Two-dimensional vibrational-electronic spectroscopy

Courtney, Trevor L.; Fox, Zachary W.; Slenkamp, Karla M.; Khalil, Munira

doi:10.1063/1.4932983

Title: Two-dimensional vibrational-electronic spectroscopy

Journal Article · Wed Oct 21 00:00:00 EDT 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4932983· OSTI ID:1469485

Courtney, Trevor L. ^[1]; Fox, Zachary W. ^[1]; Slenkamp, Karla M. ^[1]; Khalil, Munira ^[1]

Univ. of Washington, Seattle, WA (United States). Dept. of Chemistry

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 (ν_CN) and either a ligand-to-metal charge transfer transition ([Fe^III(CN)₆]^3- dissolved in formamide) or a metal-to-metal charge transfer (MMCT) transition ([(CN)₅Fe^IICNRu^III(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 ν_CN 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.

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Research Organization:: Univ. of Washington, Seattle, WA (United States)

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

Grant/Contract Number:: SC0012450; SC0002190

OSTI ID:: 1469485

Alternate ID(s):: OSTI ID: 1224223

Journal Information:: Journal of Chemical Physics, Vol. 143, Issue 15; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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Cited by: 48 works

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Implementation of continuous fast scanning detection in femtosecond Fourier-transform two-dimensional vibrational-electronic spectroscopy to decrease data acquisition time Fox, Zachary W.; Blair, Tyler J.; Weakly, Robert B. Review of Scientific Instruments, Vol. 89, Issue 11 https://doi.org/10.1063/1.5048523	journal	November 2018
Multispectral multidimensional spectrometer spanning the ultraviolet to the mid-infrared Song, Yin; Konar, Arkaprabha; Sechrist, Riley Review of Scientific Instruments, Vol. 90, Issue 1 https://doi.org/10.1063/1.5055244	journal	January 2019
Two-dimensional vibronic spectra from classical trajectories Polley, Kritanjan; Loring, Roger F. The Journal of Chemical Physics, Vol. 150, Issue 16 https://doi.org/10.1063/1.5093911	journal	April 2019
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
Two-dimensional electronic-Raman spectroscopy Zhang, Zhengyang; Huerta-Viga, Adriana; Tan, Howe-Siang Optics Letters, Vol. 43, Issue 4 https://doi.org/10.1364/ol.43.000939	journal	January 2018
Ultrafast structural molecular dynamics investigated with 2D infrared spectroscopy methods Kraack, Jan Philip Topics in Current Chemistry Collections https://doi.org/10.1007/978-3-030-02478-9_4	book	October 2017
Charge-transfer and impulsive electronic-to-vibrational energy conversion in ferricyanide: ultrafast photoelectron and transient infrared studies Ojeda, José; Arrell, Christopher A.; Longetti, Luca Royal Society of Chemistry https://doi.org/10.5167/uzh-157854	text	January 2017

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Title: Two-dimensional vibrational-electronic spectroscopy

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