Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase
Author(s)
Fleischer, Sharly; Lu, Jian; Zhang, Yaqing; Hwang, Harold Y.; Ofori-Okai, Benjamin Kwasi; Nelson, Keith Adam; ... Show more Show less
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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.
Date issued
2016-10Department
Massachusetts Institute of Technology. Department of ChemistryJournal
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
ISSN
0027-8424
1091-6490