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Title: Coherent Exciton Dynamics in the Presence of Underdamped Vibrations

Journal Article · · Journal of Physical Chemistry Letters
DOI:https://doi.org/10.1021/jz502701u· OSTI ID:1407274
 [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)
+ Show Author Affiliations

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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1407274
Journal Information:
Journal of Physical Chemistry Letters, Vol. 6, Issue 4; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 60 works
Citation information provided by
Web of Science

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Cited By (18)

Signatures of Strong Vibronic Coupling Mediating Coherent Charge Transfer in Two-Dimensional Electronic Spectroscopy journal August 2019
The hierarchical and perturbative forms of stochastic Schrödinger equations and their applications to carrier dynamics in organic materials journal July 2018
Efficient long-distance energy transport in molecular systems through adiabatic passage journal July 2019
Polaron effects on the performance of light-harvesting systems: a quantum heat engine perspective journal January 2016
Ultrafast transient absorption revisited: Phase-flips, spectral fingers, and other dynamical features journal May 2016
Exciton-vibrational resonance and dynamics of charge separation in the photosystem II reaction center journal January 2017
Energy transfer in structured and unstructured environments: Master equations beyond the Born-Markov approximations journal January 2016
Non-canonical distribution and non-equilibrium transport beyond weak system-bath coupling regime: A polaron transformation approach journal May 2016
Enhanced exciton transport in an optical cavity field with spatially varying profile journal July 2019
Primary Charge Separation in the Photosystem II Reaction Center Revealed by a Global Analysis of the Two-dimensional Electronic Spectra journal September 2017
Quantum ergodicity and energy flow in molecules journal July 2015
Non-equilibrium stationary coherences in photosynthetic energy transfer under weak-field incoherent illumination journal March 2018
Effect of an underdamped vibration with both diagonal and off‐diagonal exciton–phonon interactions on excitation energy transfer journal December 2018
Energy transfer in structured and unstructured environments: master equations beyond the Born-Markov approximations text January 2015
The hierarchical and perturbative forms of stochastic Schrödinger equations and their applications to carrier dynamics in organic materials text January 2018
Efficient long-distance energy transport in molecular systems through adiabatic passage text January 2019
The Role of Resonant Vibrations in Electronic Energy Transfer journal March 2016
Simple Quantum Dynamics with Thermalization journal December 2017

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74 ATOMIC AND MOLECULAR PHYSICS
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