# Exact stochastic unraveling of an optical coherence dynamics by cumulant expansion.

@article{Olina2014ExactSU, title={Exact stochastic unraveling of an optical coherence dynamics by cumulant expansion.}, author={Jan Ol{\vs}ina and Tobias Kramer and Christoph Kreisbeck and Tom{\'a}{\vs} Man{\vc}al}, journal={The Journal of chemical physics}, year={2014}, volume={141 16}, pages={ 164109 } }

A numerically exact Monte Carlo scheme for calculation of open quantum system dynamics is proposed and implemented. The method consists of a Monte Carlo summation of a perturbation expansion in terms of trajectories in Liouville phase-space with respect to the coupling between the excited states of the molecule. The trajectories are weighted by a complex decoherence factor based on the second-order cumulant expansion of the environmental evolution. The method can be used with an arbitrary…

## 15 Citations

Nonadiabatic effects in electronic and nuclear dynamics

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This review gives an overview of different nonadiabatic processes that manifest themselves in electronic and nuclear dynamics ranging from the nonadiABatic phenomena taking place during tunnel ionization of atoms in strong laser fields to the radiationless relaxation through conical intersections and the nonidiabatic coupling of vibrational modes and the computational approaches that have been developed to describe such phenomena.

Treatment of Herzberg-Teller and non-Condon effects in optical spectra with Hierarchical Equations of Motion

- PhysicsChemical Physics
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Strong Exciton-Vibrational Coupling in Molecular Assemblies. Dynamics Using the Polaron Transformation in HEOM Space.

- PhysicsThe journal of physical chemistry. A
- 2021

This article describes for the first time how PT becomes applicable in the framework of the "Hierarchical Equations of Motion" (HEOM) approach for treatment of open quantum systems by deriving hierarchical equations of PT which lead to a shift in the excited state potential energy surface to compensate its displacement.

Combined treatment of relaxation and fluctuation dynamics in the calculation of two-dimensional electronic spectra.

- PhysicsThe Journal of chemical physics
- 2014

It is shown that population transfer and dissipative fluctuation dynamics cannot be described independent of each other in general.

Accuracy of approximate methods for the calculation of absorption-type linear spectra with a complex system-bath coupling

- Physics
- 2022

The accuracy of approximate methods for calculating linear optical spectra depends on many variables. In this study, we ﬁx most of these parameters to typical values found in photosynthetic…

Scalable High-Performance Algorithm for the Simulation of Exciton Dynamics. Application to the Light-Harvesting Complex II in the Presence of Resonant Vibrational Modes.

- PhysicsJournal of chemical theory and computation
- 2014

This work adapt and extend the exact hierarchical equation of motion (HEOM) method to various high-performance many-core platforms using the Open Compute Language (OpenCL) and investigates the impact of resonantly coupled vibrations on the relaxation and shows that the transfer does not rely on a fine-tuning of specific modes.

Single Molecule Spectroscopy of Monomeric LHCII: Experiment and Theory

- Physics, ChemistryScientific reports
- 2016

This work derives approximate equations of motion for excited state dynamics of a multilevel open quantum system weakly interacting with light to describe fluorescence-detected single molecule spectra and shows that with reasonable assumptions about its interaction with chlorophylls, Lut 1 can act as an efficient fluorescence quencher in LHCII.

Modeling of Transient Absorption Spectra in Exciton-Charge-Transfer Systems.

- PhysicsThe journal of physical chemistry. B
- 2017

It is shown that the nonperturbative hierarchical equations of motion method captures the finite duration of the laser-molecule interactions and the reorganization process during the exciton migration in a model exciton system, including the charge-transfer state.

Lineshape theory of pigment-protein complexes: How the finite relaxation time of nuclei influences the exciton relaxation-induced lifetime broadening.

- PhysicsThe Journal of chemical physics
- 2016

An analytical expression, termed Non-equilibrium Modified Redfield (NeMoR) theory, is provided for the lifetime broadening that takes into account the finite nuclear relaxation time and it is found that, for a widely used experimental spectral density of the exciton-vibrational coupling of pigment-protein complexes, the NeMoR spectrum at low-temperatures is better approximated by Redfield than by modified Redfield theory.

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