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2D THz-THz-Raman Photon-Echo Spectroscopy of Molecular Vibrations in Liquid Bromoform

Finneran, Ian A. and Welsch, Ralph and Allodi, Marco A. and Miller, Thomas F., III and Blake, Geoffrey A. (2017) 2D THz-THz-Raman Photon-Echo Spectroscopy of Molecular Vibrations in Liquid Bromoform. Journal of Physical Chemistry Letters, 8 (18). pp. 4640-4644. ISSN 1948-7185. https://resolver.caltech.edu/CaltechAUTHORS:20170914-123518924

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Abstract

Fundamental properties of molecular liquids are governed by long-range interactions that most prominently manifest at terahertz (THz) frequencies. Here we report the detection of nonlinear THz photon-echo (rephasing) signals in liquid bromoform using THz-THz-Raman spectroscopy. Together, the many observed signatures span frequencies from 0.5 to 8.5 THz and result from couplings between thermally populated ladders of vibrational states. The strongest peaks in the spectrum are found to be multiquantum dipole and 1-quantum polarizability transitions and may arise from nonlinearities in the intramolecular dipole moment surface driven by intermolecular interactions.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.jpclett.7b02106DOIArticle
http://pubs.acs.org/doi/abs/10.1021/acs.jpclett.7b02106PublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/acs.jpclett.7b02106PublisherSupporting Information
ORCID:
AuthorORCID
Finneran, Ian A.0000-0003-2506-4652
Allodi, Marco A.0000-0002-3289-1659
Miller, Thomas F., III0000-0002-1882-5380
Blake, Geoffrey A.0000-0003-0787-1610
Additional Information:© 2017 American Chemical Society. Received: August 10, 2017; Accepted: September 6, 2017; Published: September 6, 2017. We acknowledge Dr. Mostafa Shalaby (Paul Scherrer Institut, Switzerland) for suggesting the use of a diamond window and polarizer beam combiner and the National Science Foundation (Grants CHE-1214123 and CHE-1057112) for financial support. We also thank Matt Welborn, Ioan Magdau, Brett Savoie, and Feizhi Ding for helpful discussions. R.W. acknowledges financial support from the Deutsche Forschungsgemeinschaft under grant number WE 5762/1-1. M.A.A. acknowledges current support from a Yen Postdoctoral Fellowship from the Institute for Biophysical Dynamics at the University of Chicago. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
NSFCHE-1214123
NSFCHE-1057112
Deutsche Forschungsgemeinschaft (DFG)WE 5762/1-1
University of ChicagoUNSPECIFIED
Issue or Number:18
Record Number:CaltechAUTHORS:20170914-123518924
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170914-123518924
Official Citation:2D THz-THz-Raman Photon-Echo Spectroscopy of Molecular Vibrations in Liquid Bromoform Ian A. Finneran, Ralph Welsch, Marco A. Allodi, Thomas F. Miller, III, and Geoffrey A. Blake The Journal of Physical Chemistry Letters 2017 8 (18), 4640-4644 DOI: 10.1021/acs.jpclett.7b02106
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:81443
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:14 Sep 2017 22:03
Last Modified:03 Oct 2019 18:42

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