Annihilation Dynamics of Molecular Excitons Measured at a Single Perturbative Excitation Energy

Heshmatpour, Constantin; Malevich, Pavel; Plasser, Felix; Menger, Maximilian F. S. J.; Lambert, Christoph; Šanda, František; Hauer, Jürgen

doi:10.1021/acs.jpclett.0c02141

Cited by 17 publications

(13 citation statements)

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“…Electronic states with doubly excited characters have aroused interest and generated lively debate in recent years. Their involvement in singlet ssion [1][2][3] can provide a promising route towards highly efficient photovoltaic devices, but they are also of particular interest in other technological applications, such as non-linear optical spectroscopy, [4][5][6] and thermally activated delayed uorescence. 7 In the photochemistry of polyenes [8][9][10] and derived systems, such as carotenoids, 11,12 states with partially doubly excited character play a crucial role and have been investigated for over 50 years, yet, still inciting ery discussions.…”

Section: Introductionmentioning

confidence: 99%

Classification of doubly excited molecular electronic states

et al. 2023

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Section: Introductionmentioning

confidence: 99%

Classification of doubly excited molecular electronic states

et al. 2023

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“…The use of strong pulses may provide information about the material system dynamics beyond that obtainable with weak-pulse techniques. Strong pulses may be used, e.g., to improve time resolution, to enhance desired features (e.g., weak transitions) in signals, to overcome electronic dephasing and vibrational relaxation, to manipulate nonadiabatic couplings, to enhance specific WPs by tuning the pulse strength/duration, , or to study the contribution of a specific process to the signal . The increase of the pulse strength permits the amplification of specific 4WM, 6WM, and higher-order contributions to the measured signal. , Hence, the pulse strength can be considered as an experimentally controllable parameter which, along with the pulse carrier frequencies and delay times, can be optimized for obtaining more information on the molecular system.…”

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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“…The HEOM, a computationally demanding technique, has been applied successfully to several model systems, [13][14][15][16][17] where, typically, molecular vibrations are not explicitly included into the system, but are clamped into the bath. On the other hand, the less demanding Redfield model is widely exploited to date, [18][19][20][21][22][23][24] particularly to simulate spectroscopic properties of systems where the vibrational coupling is prominent.…”

Section: Introductionmentioning

confidence: 99%