Elucidation of near-resonance vibronic coherence lifetimes by nonadiabatic electronic-vibrational state character mixing.

Authors:
Dr Marco A Allodi, PhD
Dr Marco A Allodi, PhD
The University of Chicago
Yen Postdoctoral Scholar
Laser Spectroscopy, Molecular Dynamics, Biophysics, Astrochemistry
Chicago, IL | USA

Proc Natl Acad Sci U S A 2018 Aug 9. Epub 2018 Aug 9.

Qatar Environment and Energy Research Institute, Hamad Bin Khalifa University, Qatar Foundation, Doha, Qatar;

Recent work suggests that the long-lived coherences observed in both natural and artificial light-harvesting systems (such as the Fenna-Matthews-Olson complex) could be attributed to the mixing of the pigments' electronic and vibrational degrees of freedom. To investigate the underlying mechanism of these long coherence lifetimes, a sophisticated description of interactions between the molecular aggregates and the nonequilibrium fluctuations in the surrounding environment is necessary. This is done by implementing the hierarchical equations of motion approach on model homodimers, a method used in the intermediate coupling regime for many molecular aggregates wherein the nonequilibrium environment phonons play nontrivial roles in exciton dynamics. Here we report a character change in the vibronic states-reflective of property mixing between the electronic and vibrational states-induced by an interplay between system coupling parameters within the exciton-vibrational near-resonance regime. This mixing dictates vital aspects of coherence lifetime; by tracking the degree of mixing, we are able to elucidate the relationship between coherence lifetime and both the electronic energy fluctuation and the vibrational relaxation dephasing pathways.

Download full-text PDF

Source
http://dx.doi.org/10.1073/pnas.1701390115DOI Listing

Still can't find the full text of the article?

We can help you send a request to the authors directly.
August 2018
30 Reads
9.810 Impact Factor

Article Mentions


Provided by Crossref Event Data
crossref
Crossref: Crossref
June 23, 2019, 8:00 pm EST

Publication Analysis

Top Keywords

molecular aggregates
8
coherence lifetimes
8
electronic vibrational
8
aggregates nonequilibrium
8
coherence lifetime
8
mixing
5
implementing hierarchical
4
dictates vital
4
environment implementing
4
mixing dictates
4
hierarchical equations
4
near-resonance regime
4
approach model
4
motion approach
4
regime mixing
4
equations motion
4
surrounding environment
4
vital aspects
4
mixing electronic
4
long coherence
4

References

(Supplied by CrossRef)
Quantum biology
Lambert et al.
Nat Phys 2013
Quantum coherence in biological systems
Lloyd et al.
J Phys Conf Ser 2011
Quantum effects in biology
Fleming et al.
Proc Chem 2011

Similar Publications