“…The derivation is conveniently achieved via projection operator technique [27,37]. Two general schemes exist.…”
Section: Second Order Relaxation Theoriesmentioning
confidence: 99%
“…time-non-local master equation for the RDM with a convolution memory term. Alternatively, a different projector operator identity can be used to derive EM which is time-local, leading to so-called convolutionless master equation [37]. Interested reader can refer to Refs.…”
Section: Second Order Relaxation Theoriesmentioning
confidence: 99%
“…Interested reader can refer to Refs. [25,26,37] for details of the derivations and comparison of the two schemes. Below, we will use specific second order approximation to the general equations.…”
Section: Second Order Relaxation Theoriesmentioning
International audienceWe compare four different types of equations of motion for reduced density matrix of a system of molecular excitons interacting with thermodynamic bath. All four equations are of second order in the linear system-bath interaction Hamiltonian, with different approximations applied in their derivation. In particular we compare time-nonlocal equations obtained from so-called Nakajima-Zwanzig identity and the time-local equations resulting from the partial ordering prescription of the cummulant expansion. In each of these equations we alternatively apply secular approximation to decouple population and coherence dynamics from each other. We focus on the dynamics of intraband electronic coherences of the excitonic system which can be traced by coherent two-dimensional spectroscopy. We discuss the applicability of the four relaxation theories to simulations of population and coherence dynamics, and identify features of the two-dimensional coherent spectrum that allow us to distinguish time-nonlocal effects
“…The derivation is conveniently achieved via projection operator technique [27,37]. Two general schemes exist.…”
Section: Second Order Relaxation Theoriesmentioning
confidence: 99%
“…time-non-local master equation for the RDM with a convolution memory term. Alternatively, a different projector operator identity can be used to derive EM which is time-local, leading to so-called convolutionless master equation [37]. Interested reader can refer to Refs.…”
Section: Second Order Relaxation Theoriesmentioning
confidence: 99%
“…Interested reader can refer to Refs. [25,26,37] for details of the derivations and comparison of the two schemes. Below, we will use specific second order approximation to the general equations.…”
Section: Second Order Relaxation Theoriesmentioning
International audienceWe compare four different types of equations of motion for reduced density matrix of a system of molecular excitons interacting with thermodynamic bath. All four equations are of second order in the linear system-bath interaction Hamiltonian, with different approximations applied in their derivation. In particular we compare time-nonlocal equations obtained from so-called Nakajima-Zwanzig identity and the time-local equations resulting from the partial ordering prescription of the cummulant expansion. In each of these equations we alternatively apply secular approximation to decouple population and coherence dynamics from each other. We focus on the dynamics of intraband electronic coherences of the excitonic system which can be traced by coherent two-dimensional spectroscopy. We discuss the applicability of the four relaxation theories to simulations of population and coherence dynamics, and identify features of the two-dimensional coherent spectrum that allow us to distinguish time-nonlocal effects
“…We consider a time evolution of the density matrix ρ(t) of HFS states using the generalized master equation [12,13] that, within a secular approximation, can be written as…”
Section: Time Evolution Of the Density Matrixmentioning
Collisions of metastable antiprotonic helium with ordinary He atoms can induce transitions between hyperfine structure (HFS) sublevels and thus relaxation of the populations as well as shift and broadening of M1 microwave spectral lines. Previously we have considered these effects, using quantum close-coupling method for the collisions and the model interatomic interaction involving tensor term (Korenman and Yudin, J Phys B At Mol Opt Phys 39: [1473][1474][1475][1476][1477][1478][1479][1480][1481][1482][1483][1484] 2006). In this paper we extend the consideration in two lines: (i) collisional transition rates, shifts and broadenings of M1-lines are considered in relation to the strength of the tensor interaction; (ii) time evolution of the density matrix of HFS states is considered using the generalized master equation with the calculated elementary characteristics. A good agreement with the recent experimental data on the time dependence of optimum signal-to-noise ratio and of linewidth is obtained using the strength of tensor interactions as a free parameter.
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