Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase
Name
Lu-2016-Nonlinear two-dimensional terahertz ph.pdf
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1.59 MB
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Checksum (MD5)
30048a746f43155987ced45892ac6377
Author(s)
Fleischer, Sharly
Lu, Jian
Zhang, Yaqing
Hwang, Harold Y.
Ofori-Okai, Benjamin Kwasi
Nelson, Keith Adam
Date Issued
October 2016
Journal
Proceedings of the National Academy of Sciences
Publisher
National Academy of Sciences (U.S.)
Citation
Lu, Jian; Zhang, Yaqing; Hwang, Harold Y.; Ofori-Okai, Benjamin K.; Fleischer, Sharly and Nelson, Keith A. “Nonlinear Two-Dimensional Terahertz Photon Echo and Rotational Spectroscopy in the Gas Phase.” Proceedings of the National Academy of Sciences 113, no. 42 (October 2016): 11800–11805. © National Academy of Sciences
Version
Final published version
Abstract
Ultrafast 2D spectroscopy uses correlated multiple light−matter interactions for retrieving dynamic features that may otherwise be hidden under the linear spectrum; its extension to the terahertz regime of the electromagnetic spectrum, where a rich variety of material degrees of freedom reside, remains an experimental challenge. We report a demonstration of ultrafast 2D terahertz spectroscopy of gas-phase molecular rotors at room temperature. Using time-delayed terahertz pulse pairs, we observe photon echoes and other nonlinear signals resulting from molecular dipole orientation induced by multiple terahertz field−dipole interactions. The nonlinear time domain orientation signals are mapped into the frequency domain in 2D rotational spectra that reveal J-state-resolved nonlinear rotational dynamics. The approach enables direct observation of correlated rotational transitions and may reveal rotational coupling and relaxation pathways in the ground electronic and vibrational state.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
https://doi.org/10.1073/pnas.1609558113
