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Title: Coherent quantum dynamics in donor–bridge–acceptor systems: beyond the hopping and super-exchange mechanisms

Journal Article · · New Journal of Physics
 [1];  [2];  [2]
  1. City Univ. of New York (CUNY), NY (United States); Columbia Univ., New York, NY (United States)
  2. Columbia Univ., New York, NY (United States)
+ Show Author Affiliations

The population transfer dynamics of model donor–bridge–acceptor systems is studied by comparing a recently developed polaron-transformed quantum master equation (PQME) with the well-known Redfield and Förster theories of quantum transport. We show that the PQME approach reduces to these two theories in their respective limits of validity and naturally interpolates between them as a function of the system–bath coupling strength. By exploring the parameter space of our model problem, we identify novel regimes of transport dynamics in bridged systems like those encountered in biological and organic energy transfer problems. Furthermore, we demonstrate that three-level systems like the ones studied herein represent ideal minimal models for the identification of quantum coherent transport as embodied in super-exchange phenomena that cannot be captured by Förster-like hopping approaches.

Research Organization:
City Univ. of New York (CUNY), NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Contributing Organization:
Department of Chemistry, Columbia University
Grant/Contract Number:
SC0001393
OSTI ID:
1751949
Report Number(s):
DOE-Queens-1393-10
Journal Information:
New Journal of Physics, Vol. 15, Issue 10; Related Information: Seogjoo Jang, Timothy Berkelbach, and David R. Reichman, “Coherent quantum dynamics in donor-bridge-acceptor nonadiabatic processes: Beyond the hopping and super-exchange mechanisms,” New Journal of Physics, 15, 105020 (2013); ISSN 1367-2630
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 27 works
Citation information provided by
Web of Science

References (43)

Chemical and Electrochemical Electron-Transfer Theory journal October 1964
Coherently wired light-harvesting in photosynthetic marine algae at ambient temperature journal February 2010
Time-Dependent Semiclassical Scattering Theory. II. Atomic Collisions journal May 1969
Nonequilibrium generalization of Förster–Dexter theory for excitation energy transfer journal January 2002
Influence of phonons on exciton transfer dynamics: comparison of the Redfield, Förster, and modified Redfield equations journal August 2002
Dielectric friction and the transition from adiabatic to nonadiabatic electron transfer. I. Solvation dynamics in Liouville space journal March 1988
Tunneling versus Hopping in Mixed-Valence Oligo- p -phenylenevinylene Polychlorinated Bis(triphenylmethyl) Radical Anions journal April 2011
The Theory of Relaxation Processes book January 1965
Electronic excitation dynamics in multichromophoric systems described via a polaron-representation master equation journal October 2011
Unified expression for the rate constant of the bridged electron transfer derived by renormalization journal October 2009
Low-temperature dynamical simulation of spin-boson systems journal November 1994
Theoretical examination of quantum coherence in a photosynthetic system at physiological temperature journal October 2009
A semiclassical self‐consistent‐field approach to dissipative dynamics: The spin–boson problem journal July 1995
Superexchange and electron transfer in the photosynthetic reaction center journal August 1989
Crossover from Single-Step Tunneling to Multistep Hopping for Molecular Triplet Energy Transfer journal June 2010
10th Spiers Memorial Lecture. Transfer mechanisms of electronic excitation journal January 1959
Long-time quantum simulation of the primary charge separation in bacterial photosynthesis. journal April 1996
Observation of ‘third sound’ in superfluid 3He journal December 1998
Variable Range Hopping and Electrical Conductivity along the DNA Double Helix journal June 2001
Using Meta Conjugation To Enhance Charge Separation versus Charge Recombination in Phenylacetylene Donor−Bridge−Acceptor Complexes journal November 2005
Langevin and master equation in quantum mechanics journal June 1997
Consistent treatment of coherent and incoherent energy transfer dynamics using a variational master equation journal September 2011
Diabatic surfaces and the pathway for primary electron transfer in a photosynthetic reaction center journal May 1993
Mixed quantum-classical dynamics: mean-field and surface-hopping conference November 2011
Theory of multichromophoric coherent resonance energy transfer: A polaronic quantum master equation approach journal July 2011
Electrostatic control of charge separation in bacterial photosynthesis journal June 1990
Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems journal April 2007
Coherent Intrachain Energy Migration in a Conjugated Polymer at Room Temperature journal January 2009
Improved Feynman propagators on a grid and non-adiabatic corrections within the path integral framework journal June 1992
Dynamics of the dissipative two-state system journal January 1987
Quantum chemical probes of electron-transfer kinetics: the nature of donor-acceptor interactions journal July 1991
Tunneling versus sequential long‐range electron transfer: Analogy with pump–probe spectroscopy journal December 1989
Fourth-order quantum master equation and its Markovian bath limit journal February 2002
Dynamics of Light Harvesting in Photosynthesis journal May 2009
Theory of coherent resonance energy transfer for coherent initial condition journal October 2009
Microscopic theory of singlet exciton fission. I. General formulation journal March 2013
Protein Dynamics Control the Kinetics of Initial Electron Transfer in Photosynthesis journal May 2007
Microscopic theory of singlet exciton fission. II. Application to pentacene dimers and the role of superexchange journal March 2013
Generalized Theory of Relaxation journal February 1957
Exciton-migration and three-pulse femtosecond optical spectroscopies of photosynthetic antenna complexes journal May 1998
Coherent versus incoherent excitation energy transfer in molecular systems journal October 2012
Theory of coherent resonance energy transfer journal September 2008
In situ superexchange electron transfer through a single molecule: A rectifying effect journal April 2006

Cited By (8)

Tracing feed-back driven exciton dynamics in molecular aggregates journal January 2018
Microscopic theory of singlet exciton fission. III. Crystalline pentacene journal August 2014
Spin-selective electron transfer reactions of radical pairs: Beyond the Haberkorn master equation journal August 2018
Studying rare nonadiabatic dynamics with transition path sampling quantum jump trajectories journal December 2018
Delocalized excitons in natural light-harvesting complexes journal August 2018
Delocalized excitons in natural light harvesting complexes text January 2018
Spin-selective electron transfer reactions of radical pairs: beyond the Haberkorn master equation text January 2018
Studying rare nonadiabatic dynamics with transition path sampling quantum jump trajectories text January 2018

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Resonance energy transfer
Donor-bridge-acceptor
Quantum coherence
Polaron transform
Quantum master equation