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Title: Two-dimensional vibrational-electronic spectroscopy

Abstract

Two-dimensional vibrational-electronic (2D VE) spectroscopy is a femtosecond Fourier transform (FT) third-order nonlinear technique that creates a link between existing 2D FT spectroscopies in the vibrational and electronic regions of the spectrum. 2D VE spectroscopy enables a direct measurement of infrared (IR) and electronic dipole moment cross terms by utilizing mid-IR pump and optical probe fields that are resonant with vibrational and electronic transitions, respectively, in a sample of interest. We detail this newly developed 2D VE spectroscopy experiment and outline the information contained in a 2D VE spectrum. We then use this technique and its single-pump counterpart (1D VE) to probe the vibrational-electronic couplings between high frequency cyanide stretching vibrations (νCN) and either a ligand-to-metal charge transfer transition ([FeIII(CN)6]3- dissolved in formamide) or a metal-to-metal charge transfer (MMCT) transition ([(CN)5FeIICNRuIII(NH3)5]- dissolved in formamide). The 2D VE spectra of both molecules reveal peaks resulting from coupled high- and low-frequency vibrational modes to the charge transfer transition. The time-evolving amplitudes and positions of the peaks in the 2D VE spectra report on coherent and incoherent vibrational energy transfer dynamics among the coupled vibrational modes and the charge transfer transition. The selectivity of 2D VE spectroscopy to vibronic processes is evidenced frommore » the selective coupling of specific νCN modes to the MMCT transition in the mixed valence complex. The lineshapes in 2D VE spectra report on the correlation of the frequency fluctuations between the coupled vibrational and electronic frequencies in the mixed valence complex which has a time scale of 1 ps. Lastly, the details and results of this study confirm the versatility of 2D VE spectroscopy and its applicability to probe how vibrations modulate charge and energy transfer in a wide range of complex molecular, material, and biological systems.« less

Authors:
 [1];  [1];  [1];  [1]
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  1. Univ. of Washington, Seattle, WA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Univ. of Washington, Seattle, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1469485
Alternate Identifier(s):
OSTI ID: 1224223
Grant/Contract Number:  
SC0012450; SC0002190
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 143; Journal Issue: 15; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Courtney, Trevor L., Fox, Zachary W., Slenkamp, Karla M., and Khalil, Munira. Two-dimensional vibrational-electronic spectroscopy. United States: N. p., 2015. Web. doi:10.1063/1.4932983.
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Courtney, Trevor L., Fox, Zachary W., Slenkamp, Karla M., & Khalil, Munira. Two-dimensional vibrational-electronic spectroscopy. United States. https://doi.org/10.1063/1.4932983
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Courtney, Trevor L., Fox, Zachary W., Slenkamp, Karla M., and Khalil, Munira. Wed . "Two-dimensional vibrational-electronic spectroscopy". United States. https://doi.org/10.1063/1.4932983. https://www.osti.gov/servlets/purl/1469485.
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@article{osti_1469485,
title = {Two-dimensional vibrational-electronic spectroscopy},
author = {Courtney, Trevor L. and Fox, Zachary W. and Slenkamp, Karla M. and Khalil, Munira},
abstractNote = {Two-dimensional vibrational-electronic (2D VE) spectroscopy is a femtosecond Fourier transform (FT) third-order nonlinear technique that creates a link between existing 2D FT spectroscopies in the vibrational and electronic regions of the spectrum. 2D VE spectroscopy enables a direct measurement of infrared (IR) and electronic dipole moment cross terms by utilizing mid-IR pump and optical probe fields that are resonant with vibrational and electronic transitions, respectively, in a sample of interest. We detail this newly developed 2D VE spectroscopy experiment and outline the information contained in a 2D VE spectrum. We then use this technique and its single-pump counterpart (1D VE) to probe the vibrational-electronic couplings between high frequency cyanide stretching vibrations (νCN) and either a ligand-to-metal charge transfer transition ([FeIII(CN)6]3- dissolved in formamide) or a metal-to-metal charge transfer (MMCT) transition ([(CN)5FeIICNRuIII(NH3)5]- dissolved in formamide). The 2D VE spectra of both molecules reveal peaks resulting from coupled high- and low-frequency vibrational modes to the charge transfer transition. The time-evolving amplitudes and positions of the peaks in the 2D VE spectra report on coherent and incoherent vibrational energy transfer dynamics among the coupled vibrational modes and the charge transfer transition. The selectivity of 2D VE spectroscopy to vibronic processes is evidenced from the selective coupling of specific νCN modes to the MMCT transition in the mixed valence complex. The lineshapes in 2D VE spectra report on the correlation of the frequency fluctuations between the coupled vibrational and electronic frequencies in the mixed valence complex which has a time scale of 1 ps. Lastly, the details and results of this study confirm the versatility of 2D VE spectroscopy and its applicability to probe how vibrations modulate charge and energy transfer in a wide range of complex molecular, material, and biological systems.},
doi = {10.1063/1.4932983},
journal = {Journal of Chemical Physics},
number = 15,
volume = 143,
place = {United States},
year = {Wed Oct 21 00:00:00 EDT 2015},
month = {Wed Oct 21 00:00:00 EDT 2015}
}
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  • DOI: 10.1109/cleoe-iqec.2013.6801061

Optical Two-Dimensional Fourier Transform Spectroscopy of Semiconductors
conference, January 2009

  • Cundiff, S. T.; Bristow, A. D.; Karaiskaj, D.
  • Frontiers in Optics 2009/Laser Science XXV/Fall 2009 OSA Optics & Photonics Technical Digest
  • DOI: 10.1364/ls.2009.lswc3

Dual-Frequency 2D IR Photon Echo of a Hydrogen Bond
book, January 2005

Two-dimensional Raman-terahertz spectroscopy of water
text, January 2013

  • Savolainen, J.; Ahmed, S.; Hamm, P.
  • National Academy of Sciences
  • DOI: 10.5167/uzh-88173
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    • Zhang, Zhengyang; Huerta-Viga, Adriana; Tan, Howe-Siang
    • Optics Letters, Vol. 43, Issue 4
    • DOI: 10.1364/ol.43.000939

    Ultrafast structural molecular dynamics investigated with 2D infrared spectroscopy methods
    book, October 2017

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