Determining the static electronic and vibrational energy correlations via two-dimensional electronic-vibrational spectroscopy

Dong, Hui; Lewis, Nicholas H.  C.; Oliver, Thomas A.  A.; Fleming, Graham R.

doi:10.1063/1.4919684

Title: Determining the static electronic and vibrational energy correlations via two-dimensional electronic-vibrational spectroscopy

Journal Article · Thu May 07 00:00:00 EDT 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4919684· OSTI ID:1254483

Dong, Hui ^[1];

^[1];

^[1]

Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States). Kavli Energy NanoSciences Institute

Changes in the electronic structure of pigments in protein environments and of polar molecules in solution inevitably induce a re-adaption of molecular nuclear structure. Both changes of electronic and vibrational energies can be probed with visible or infrared lasers, such as two-dimensional electronic spectroscopy or vibrational spectroscopy. The extent to which the two changes are correlated remains elusive. The recent demonstration of two-dimensional electronic-vibrational (2DEV) spectroscopy potentially enables a direct measurement of this correlation experimentally. However, it has hitherto been unclear how to characterize the correlation from the spectra. In this report, we present a theoretical formalism to demonstrate the slope of the nodal line between the excited state absorption and ground state bleach peaks in the spectra as a characterization of the correlation between electronic and vibrational transition energies. In conclusion, we also show the dynamics of the nodal line slope is correlated to the vibrational spectral dynamics. Additionally, we demonstrate the fundamental 2DEV spectral line-shape of a monomer with newly developed response functions

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Research Organization:: University of California, Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC03- 76SF000098; NSF CHE- 1012168; CHE-1362830

OSTI ID:: 1254483

Alternate ID(s):: OSTI ID: 1228215

Journal Information:: Journal of Chemical Physics, Vol. 142, Issue 17; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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Recent advances in multidimensional ultrafast spectroscopy Oliver, Thomas A. A. Royal Society Open Science, Vol. 5, Issue 1 https://doi.org/10.1098/rsos.171425	journal	January 2018
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