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A method for the direct measurement of electronic site populations in a molecular aggregate using two-dimensional electronic-vibrational spectroscopy

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Original languageEnglish
Pages (from-to)124203-1-124203-13
Number of pages13
JournalJournal of Chemical Physics
Volume143
Early online date28 Sep 2015
DOIs
DateAccepted/In press - 9 Sep 2015
DateE-pub ahead of print - 28 Sep 2015
DatePublished (current) - 28 Sep 2015

Abstract

Two dimensional electronic spectroscopy has proved to be a valuable experimental technique to reveal electronic excitation dynamics in photosynthetic pigment-protein complexes, nanoscale semiconductors, organic photovoltaic materials, and many other types of systems. It does not, however, provide direct information concerning the spatial structure and dynamics of excitons. 2D infrared spectroscopy has become a widely used tool for studying structural dynamics but is incapable of directly providing information concerning electronic excited states. 2D electronic-vibrational (2DEV) spectroscopy provides a link between these domains, directly connecting the electronic excitation with the vibrational structure of the system under study. In this work, we derive response functions for the 2DEV spectrum of a molecular dimer and propose a method by which 2DEV spectra could be used to directly measure the electronic site populations as a function of time following the initial electronic excitation. We present results from the response function simulations which show that our proposed approach is substantially valid. This method provides, to our knowledge, the first direct experimental method for measuring the electronic excited state dynamics in the spatial domain, on the molecular scale.

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    Rights statement: © 2015 AIP Publishing LLC, This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article has been submitted to/accepted by [Journal of Chemical Physics]. After it is published, it will be found at (http://dx.doi.org/10.1063/1.4931634).

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