Coherent quantum dynamics in donor–bridge–acceptor systems: beyond the hopping and super-exchange mechanisms
Journal Article
·
· New Journal of Physics
- City Univ. of New York (CUNY), NY (United States); Columbia Univ., New York, NY (United States); Queens College, City University of New York
- Columbia Univ., New York, NY (United States)
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
- Alternate ID(s):
- OSTI ID: 22186698
OSTI ID: 1161727
OSTI ID: 1168095
OSTI ID: 1384144
- Report Number(s):
- DOE-Queens-1393-10
- Journal Information:
- New Journal of Physics, Journal Name: New Journal of Physics Journal Issue: 10 Vol. 15; ISSN 1367-2630
- Publisher:
- IOP PublishingCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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