Transient Two-Dimensional Electronic Spectroscopy: Coherent Dynamics at Arbitrary Times along the Reaction Coordinate

Aritra Mandal, Jonathan D. Schultz, Yi Lin Wu, Adam F. Coleman, Ryan M. Young, Michael R. Wasielewski

Research output: Contribution to journalArticle

1 Citation (Scopus)

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.

Original languageEnglish
Pages (from-to)3509-3515
Number of pages7
JournalJournal of Physical Chemistry Letters
Volume10
Issue number13
DOIs
Publication statusPublished - Jul 5 2019

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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