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Title: Coherent exciton-vibrational dynamics and energy transfer in conjugated organics

Coherence, signifying concurrent electron-vibrational dynamics in complex natural and man-made systems, is currently a subject of intense study. Understanding this phenomenon is important when designing carrier transport in optoelectronic materials. Here, excited state dynamics simulations reveal a ubiquitous pattern in the evolution of photoexcitations for a broad range of molecular systems. Symmetries of the wavefunctions define a specific form of the non-adiabatic coupling that drives quantum transitions between excited states, leading to a collective asymmetric vibrational excitation coupled to the electronic system. This promotes periodic oscillatory evolution of the wavefunctions, preserving specific phase and amplitude relations across the ensemble of trajectories. The simple model proposed here explains the appearance of coherent exciton-vibrational dynamics due to non-adiabatic transitions, which is universal across multiple molecular systems. The observed relationships between electronic wavefunctions and the resulting functionalities allows us to understand, and potentially manipulate, excited state dynamics and energy transfer in molecular materials.
Authors:
 [1] ;  [2] ;  [2] ;  [2] ;  [2] ; ORCiD logo [3] ;  [4] ;  [2] ;  [4] ; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. National Univ. of Quilmes, Bernal (Argentina)
  3. National Univ. of Colombia, Bogotá (Colombia). Dept. of Chemistry
  4. Univ. of Florida, Gainesville, FL (United States). Dept. of Chemistry
Publication Date:
Report Number(s):
LA-UR-17-30143
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC52-06NA25396; PICT- 2014–2662
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA); LANL Laboratory Directed Research and Development (LDRD) Program; National Scientific and Technical Research Council (CONICET) (Argentina); National Univ. of Quilmes (UNQ) (Argentina); National Agency of Scientific and Technological Promotion (ANPCyT) (Argentina)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Inorganic and Physical Chemistry
OSTI Identifier:
1457307

Nelson, Tammie R., Ondarse-Alvarez, Dianelys, Oldani, Nicolas, Rodriguez-Hernandez, Beatriz, Alfonso-Hernandez, Laura, Galindo, Johan F., Kleiman, Valeria D., Fernandez-Alberti, Sebastian, Roitberg, Adrian E., and Tretiak, Sergei. Coherent exciton-vibrational dynamics and energy transfer in conjugated organics. United States: N. p., Web. doi:10.1038/s41467-018-04694-8.
Nelson, Tammie R., Ondarse-Alvarez, Dianelys, Oldani, Nicolas, Rodriguez-Hernandez, Beatriz, Alfonso-Hernandez, Laura, Galindo, Johan F., Kleiman, Valeria D., Fernandez-Alberti, Sebastian, Roitberg, Adrian E., & Tretiak, Sergei. Coherent exciton-vibrational dynamics and energy transfer in conjugated organics. United States. doi:10.1038/s41467-018-04694-8.
Nelson, Tammie R., Ondarse-Alvarez, Dianelys, Oldani, Nicolas, Rodriguez-Hernandez, Beatriz, Alfonso-Hernandez, Laura, Galindo, Johan F., Kleiman, Valeria D., Fernandez-Alberti, Sebastian, Roitberg, Adrian E., and Tretiak, Sergei. 2018. "Coherent exciton-vibrational dynamics and energy transfer in conjugated organics". United States. doi:10.1038/s41467-018-04694-8. https://www.osti.gov/servlets/purl/1457307.
@article{osti_1457307,
title = {Coherent exciton-vibrational dynamics and energy transfer in conjugated organics},
author = {Nelson, Tammie R. and Ondarse-Alvarez, Dianelys and Oldani, Nicolas and Rodriguez-Hernandez, Beatriz and Alfonso-Hernandez, Laura and Galindo, Johan F. and Kleiman, Valeria D. and Fernandez-Alberti, Sebastian and Roitberg, Adrian E. and Tretiak, Sergei},
abstractNote = {Coherence, signifying concurrent electron-vibrational dynamics in complex natural and man-made systems, is currently a subject of intense study. Understanding this phenomenon is important when designing carrier transport in optoelectronic materials. Here, excited state dynamics simulations reveal a ubiquitous pattern in the evolution of photoexcitations for a broad range of molecular systems. Symmetries of the wavefunctions define a specific form of the non-adiabatic coupling that drives quantum transitions between excited states, leading to a collective asymmetric vibrational excitation coupled to the electronic system. This promotes periodic oscillatory evolution of the wavefunctions, preserving specific phase and amplitude relations across the ensemble of trajectories. The simple model proposed here explains the appearance of coherent exciton-vibrational dynamics due to non-adiabatic transitions, which is universal across multiple molecular systems. The observed relationships between electronic wavefunctions and the resulting functionalities allows us to understand, and potentially manipulate, excited state dynamics and energy transfer in molecular materials.},
doi = {10.1038/s41467-018-04694-8},
journal = {Nature Communications},
number = ,
volume = 9,
place = {United States},
year = {2018},
month = {6}
}