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Low-frequency anharmonic couplings in bromoform revealed from 2D Raman-THz spectroscopy: From the liquid to the crystalline phase


Mousavi, Seyyed Jabbar; Berger, Arian; Hamm, Peter; Shalit, Andrey (2022). Low-frequency anharmonic couplings in bromoform revealed from 2D Raman-THz spectroscopy: From the liquid to the crystalline phase. Journal of Chemical Physics, 156(17):174501.

Abstract

Two-dimensional (2D) Raman-THz spectroscopy in the frequency of up to 7 THz has been applied to study the crystalline β-phase of bromoform (CHBr3). As for liquid CHBr3, cross peaks are observed, which, however, sharpen up in the crystalline sample and split into assignable sub-contributions. In the Raman dimension, the frequency positions of these cross peaks coincide with the intramolecular bending modes of the CHBr3 molecules and in the THz dimension with the IR-active lattice modes of the crystal. This work expands the applicability of this new 2D spectroscopic technique to solid samples at cryogenic temperatures. Furthermore, it provides new experimental evidence that the cross peaks, indeed, originate from the coupling between intra- and intermolecular vibrational modes.

Abstract

Two-dimensional (2D) Raman-THz spectroscopy in the frequency of up to 7 THz has been applied to study the crystalline β-phase of bromoform (CHBr3). As for liquid CHBr3, cross peaks are observed, which, however, sharpen up in the crystalline sample and split into assignable sub-contributions. In the Raman dimension, the frequency positions of these cross peaks coincide with the intramolecular bending modes of the CHBr3 molecules and in the THz dimension with the IR-active lattice modes of the crystal. This work expands the applicability of this new 2D spectroscopic technique to solid samples at cryogenic temperatures. Furthermore, it provides new experimental evidence that the cross peaks, indeed, originate from the coupling between intra- and intermolecular vibrational modes.

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Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > General Physics and Astronomy
Physical Sciences > Physical and Theoretical Chemistry
Uncontrolled Keywords:Physical and Theoretical Chemistry, General Physics and Astronomy
Language:English
Date:7 May 2022
Deposited On:04 Jan 2023 09:55
Last Modified:29 Mar 2024 02:37
Publisher:American Institute of Physics
ISSN:0021-9606
OA Status:Hybrid
Publisher DOI:https://doi.org/10.1063/5.0090520
PubMed ID:35525660
Project Information:
  • : FunderSwiss National Science Foundation (SNF) through the National Center of Competence and Research (NCCR) MUST
  • : Grant ID
  • : Project Title
  • : FunderMaxWater network of the Maxnbsp;Planck Society
  • : Grant ID
  • : Project Title
  • Content: Published Version
  • Language: English
  • Licence: Creative Commons: Attribution 4.0 International (CC BY 4.0)
  • Content: Accepted Version
  • Language: English