Modeling of noise-assisted quantum transfer between donor and acceptor with finite bandwidths

Journal Article · Thu Oct 03 00:00:00 EDT 2019 · Journal of Physics. A, Mathematical and Theoretical

DOI:https://doi.org/10.1088/1751-8121/ab4502· OSTI ID:1768535

Nesterov, Alexander I. ^[1]; Berman, Gennady P. ^[2]; Merkli, Marco ^[3]; Saxena, Avadh ^[2]

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1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. de Guadalajara, Jalisco (Mexico)
2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Memorial Univ. of Newfoundland, Newfoundland (Canada)

We present an analytical and numerical study of noise-assisted quantum exciton (electron) transfer (ET) in a dimer consisting of donor and acceptor, modeled by interacting continuous electron bands of finite widths. We start with discrete energy levels for both bands. The interaction with the environment is modeled by a stationary stochastic process (noise) acting on all the donor and acceptor energy levels. Then, by using a continuous limit for the electron spectra, we derive integro-differential equations for the ET dynamics between the two bands. Finally, we derive from these equations rate-type differential equations for the ET dynamics. We formulate the conditions of validity of the rate-type equations. We consider different regions of parameters characterizing the widths of the donor and acceptor bands and the strength of the dimer-noise interaction. For a simplified model with a single energy level donor and a continuous acceptor band, we derive a generalized simple analytic expression and provide numerical simulations for the ET rate. They are consistent with Wigner–Weisskopf, Förster-type, and Marcus-type expressions, in their corresponding regime of parameters. For a weak dimer-noise interaction, our approach leads to the Wigner–Weisskopf ET rate, or to the Förster-type ET rate, depending on other parameters. In the limit of strong dimer-noise interaction, our approach is non-perturbative in the dimer-noise interaction constant, and it recovers the Marcus-type ET rate. Our analytic results are confirmed by numerical simulations. We demonstrate how our theoretical results are modified when both the donor and the acceptor are described by finite bands. We also show that, for a relatively wide acceptor band, the efficiency of the ET from donor to acceptor can be close to 100% for a broad range of noise amplitudes, for both 'downhill' and 'uphill' ET, for sharp and flat redox potentials, and for reasonably short times. We discuss possible applications of our approach.

• Research Organization: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
• Sponsoring Organization: USDOE Laboratory Directed Research and Development (LDRD) Program
• Grant/Contract Number: 89233218CNA000001
• OSTI ID: 1768535
• Alternate ID(s): OSTI ID: 22988473
• Report Number(s): LA-UR--18-31605
• Journal Information: Journal of Physics. A, Mathematical and Theoretical, Journal Name: Journal of Physics. A, Mathematical and Theoretical Journal Issue: 43 Vol. 52; ISSN 1751-8113
• Publisher: IOP Publishing
• Country of Publication: United States
• Language: English

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