Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 113, Issue 25, Pages 6857-6861Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1605631113
Keywords
ultrafast dynamics; terahertz; coherent multidimensional spectroscopy
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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
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1214123, 1057112] Funding Source: National Science Foundation
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We present 2D terahertz-terahertz-Raman (2D TTR) spectroscopy, the first technique, to our knowledge, to interrogate a liquid with multiple pulses of terahertz (THz) light. This hybrid approach isolates nonlinear signatures in isotropic media, and is sensitive to the coupling and anharmonicity of thermally activated THz modes that play a central role in liquid-phase chemistry. Specifically, by varying the timing between two intense THz pulses, we control the orientational alignment of molecules in a liquid, and non-linearly excite vibrational coherences. A comparison of experimental and simulated 2D TTR spectra of bromoform (CHBr3), carbon tetrachloride (CCl4), and dibromodichloromethane (CBr2Cl2) shows previously unobserved off-diagonal anharmonic coupling between thermally populated vibrational modes.
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