Simulation of femtosecond “double-slit” experiments for a chromophore in a dissipative environment

Gelin, Maxim F.; Tanimura, Yoshitaka; Domcke, Wolfgang

doi:10.1063/1.4832876

Cited by 19 publications

(20 citation statements)

References 67 publications

(88 reference statements)

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“…Within the rotating‐wave approximation (RWA), the complex valued electric field is combined with the respective excitation and de‐excitation parts of the dipole operator:

H_{field} (t) = - \sum_{p} {bolde}_{p} \cdot [{\overset{truê}{boldμ}}^{+} E_{p}^{-} (r, t) + {\overset{truê}{boldμ}}^{-} E_{p}^{+} (r, t)]

…”

Section: Methodsmentioning

confidence: 99%

Efficient calculation of open quantum system dynamics and time‐resolved spectroscopy with distributed memory HEOM (DM‐HEOM)

et al. 2018

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Time- and frequency-resolved optical signals provide insights into the properties of light-harvesting molecular complexes, including excitation energies, dipole strengths and orientations, as well as in the exciton energy flow through the complex. The hierarchical equations of motion (HEOM) provide a unifying theory, which allows one to study the combined effects of system-environment dissipation and non-Markovian memory without making restrictive assumptions about weak or strong couplings or separability of vibrational and electronic degrees of freedom. With increasing system size the exact solution of the open quantum system dynamics requires memory and compute resources beyond a single compute node. To overcome this barrier, we developed a scalable variant of HEOM. Our distributed memory HEOM, DM-HEOM, is a universal tool for open quantum system dynamics. It is used to accurately compute all experimentally accessible time- and frequency-resolved processes in light-harvesting molecular complexes with arbitrary system-environment couplings for a wide range of temperatures and complex sizes. © 2018 Wiley Periodicals, Inc.

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“…Within the rotating‐wave approximation (RWA), the complex valued electric field is combined with the respective excitation and de‐excitation parts of the dipole operator:

H_{field} (t) = - \sum_{p} {bolde}_{p} \cdot [{\overset{truê}{boldμ}}^{+} E_{p}^{-} (r, t) + {\overset{truê}{boldμ}}^{-} E_{p}^{+} (r, t)]

…”

Section: Methodsmentioning

confidence: 99%

Efficient calculation of open quantum system dynamics and time‐resolved spectroscopy with distributed memory HEOM (DM‐HEOM)

et al. 2018

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“…A microscopic treatment of electronic dephasing is also possible (see, e.g., Ref. [27]), but the phenomenological description via Equation (12) is sufficient for the purposes of the present work [8,11,28].…”

Section: Theoretical Frameworkmentioning

confidence: 99%

“…The intensity of the double-pump SM signal can be expanded in the system-field coupling as [11,12,27] S(τ)=∑k=2,4,6,...Sk(τ), where k corresponds to the number of interactions of the chromophore with the laser pulses and Sk(τ)∼E0k. For sufficiently weak pulses, the signal is represented by S2(τ), scales linearly with the pulse intensity, and can be expressed through the linear response function [11].…”

Section: Theoretical Frameworkmentioning

confidence: 99%

Monitoring of Nonadiabatic Effects in Individual Chromophores by Femtosecond Double-Pump Single-Molecule Spectroscopy: A Model Study

et al. 2019

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We explore, by theoretical modeling and computer simulations, how nonadiabatic couplings of excited electronic states of a polyatomic chromophore manifest themselves in single-molecule signals on femtosecond timescales. The chromophore is modeled as a system with three electronic states (the ground state and two non-adiabatically coupled excited states) and a Condon-active vibrational mode which, in turn, is coupled to a harmonic oscillator heat bath. For this system, we simulate double-pump single-molecule signals with fluorescence detection for different system-field interaction strengths, from the weak-coupling regime to the strong-coupling regime. While the signals are determined by the coherence of the electronic density matrix in the weak-coupling regime, they are determined by the populations of the electronic density matrix in the strong-coupling regime. As a consequence, the signals in the strong coupling regime allow the monitoring of nonadiabatic electronic population dynamics and are robust with respect to temporal inhomogeneity of the optical gap, while signals in the weak-coupling regime are sensitive to fluctuations of the optical gap and do not contain information on the electronic population dynamics.

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“…Electronic coherence plays an essential role in the study of nonlinear optical response in photoisomerization processes. Here, we study photoisomerization processes using multi-state hierarchical quantum Fokker-Planck equations of motion (MS-QHFPE) approach [21][22][23], which is an extension of reduced hierarchical equations of motion for open quantum dynamics [20,[49][50][51][52][53][54][55][56][57][58][59][60][61][62][63][64][65][66]. This approach allows us to study the dynamics of quantum open systems as well as nonlinear optical spectra in a numerically rigorous manner.…”

Section: Introductionmentioning

confidence: 99%

Probing photoisomerization processes by means of multi-dimensional electronic spectroscopy: The multi-state quantum hierarchical Fokker-Planck equation approach

Ikeda

Tanimura

2017

The Journal of Chemical Physics

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Photoisomerization in a system with multiple electronic states and anharmonic potential surfaces in a dissipative environment is investigated using a rigorous numerical method employing quantum hierarchical Fokker-Planck equations (QHFPEs) for multi-state systems. We have developed a computer code incorporating QHFPE for general-purpose computing on graphics processing units that can treat multi-state systems in phase space with any strength of diabatic coupling of electronic states under non-perturbative and non-Markovian system-bath interactions. This approach facilitates the calculation of both linear and nonlinear spectra. We computed Wigner distributions for excited, ground, and coherent states. We then investigated excited state dynamics involving transitions among these states by analyzing linear absorption and transient absorption processes and multi-dimensional electronic spectra with various values of heat bath parameters. Our results provide predictions for spectroscopic measurements of photoisomerization dynamics. The motion of excitation and ground state wavepackets and their coherence involved in the photoisomerization were observed as the profiles of positive and negative peaks of two-dimensional spectra.

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Simulation of femtosecond “double-slit” experiments for a chromophore in a dissipative environment

Cited by 19 publications

References 67 publications

Efficient calculation of open quantum system dynamics and time‐resolved spectroscopy with distributed memory HEOM (DM‐HEOM)

Efficient calculation of open quantum system dynamics and time‐resolved spectroscopy with distributed memory HEOM (DM‐HEOM)

Monitoring of Nonadiabatic Effects in Individual Chromophores by Femtosecond Double-Pump Single-Molecule Spectroscopy: A Model Study

Probing photoisomerization processes by means of multi-dimensional electronic spectroscopy: The multi-state quantum hierarchical Fokker-Planck equation approach

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