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Title: Coherent Exciton Dynamics in the Presence of Underdamped Vibrations

Abstract

Recent ultrafast optical experiments show that excitons in large biological light-harvesting complexes are coupled to molecular vibration modes. These high-frequency vibrations will not only affect the optical response, but also drive the exciton transport. Here, using a model dimer system, the frequency of the underdamped vibration is shown to have a strong effect on the exciton dynamics such that quantum coherent oscillations in the system can be present even in the case of strong noise. Two mechanisms are identified to be responsible for the enhanced transport efficiency: critical damping due to the tunable effective strength of the coupling to the bath, and resonance coupling where the vibrational frequency coincides with the energy gap in the system. The interplay of these two mechanisms determines parameters responsible for the most efficient transport, and these optimal control parameters are comparable to those in realistic light-harvesting complexes. Interestingly, oscillations in the excitonic coherence at resonance are suppressed in comparison to the case of an off-resonant vibration.

Authors:
 [1];  [2];  [3];  [4]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Singapore-MIT Alliance for Research and Technology (Singapore)
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Singapore-MIT Alliance for Research and Technology (Singapore)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1407274
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 6; Journal Issue: 4; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; chlorosome; excitation energy transfer; exciton diffusion; exciton-vibration coupling; green sulfur bacteria; light-harvesting antenna system; non-Markovian effects

Citation Formats

Dijkstra, Arend G., Wang, Chen, Cao, Jianshu, and Fleming, Graham R. Coherent Exciton Dynamics in the Presence of Underdamped Vibrations. United States: N. p., 2015. Web. doi:10.1021/jz502701u.
Dijkstra, Arend G., Wang, Chen, Cao, Jianshu, & Fleming, Graham R. Coherent Exciton Dynamics in the Presence of Underdamped Vibrations. United States. doi:10.1021/jz502701u.
Dijkstra, Arend G., Wang, Chen, Cao, Jianshu, and Fleming, Graham R. Thu . "Coherent Exciton Dynamics in the Presence of Underdamped Vibrations". United States. doi:10.1021/jz502701u. https://www.osti.gov/servlets/purl/1407274.
@article{osti_1407274,
title = {Coherent Exciton Dynamics in the Presence of Underdamped Vibrations},
author = {Dijkstra, Arend G. and Wang, Chen and Cao, Jianshu and Fleming, Graham R.},
abstractNote = {Recent ultrafast optical experiments show that excitons in large biological light-harvesting complexes are coupled to molecular vibration modes. These high-frequency vibrations will not only affect the optical response, but also drive the exciton transport. Here, using a model dimer system, the frequency of the underdamped vibration is shown to have a strong effect on the exciton dynamics such that quantum coherent oscillations in the system can be present even in the case of strong noise. Two mechanisms are identified to be responsible for the enhanced transport efficiency: critical damping due to the tunable effective strength of the coupling to the bath, and resonance coupling where the vibrational frequency coincides with the energy gap in the system. The interplay of these two mechanisms determines parameters responsible for the most efficient transport, and these optimal control parameters are comparable to those in realistic light-harvesting complexes. Interestingly, oscillations in the excitonic coherence at resonance are suppressed in comparison to the case of an off-resonant vibration.},
doi = {10.1021/jz502701u},
journal = {Journal of Physical Chemistry Letters},
number = 4,
volume = 6,
place = {United States},
year = {2015},
month = {1}
}

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