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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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)...)
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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 | ||||||
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| 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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