| Literature DB >> 27274067 |
Ian A Finneran1, Ralph Welsch1, Marco A Allodi1, Thomas F Miller1, Geoffrey A Blake2.
Abstract
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 nonlinearly 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.Entities:
Keywords: coherent multidimensional spectroscopy; terahertz; ultrafast dynamics
Year: 2016 PMID: 27274067 PMCID: PMC4922159 DOI: 10.1073/pnas.1605631113
Source DB: PubMed Journal: Proc Natl Acad Sci U S A ISSN: 0027-8424 Impact factor: 11.205