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Title: Multiscale Investigation of Thermal Fluctuations on Solar-Energy Conversion

Abstract

Photoinduced charge transfer (CT) plays a central role in biologically significant systems and in applications that harvest solar energy. We investigate the relationship of CT kinetics and conformation in a molecular triad. The triad, consisting of carotenoid, porphyrin, and fullerene is structurally flexible and able to acquire significantly varied conformations under ambient conditions. With an integrated approach of quantum calculations and molecular dynamics simulations, we compute the rate of CT at two distinctive conformations. The linearly extended conformation, in which the donor (carotenoid) and the acceptor (fullerene) are separated by nearly 50 Å, enables charge separation through a sequential CT process. A representative bent conformation that is entropically dominant, however, attenuates the CT, although the donor and the acceptor are spatially closer. Our computed rate of CT at the linear conformation is in good agreement with measured values. Our work provides unique fundamental understanding of the photoinduced CT process in the molecular triad.

Authors:
 [1]
  1. Univ. of Houston, TX (United States)
Publication Date:
Research Org.:
Univ. of Houston, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1360784
Report Number(s):
DOE-UH-04832
DOE Contract Number:  
SC0004832
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
30 DIRECT ENERGY CONVERSION; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Cheung, Margaret Shun. Multiscale Investigation of Thermal Fluctuations on Solar-Energy Conversion. United States: N. p., 2014. Web. doi:10.2172/1360784.
Cheung, Margaret Shun. Multiscale Investigation of Thermal Fluctuations on Solar-Energy Conversion. United States. doi:10.2172/1360784.
Cheung, Margaret Shun. Mon . "Multiscale Investigation of Thermal Fluctuations on Solar-Energy Conversion". United States. doi:10.2172/1360784. https://www.osti.gov/servlets/purl/1360784.
@article{osti_1360784,
title = {Multiscale Investigation of Thermal Fluctuations on Solar-Energy Conversion},
author = {Cheung, Margaret Shun},
abstractNote = {Photoinduced charge transfer (CT) plays a central role in biologically significant systems and in applications that harvest solar energy. We investigate the relationship of CT kinetics and conformation in a molecular triad. The triad, consisting of carotenoid, porphyrin, and fullerene is structurally flexible and able to acquire significantly varied conformations under ambient conditions. With an integrated approach of quantum calculations and molecular dynamics simulations, we compute the rate of CT at two distinctive conformations. The linearly extended conformation, in which the donor (carotenoid) and the acceptor (fullerene) are separated by nearly 50 Å, enables charge separation through a sequential CT process. A representative bent conformation that is entropically dominant, however, attenuates the CT, although the donor and the acceptor are spatially closer. Our computed rate of CT at the linear conformation is in good agreement with measured values. Our work provides unique fundamental understanding of the photoinduced CT process in the molecular triad.},
doi = {10.2172/1360784},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2014},
month = {9}
}