Jump to main content
Jump to site search

Issue 33, 2018

Tracing feed-back driven exciton dynamics in molecular aggregates

Author affiliations

Abstract

Perturbative treatment of excitation dynamics in molecular systems with respect to external interactions with a dissipative environment is extensively used for the description of excitation energy transfer and relaxation. However the simulated dynamics becomes sensitive to a specific representation basis set, which makes the conclusions obscure and questionable. We revisit questions of excitation creation patterns, coherent dynamics, relaxation and detection from a theoretical viewpoint, and demonstrate that a mixture of specific requirements should be met to observe coherent phenomena and incoherent decay processes. We discuss how intermixing of coherent components in relaxation phenomena is related to a non-perturbative regime of dynamics leading to nonlinear feed-back effects where bath relaxation also affects excitation wavepackets. We also discuss how bath equilibration causes local heating effects which is often neglected in numerical simulations. The parameters reflecting the complexity of the processes are related to excitation delocalization patterns in various basis representations. While these seem to be auxiliary nonobservable features, their evaluation allows better investigation of the physical behavior of quantum relaxation processes in molecular aggregate systems.

Graphical abstract: Tracing feed-back driven exciton dynamics in molecular aggregates

Article information


Submitted
30 Jan 2018
Accepted
23 Jul 2018
First published
23 Jul 2018

Phys. Chem. Chem. Phys., 2018,20, 21225-21240
Article type
Perspective

Tracing feed-back driven exciton dynamics in molecular aggregates

D. Abramavicius, V. Chorošajev and L. Valkunas, Phys. Chem. Chem. Phys., 2018, 20, 21225 DOI: 10.1039/C8CP00682B

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.


Social activity

Search articles by author

Spotlight

Advertisements