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Physical Review A

Relaxation of quantum systems weakly coupled to a bath. II. Formal analysis of the total-time-ordering-cumulant and partial-time-ordering-cumulant spectral line shapes

J. Bretón, Arturo Hardisson, F. Mauricio, Santiago Velasco

Published Jul 1, 1984• 22 citations
Publisher

Abstract

Given a quantum system of a few degrees of freedom in weak interaction with a bath, the expressions which connect its total-time-ordering-cumulant and partial-time-ordering-cumulant relaxation with the corresponding spectral line shapes of dipolar absorption are deduced. For simplicity we consider a system with a nondegenerate and nonequidistant energy spectrum. A special study in the cases of isolated resonances and of a weak interference effect between resonances is made.

DOI
10.1103/physreva.30.553

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Physical Review A•May 1, 1979•48 citations
Given a quantum system of a few degrees of freedom in weak interaction with a bath, the expressions which connect its total-time-ordering-cumulant and partial-time-ordering-cumulant relaxation with the corresponding spectral line shapes of dipolar absorption are deduced. For simplicity we consider a system with a nondegenerate and nonequidistant energy spectrum. A special study in the cases of isolated resonances and of a weak interference effect between resonances is made.
The present paper studies the formal aspects of the total-time-ordering-cumulant (TTOC) and the partial-time-ordering-cumulant (PTOC) relaxations of a quantum system, of few degrees of freedom, in weak interaction with a bath, both within and outside the Markovian limit. To this end, the general expressions connecting the matrix elements of the TTOC and PTOC relaxation superoperators with the bath correlation functions are determined. Special attention is paid to two particular cases: a system with a nonequidistant energy spectrum and a system with an equidistant energy spectrum. Discussions revolve mainly around the possibility of applying the secular approximation to the TTOC and PTOC master equations for the off-diagonal matrix elements of the reduced-density operator of the system.
We consider light scattering from a multilevel system (e.g., a molecule) interacting with several heat baths. The Liouville space approach is employed and weak incident radiation intensity is assumed, whereas the light scattering process is described in the lowest appropriate order in the interaction between the molecule and the incident and emitted photons. The interaction with other radiation field modes as well as with the thermal baths is treated more fully, such as to account for the correct damping terms and their temperature dependence. The formalism is suited for light scattering from an impurity molecule in both gas and dense phases. The thermal baths induce relaxation within the manifold of excited states as well as transitions to nonradiative channels. Damping due to such transitions (as well as radiative damping) corresponds to interactions with zero temperature baths. The physical interpretation of such a bath depends on the nature of the particular damping process. Thermal relaxation within the excited manifold is induced by interaction with the environment represented by a bath of temperature T. Part of this interaction which is diagonal in the molecular space corresponds to the so-called ’’quasielastic collisions’’ and induces modulations of the molecular energy levels and broadening of the relaxed emission. The remainder, nondiagonal part induces actual transitions between the excited molecular energy levels. The formalism yields in a single calculation expressions for the cross section for both the coherent (Raman) scattering process and the relaxed luminescence and enables us to discuss the effects of different factors such as temperature and quenching processes on the relative yields for these processes. The formalism also allows for interference between different levels of the excited manifold due to coupling of several levels to the same bath, and makes it possible to study the effect of thermal relaxation on these interference phenomena.
A general form of admittance is derived using the relaxation method under thermal equilibrium initial conditions from a second-order TCL equation with no external driving terms. Its admittance is shown to include the two interference terms in the TCLE method (method of TCL equations with external driving terms). Effects of the first and second interference terms in the TCLE method are numerically discussed for a quantal spin (magnitude 1/2) interacting with a spin-like bath and with a boson-like bath, respectively. It is shown that the first interference term which represents effects of the initial correlation and which is neglected in the relaxation method under decoupled initial conditions of the spin and bath, produces the effects which enhance the peaks of line shapes slightly and which abase the line shapes at the small frequency region, and becomes larger as the characteristic frequency of the heat bath becomes smaller.
The problem of resonant interaction between an electromagnetic radiation field and a vibronic system, such as a molecule or a localized electronphonon system, is considered. The vibronic coupling is assumed to result from displaced and distorted potential energy surfaces for the vibrational motion in the electronic quantum states involved in the resonant interaction with the radiation field. Furthermore, the vibrational energy relaxation is taken into account without assumptions about Markovian-type relaxation. In order to study correlation properties of higher than second order in the electric field strength of the light emitted a method of calculation of the expectation value of an arbitrary product combination of effective time evolution operators of the vibronic system is developed. The calculations are performed by utilizing Feynman's disentangling and operator ordering techniques and yield closed solutions in the low-temperature limit. The theory is used for studying the intensity and the normally ordered intensity correlation function of the resonance fluorescence light from a two-atom molecule excited by a relatively weak laser field, which undergoes phase fluctuations. It is shown that the vibronic coupling can give rise to an anticorrelation effect which is substantially stronger than in the case of resonance fluorescence from an atom. For the case of small vibrational damping a general formula which directly connects the asymptotic long-time behaviour of the normalized intensity correlation function with the vibrational relaxation in the molecule is deduced. It should be convenient for the determination of very small vibrational decay rates.
The resonant response of a multilevel atomic system to strong coherent radiation is analyzed using an extension of the methods of time-independent scattering theory, adapted to the density-matrix formalism in order to include thermal bath effects. General steady-state expressions are derived for self-attenuation and resonance scattering rates in strong saturating fields, as functions of the coupling strengths, relaxation parameters, and frequency detunings. Formal expressions are given for radiative-damping and collision-broadening relaxation parameters, relating the latter to scattering amplitudes. Modifications of collision-broadening parameters by the presence of very strong fields are discussed. The Bloch equations are derived by transformation to the time domain, under specified conditions.