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Nonlinear terahertz coherent excitation of vibrational modes of liquids

Allodi, Marco A. and Finneran, Ian A. and Blake, Geoffrey A. (2015) Nonlinear terahertz coherent excitation of vibrational modes of liquids. Journal of Chemical Physics, 143 (23). Art. No. 234204. ISSN 0021-9606.

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We report the first coherent excitation of intramolecular vibrational modes via the nonlinear interaction of a TeraHertz (THz) light field with molecular liquids. A terahertz-terahertz-Raman pulse sequence prepares the coherences with a broadband, high-energy, (sub)picosecond terahertz pulse, that are then measured in a terahertz Kerr effect spectrometer via phase-sensitive, heterodyne detection with an optical pulse. The spectrometer reported here has broader terahertz frequency coverage, and an increased sensitivity relative to previously reported terahertz Kerr effect experiments. Vibrational coherences are observed in liquid diiodomethane at 3.66 THz (122 cm^(−1)), and in carbon tetrachloride at 6.50 THz (217 cm^(−1)), in exact agreement with literature values of those intramolecular modes. This work opens the door to 2D spectroscopies, nonlinear in terahertz field, that can study the dynamics of condensed-phase molecular systems, as well as coherent control at terahertz frequencies.

Item Type:Article
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URLURL TypeDescription
Allodi, Marco A.0000-0002-3289-1659
Finneran, Ian A.0000-0003-2506-4652
Blake, Geoffrey A.0000-0003-0787-1610
Additional Information:© 2015 AIP Publishing LLC. Received 23 October 2015; accepted 7 December 2015; published online 21 December 2015. The authors gratefully acknowledge financial support from the National Science Foundation (Grant Nos. CHE-1214123, CHE-0722330, and the NSF Graduate Research Fellowship Program). M.A.A. acknowledges current support from a Yen Postdoctoral Fellowship from The Institute for Biophysical Dynamics at The University of Chicago.
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NSF Graduate Research FellowshipUNSPECIFIED
University of ChicagoUNSPECIFIED
Issue or Number:23
Record Number:CaltechAUTHORS:20160104-130158790
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Official Citation:Nonlinear terahertz coherent excitation of vibrational modes of liquids Allodi, Marco A. and Finneran, Ian A. and Blake, Geoffrey A., The Journal of Chemical Physics, 143, 234204 (2015), DOI:
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:63331
Deposited By: Tony Diaz
Deposited On:04 Jan 2016 23:20
Last Modified:10 Dec 2020 20:49

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