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Transient two-dimensional electronic spectroscopy: coherent dynamics at arbitrary times along the reaction coordinate

Mandal, Aritra, Schultz, Jonathan D., Wu, Yi-Lin, Coleman, Adam F., Young, Ryan M. and Wasielewski, Michael R. 2019. Transient two-dimensional electronic spectroscopy: coherent dynamics at arbitrary times along the reaction coordinate. Journal of Physical Chemistry Letters 10 , pp. 3509-3515. 10.1021/acs.jpclett.9b00826

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Abstract

Recent advances in two-dimensional electronic spectroscopy (2DES) have enabled identification of fragile quantum coherences in condensed-phase systems near the equilibrium molecular geometry. In general, traditional 2DES cannot measure such coherences associated with photophysical processes that occur at times significantly after the initially prepared state has dephased, such as the evolution of the initial excited state into a charge transfer state. We demonstrate the use of transient two-dimensional electronic spectroscopy (t-2DES) to probe coherences in an electron donor–acceptor dyad consisting of a perylenediimide (PDI) acceptor and a perylene (Per) donor. An actinic pump pulse prepares the lowest excited singlet state of PDI followed by formation of the PDI•––Per•+ ion pair, which is probed at different times following the actinic pulse using 2DES. Analysis of the observed coherences provides information about electronic, vibronic, and vibrational interactions at any time along the reaction coordinate for ion pair formation.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Publisher: American Chemical Society
ISSN: 1948-7185
Funders: National Science Foundation
Date of First Compliant Deposit: 19 June 2019
Date of Acceptance: 6 June 2019
Last Modified: 06 Jun 2020 02:05
URI: http://orca.cf.ac.uk/id/eprint/123564

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