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Title: Electronic Delocalization, Vibrational Dynamics and Energy Transfer in Organic Chromophores

The efficiency of materials developed for solar energy and technological applications depends on the interplay between molecular architecture and light-induced electronic energy redistribution. The spatial localization of electronic excitations is very sensitive to molecular distortions. Vibrational nuclear motions can couple to electronic dynamics driving changes in localization. The electronic energy transfer among multiple chromophores arises from several distinct mechanisms that can give rise to experimentally measured signals. Atomistic simulations of coupled electron-vibrational dynamics can help uncover the nuclear motions directing energy flow. Through careful analysis of excited state wave function evolution and a useful fragmenting of multichromophore systems, through-bond transport and exciton hopping (through-space) mechanisms can be distinguished. Such insights are crucial in the interpretation of fluorescence anisotropy measurements and can aid materials design. Finally, this Perspective highlights the interconnected vibrational and electronic motions at the foundation of nonadiabatic dynamics where nuclear motions, including torsional rotations and bond vibrations, drive electronic transitions.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Univ. Nacional de Quilmes, Bernal (Argentina)
  3. Univ. of Florida, Gainesville, FL (United States)
Publication Date:
Report Number(s):
LA-UR-17-23765
Journal ID: ISSN 1948-7185; TRN: US1800642
Grant/Contract Number:
AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal Issue: 13; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Material Science
OSTI Identifier:
1414116

Nelson, Tammie Renee, Fernandez Alberti, Sebastian, Roitberg, Adrian, and Tretiak, Sergei. Electronic Delocalization, Vibrational Dynamics and Energy Transfer in Organic Chromophores. United States: N. p., Web. doi:10.1021/acs.jpclett.7b00790.
Nelson, Tammie Renee, Fernandez Alberti, Sebastian, Roitberg, Adrian, & Tretiak, Sergei. Electronic Delocalization, Vibrational Dynamics and Energy Transfer in Organic Chromophores. United States. doi:10.1021/acs.jpclett.7b00790.
Nelson, Tammie Renee, Fernandez Alberti, Sebastian, Roitberg, Adrian, and Tretiak, Sergei. 2017. "Electronic Delocalization, Vibrational Dynamics and Energy Transfer in Organic Chromophores". United States. doi:10.1021/acs.jpclett.7b00790. https://www.osti.gov/servlets/purl/1414116.
@article{osti_1414116,
title = {Electronic Delocalization, Vibrational Dynamics and Energy Transfer in Organic Chromophores},
author = {Nelson, Tammie Renee and Fernandez Alberti, Sebastian and Roitberg, Adrian and Tretiak, Sergei},
abstractNote = {The efficiency of materials developed for solar energy and technological applications depends on the interplay between molecular architecture and light-induced electronic energy redistribution. The spatial localization of electronic excitations is very sensitive to molecular distortions. Vibrational nuclear motions can couple to electronic dynamics driving changes in localization. The electronic energy transfer among multiple chromophores arises from several distinct mechanisms that can give rise to experimentally measured signals. Atomistic simulations of coupled electron-vibrational dynamics can help uncover the nuclear motions directing energy flow. Through careful analysis of excited state wave function evolution and a useful fragmenting of multichromophore systems, through-bond transport and exciton hopping (through-space) mechanisms can be distinguished. Such insights are crucial in the interpretation of fluorescence anisotropy measurements and can aid materials design. Finally, this Perspective highlights the interconnected vibrational and electronic motions at the foundation of nonadiabatic dynamics where nuclear motions, including torsional rotations and bond vibrations, drive electronic transitions.},
doi = {10.1021/acs.jpclett.7b00790},
journal = {Journal of Physical Chemistry Letters},
number = 13,
volume = 8,
place = {United States},
year = {2017},
month = {6}
}