Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 8, Issue 18, Pages 4640-4644Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.7b02106
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Funding
- National Science Foundation [CHE-1214123, CHE-1057112]
- Deutsche Forschungsgemeinschaft [WE 5762/1-1]
- Institute for Biophysical Dynamics at the University of Chicago
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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.
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