Coherent two-dimensional terahertz-terahertz-Raman spectroscopy.

Authors:
Dr Marco A Allodi, PhD
Dr Marco A Allodi, PhD
The University of Chicago
Yen Postdoctoral Scholar
Laser Spectroscopy, Molecular Dynamics, Biophysics, Astrochemistry
Chicago, IL | USA

Proc Natl Acad Sci U S A 2016 06 6;113(25):6857-61. Epub 2016 Jun 6.

Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, CA 91125; Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125

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.

Download full-text PDF

Source
http://dx.doi.org/10.1073/pnas.1605631113DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC4922159PMC

Still can't find the full text of the article?

We can help you send a request to the authors directly.
June 2016
37 Reads
8 Citations
9.810 Impact Factor

Publication Analysis

Top Keywords

pulses control
4
thz pulses
4
intense thz
4
timing intense
4
control orientational
4
orientational alignment
4
nonlinearly excite
4
liquid nonlinearly
4
molecules liquid
4
alignment molecules
4
varying timing
4
chemistry varying
4
activated thz
4
thermally activated
4
anharmonicity thermally
4
coupling anharmonicity
4
thz modes
4
modes play
4
liquid-phase chemistry
4
central role
4

References

(Supplied by CrossRef)

Similar Publications