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


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.

SUBMITTER: Lu J 

PROVIDER: S-EPMC5081644 | biostudies-literature | 2016 Oct

REPOSITORIES: biostudies-literature

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

Lu Jian J   Zhang Yaqing Y   Hwang Harold Y HY   Ofori-Okai Benjamin K BK   Fleischer Sharly S   Nelson Keith A KA  

Proceedings of the National Academy of Sciences of the United States of America 20161004 42


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  ...[more]

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