Linear and third- and fifth-order nonlinear spectroscopies of a charge transfer 
system coupled to an underdamped vibration

Dijkstra, Arend; Tanimura, Yoshitaka

doi:10.1063/1.4917025

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Linear and third- and fifth-order nonlinear spectroscopies of a charge transfer system coupled to an underdamped vibration

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Dijkstra, Arend
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

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http://dx.doi.org/10.1063/1.4917025
(Publisher version)

http://arxiv.org/abs/1502.06410
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1.4917025.pdf
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Citation

Dijkstra, A., & Tanimura, Y. (2015). Linear and third- and fifth-order nonlinear spectroscopies of a charge transfer system coupled to an underdamped vibration. The Journal of Chemical Physics, 142(21): 212423. doi:10.1063/1.4917025.

Cite as: https://hdl.handle.net/11858/00-001M-0000-0026-D0A7-D

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 fifth-order 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 non-trivial spectra with more structure than with excitonic coupling alone. Traces taken during the waiting time of a two-dimensional (2D) spectrum are dominated by vibrational motion and do not reflect the electron, hole, and exciton dynamics directly. We find that the fifth-order nonlinear response is particularly sensitive to the charge transfer process. While third-order 2D spectroscopy detects the correlation between two coherences, fifth-order 2D spectroscopy (2D population spectroscopy) is here designed to detect correlations between the excited states during two different time periods.