期刊
JOURNAL OF PHYSICAL CHEMISTRY B
卷 124, 期 10, 页码 1987-1994出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcb.9b11431
关键词
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资金
- DOE Basic Energy Sciences through the Chemical Sciences Geosciences and Biosciences Division [DE-SC0016501]
- ICAM fellowship by the Kent State University
- University of Michigan ICAM
The special pair, a bacteriochlorophyll a (BChl) dimer found at the core of bacterial reaction centers, is known to play a key role in the functionality of photosystems as a precursor to the photosynthesis process. In this paper, we analyze the inherent affinity of the special pair to rectify the intrapair photo-induced charge transfer (CT). In particular, we show that the molecular environment affects the nuclear geometry, resulting in symmetry breaking between the two possible intrapair CT processes. To this end, we study the relationships of the intrapair CT and the molecular geometry with respect to the effective dielectric constant provided by the molecular environment. We identify the special pair structural feature that breaks the symmetry between the two molecules, leading to CT rectification. Excited state energies, oscillator strengths, and electronic coupling values are obtained via time-dependent density functional theory, employing a recently developed framework based on a screened range-separated hybrid functional within a polarizable continuum model (SRSH-PCM). We analyze the rectification capability of the special pair by calculating the CT rates using a first-principles-based Fermi's golden rule approach.
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