Linear and third and fifthorder nonlinear spectroscopies of a charge transfer system coupled to an underdamped vibration
Abstract
We study hole, electron, and exciton transports in a charge transfer system in the presence of underdamped vibrational motion. We analyze the signature of these processes in the linear and third, and fifthorder nonlinear electronic spectra. Calculations are performed with a numerically exact hierarchical equations of motion method for an underdamped Brownian oscillator spectral density. We find that combining electron, hole, and exciton transfers can lead to nontrivial spectra with more structure than with excitonic coupling alone. Traces taken during the waiting time of a twodimensional (2D) spectrum are dominated by vibrational motion and do not reflect the electron, hole, and exciton dynamics directly. We find that the fifthorder nonlinear response is particularly sensitive to the charge transfer process. While thirdorder 2D spectroscopy detects the correlation between two coherences, fifthorder 2D spectroscopy (2D population spectroscopy) is here designed to detect correlations between the excited states during two different time periods.
 Authors:
 Max Planck Institute for the Structure and Dynamics of Matter, Hamburg (Germany)
 Department of Chemistry, Kyoto University, Kyoto (Japan)
 Publication Date:
 OSTI Identifier:
 22415898
 Resource Type:
 Journal Article
 Resource Relation:
 Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 21; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
 Country of Publication:
 United States
 Language:
 English
 Subject:
 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; CORRELATIONS; COUPLING; ELECTRON SPECTRA; ELECTRON SPECTROSCOPY; ELECTRONS; EQUATIONS OF MOTION; EXCITED STATES; EXCITONS; HOLES; NONLINEAR PROBLEMS; OSCILLATORS; SPECTRAL DENSITY; TWODIMENSIONAL SYSTEMS
Citation Formats
Dijkstra, Arend G., Email: arend.dijkstra@mpsd.mpg.de, Email: tanimura@kuchem.kyotou.ac.jp, and Tanimura, Yoshitaka, Email: arend.dijkstra@mpsd.mpg.de, Email: tanimura@kuchem.kyotou.ac.jp. Linear and third and fifthorder nonlinear spectroscopies of a charge transfer system coupled to an underdamped vibration. United States: N. p., 2015.
Web. doi:10.1063/1.4917025.
Dijkstra, Arend G., Email: arend.dijkstra@mpsd.mpg.de, Email: tanimura@kuchem.kyotou.ac.jp, & Tanimura, Yoshitaka, Email: arend.dijkstra@mpsd.mpg.de, Email: tanimura@kuchem.kyotou.ac.jp. Linear and third and fifthorder nonlinear spectroscopies of a charge transfer system coupled to an underdamped vibration. United States. doi:10.1063/1.4917025.
Dijkstra, Arend G., Email: arend.dijkstra@mpsd.mpg.de, Email: tanimura@kuchem.kyotou.ac.jp, and Tanimura, Yoshitaka, Email: arend.dijkstra@mpsd.mpg.de, Email: tanimura@kuchem.kyotou.ac.jp. 2015.
"Linear and third and fifthorder nonlinear spectroscopies of a charge transfer system coupled to an underdamped vibration". United States.
doi:10.1063/1.4917025.
@article{osti_22415898,
title = {Linear and third and fifthorder nonlinear spectroscopies of a charge transfer system coupled to an underdamped vibration},
author = {Dijkstra, Arend G., Email: arend.dijkstra@mpsd.mpg.de, Email: tanimura@kuchem.kyotou.ac.jp and Tanimura, Yoshitaka, Email: arend.dijkstra@mpsd.mpg.de, Email: tanimura@kuchem.kyotou.ac.jp},
abstractNote = {We study hole, electron, and exciton transports in a charge transfer system in the presence of underdamped vibrational motion. We analyze the signature of these processes in the linear and third, and fifthorder nonlinear electronic spectra. Calculations are performed with a numerically exact hierarchical equations of motion method for an underdamped Brownian oscillator spectral density. We find that combining electron, hole, and exciton transfers can lead to nontrivial spectra with more structure than with excitonic coupling alone. Traces taken during the waiting time of a twodimensional (2D) spectrum are dominated by vibrational motion and do not reflect the electron, hole, and exciton dynamics directly. We find that the fifthorder nonlinear response is particularly sensitive to the charge transfer process. While thirdorder 2D spectroscopy detects the correlation between two coherences, fifthorder 2D spectroscopy (2D population spectroscopy) is here designed to detect correlations between the excited states during two different time periods.},
doi = {10.1063/1.4917025},
journal = {Journal of Chemical Physics},
number = 21,
volume = 142,
place = {United States},
year = 2015,
month = 6
}

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