Isolated Ground-State Vibrational Coherence Measured by Fifth-Order Single-Shot Two-Dimensional Electronic Spectroscopy

William O. Hutson, Austin P. Spencer, Elad Harel*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

10 Scopus citations

Abstract

Vibrations play a critical role in many photochemical and photophysical processes in which excitations reside on the electronically excited state. However, difficulty in assigning signals from spectroscopic measurements uniquely to a specific electronic state, ground or otherwise, has exposed limitations to their physical interpretation. Here, we demonstrate the selective excitation of vibrational coherences on the ground electronic state through impulsive Raman scattering, whose weak fifth-order signal is resonantly enhanced by coupling to strong electronic transitions. The six-wave mixing signals measured using this technique are free of lower-order cascades and represent correlations between zero-quantum vibrational coherences in the ground state and single-quantum coherences between the ground and electronic states. We believe that this technique has the potential to shed much-needed insight onto some of the mysteries regarding the origin of long-lived coherences observed in photosynthetic and other coupled chromophore systems.

Original languageEnglish (US)
Pages (from-to)3636-3640
Number of pages5
JournalJournal of Physical Chemistry Letters
Volume7
Issue number18
DOIs
StatePublished - Sep 15 2016

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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