes in the Markovian limit. To verify the consistence and robustness of our approach, we apply the generalized ZN projection scheme to a simple dephasing model. We study the obtained kinetic equation both in the Markovian approximation and beyond it (for the term related to the intrinsic bath dynamics) and compare the results with the exact ones.