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Sum-Frequency Signals in 2D-Terahertz-Terahertz-Raman Spectroscopy

Mead, Griffin and Lin, Haw-Wei and Magdău, Ioan-Bogdan and Miller, Thomas F., III and Blake, Geoffrey A. (2020) Sum-Frequency Signals in 2D-Terahertz-Terahertz-Raman Spectroscopy. Journal of Physical Chemistry B, 124 (40). pp. 8904-8908. ISSN 1520-6106. doi:10.1021/acs.jpcb.0c07935.

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[img] PDF (2D-TTR single-shot spectrometer; 2D-TTR sensitivity to IRF; Halogenated methane purification; TKE response of HMs; THz field modeling; SF-RDM model. Figure S1: The optical path of the 2D-TTR single-shot spectrometer. Figure S2: Experimental (Exp)...) - Supplemental Material
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We demonstrate that halogenated methane (HM) two-dimensional (2D)-terahertz-terahertz-Raman (2D-TTR) spectra are determined by the complicated structure of the instrument response function (IRF) along ω₁ and by the molecular coherences along ω₂. Experimental improvements have helped increase the resolution and dynamic range of the measurements, including accurate THz pulse shape characterization. Sum-frequency excitations convolved with the IRF are found to quantitatively reproduce the 2D-TTR signal. A new reduced density matrix model that incorporates sum-frequency pathways, with linear and harmonic operators, fully supports this (re)interpretation of the 2D-TTR spectra.

Item Type:Article
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URLURL TypeDescription Paper
Mead, Griffin0000-0003-0067-4219
Lin, Haw-Wei0000-0002-5208-7385
Magdău, Ioan-Bogdan0000-0002-3963-5076
Miller, Thomas F., III0000-0002-1882-5380
Blake, Geoffrey A.0000-0003-0787-1610
Additional Information:© 2020 American Chemical Society. Received: September 1, 2020; Published: September 8, 2020. The authors declare no competing financial interest.
Issue or Number:40
Record Number:CaltechAUTHORS:20200909-152203413
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Official Citation:Sum-Frequency Signals in 2D-Terahertz-Terahertz-Raman Spectroscopy. Griffin Mead, Haw-Wei Lin, Ioan-Bogdan Magdău, Thomas F. Miller, and Geoffrey A. Blake. The Journal of Physical Chemistry B 2020 124 (40), 8904-8908; DOI: 10.1021/acs.jpcb.0c07935
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:105304
Deposited By: Tony Diaz
Deposited On:09 Sep 2020 23:10
Last Modified:16 Nov 2021 18:41

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