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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. https://resolver.caltech.edu/CaltechAUTHORS:20200909-152203413

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Abstract

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
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.jpcb.0c07935DOIArticle
ORCID:
AuthorORCID
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
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200909-152203413
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
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:09 Sep 2020 23:10
Last Modified:12 Oct 2020 17:57

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