Sum-Frequency Signals in 2D-Terahertz-Terahertz-Raman Spectroscopy
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.
Additional Information
© 2020 American Chemical Society. Received: September 1, 2020; Published: September 8, 2020. The authors declare no competing financial interest.Attached Files
Submitted - 2007.08694.pdf
Supplemental Material - jp0c07935_si_001.pdf
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Additional details
- Eprint ID
- 105304
- DOI
- 10.1021/acs.jpcb.0c07935
- Resolver ID
- CaltechAUTHORS:20200909-152203413
- Created
-
2020-09-09Created from EPrint's datestamp field
- Updated
-
2021-11-16Created from EPrint's last_modified field
- Caltech groups
- Division of Geological and Planetary Sciences (GPS)