Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 113, Issue 42, Pages 11800-11805Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1609558113
Keywords
ultrafast spectroscopy; multidimensional coherent spectroscopy; terahertz; rotational dynamics
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Funding
- Office of Naval Research [N00014-13-1-0509]
- Defense University Research Instrumentation Program [N00014-15-1-2879]
- National Science Foundation [CHE-1111557]
- Samsung Global Research Outreach program
- Israel Science Foundation [1065/14]
- Marie Curie Career Integration Grant [631628]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1111557] Funding Source: National Science Foundation
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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.
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