Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase

Jian Lu, Yaqing Zhang, Harold Y. Hwang, Benjamin K. Ofori-Okai, Sharly Fleischer, Keith A. Nelson*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

95 Scopus citations

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.

Original languageEnglish
Pages (from-to)11800-11805
Number of pages6
JournalProceedings of the National Academy of Sciences of the United States of America
Volume113
Issue number42
DOIs
StatePublished - 18 Oct 2016

Funding

FundersFunder number
Defense UniversityN00014-15-1-2879
National Science FoundationCHE-1111557
Office of Naval ResearchN00014-13-1-0509
Directorate for Mathematical and Physical Sciences1111557
Samsung
Marie Curie631628
Israel Science Foundation1065/14

    Keywords

    • Multidimensional coherent spectroscopy
    • Rotational dynamics
    • Terahertz
    • Ultrafast spectroscopy

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