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Ultrafast Vibrational Dynamics for Molecular Polariton Chemistry

ORAL · Invited

Abstract

Molecular vibrational polaritons are hybrid half-light, half-matter quasiparticles. Because of their hybrid photon-matter characters, it has been shown that polaritons can modify molecular potential enrgy landscapes and therefore chemical reactions. Using pump-probe and 2D IR spectroscopy to study vibrational-polaritons, we learned interesting dynamics that shed light to polariton chemistry.

In this talk, I will briefly introduce the principles of using pump probe and 2D IR spectroscopy to follow polariton dynamics, and overview a few ultrafast phenomena of molecular vibrational-polaritons due to their hybridized nature: 1.  Cavity-enabled intermolecular energy transfer,  2. Polariton accelerated barrier crossing events, 3. Polariton coherence delocalization in spaces. These results will have significant implications in new polariton chemistry and polariton based quantum technologies. 

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Publication: 1. Xiang, B. et al. Intermolecular vibrational energy transfer enabled by microcavity strong light-matter coupling. Science (New York, N.Y.) 368, 665–667 (2020).<br>2.Xiang, B. & Xiong, W. Molecular vibrational polariton: Its dynamics and potentials in novel chemistry and quantum technology. The Journal of Chemical Physics 155, 050901 (2021).<br>3. Xiang, B. et al. Two-dimensional infrared spectroscopy of vibrational polaritons. Proceedings of the National Academy of Sciences of the United States of America 115, 4845–4850 (2018).<br>4. Xiang, B. et al. Manipulating optical nonlinearities of molecular polaritons by delocalization. Science Advances 5, (2019).<br>5. Yang, Z., Xiang, B. & Xiong, W. Controlling Quantum Pathways in Molecular Vibrational Polaritons. ACS Photonics 7, 919–924 (2020).<br>6. Xiang, B., Wang, J., Yang, Z. & Xiong, W. Nonlinear infrared polaritonic interaction between cavities mediated by molecular vibrations at ultrafast time scale. Science Advances 7, (2021).<br>7. Xiang, B., Yang, Z., You, Y.-Z. & Xiong, W. Ultrafast Coherence Delocalization in Real Space Simulated by Polaritons. Advanced Optical Materials, Accepted (2021).<br>8. Xiang, B. et al. State-Selective Polariton to Dark State Relaxation Dynamics. The Journal of Physical Chemistry A 123, 5918–5927 (2019).

Presenters

  • Wei Xiong

    University of California, San Diego

Authors

  • Wei Xiong

    University of California, San Diego