Ultrafast dynamic evolution of multilevel systems in medium-strength laser fields

Wang, Zhenhao; Shi, Guoqiang; He, Yu; Wang, Quanjun; Ding, Jianyong; Sun, Shoujin; Liu, Zuoye; Hu, Bitao

doi:10.1088/1367-2630/ab145a

Cited by 3 publications

(1 citation statement)

References 40 publications

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“…A number of femtosecond 4WM experiments revealed that richer information on the photoinduced dynamics in atomic vapors, − polyatomic chromophores, − multichromophore aggregates, − and nanosystems − can be obtained by applying more intense laser pulses (see refs − for reviews). On the theoretical side, a variety of simulations of 4WM signals beyond the limit of weak system–field coupling have been reported. ,,,,− Single-molecule femtosecond spectroscopy of individual chromophores − and antenna complexes , also usually requires strong pulses.…”

Section: Nonperturbative Calculation Of the Nonlinear Polarizationmentioning

confidence: 99%

Equation-of-Motion Methods for the Calculation of Femtosecond Time-Resolved 4-Wave-Mixing and N-Wave-Mixing Signals

2022

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Femtosecond nonlinear spectroscopy is the main tool for the time-resolved detection of photophysical and photochemical processes. Since most systems of chemical interest are rather complex, theoretical support is indispensable for the extraction of the intrinsic system dynamics from the detected spectroscopic responses. There exist two alternative theoretical formalisms for the calculation of spectroscopic signals, the nonlinear response-function (NRF) approach and the spectroscopic equation-of-motion (EOM) approach. In the NRF formalism, the system–field interaction is assumed to be sufficiently weak and is treated in lowest-order perturbation theory for each laser pulse interacting with the sample. The conceptual alternative to the NRF method is the extraction of the spectroscopic signals from the solutions of quantum mechanical, semiclassical, or quasiclassical EOMs which govern the time evolution of the material system interacting with the radiation field of the laser pulses. The NRF formalism and its applications to a broad range of material systems and spectroscopic signals have been comprehensively reviewed in the literature. This article provides a detailed review of the suite of EOM methods, including applications to 4-wave-mixing and N-wave-mixing signals detected with weak or strong fields. Under certain circumstances, the spectroscopic EOM methods may be more efficient than the NRF method for the computation of various nonlinear spectroscopic signals.

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Section: Nonperturbative Calculation Of the Nonlinear Polarizationmentioning

confidence: 99%

Equation-of-Motion Methods for the Calculation of Femtosecond Time-Resolved 4-Wave-Mixing and N-Wave-Mixing Signals

2022

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Contracted description of driven degenerate multilevel quantum systems

Xu,

Sun,

Gelin

et al. 2023

The Journal of Chemical Physics

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We formulate a contraction theorem that maps quantum dynamics of a multilevel degenerate system (DS) driven by a time-dependent external field to the dynamics of the corresponding contracted non-degenerate system (CNS) of lower dimension, provided transitions between each pair of degenerate levels in the DS have identical transition dipole moments. The theorem is valid for an external field of any strength and shape, with and without rotating wave approximation in the system–field interaction. It establishes explicit relations between DS and CNS observables, significantly simplifies numerical calculations, and clarifies physical origins of the field-induced DS dynamics.

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Effects of high pulse intensity and chirp in two-dimensional electronic spectroscopy of an atomic vapor

et al. 2020

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The effects of high pulse intensity and chirp on two-dimensional electronic spectroscopy signals are experimentally investigated in the highly non-perturbative regime using atomic rubidium vapor as clean model system. Data analysis is performed based on higher-order Feynman diagrams and non-perturbative numerical simulations of the system response. It is shown that higher-order contributions may lead to a fundamental change of the static appearance and beating-maps of the 2D spectra and that chirped pulses enhance or suppress distinct higher-order pathways. We further give an estimate of the threshold intensity beyond which the high-intensity effects become visible for the system under consideration.

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Ultrafast dynamic evolution of multilevel systems in medium-strength laser fields

Cited by 3 publications

References 40 publications

Equation-of-Motion Methods for the Calculation of Femtosecond Time-Resolved 4-Wave-Mixing and N-Wave-Mixing Signals

Equation-of-Motion Methods for the Calculation of Femtosecond Time-Resolved 4-Wave-Mixing and N-Wave-Mixing Signals

Contracted description of driven degenerate multilevel quantum systems

Effects of high pulse intensity and chirp in two-dimensional electronic spectroscopy of an atomic vapor

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