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Two-dimensional infrared spectroscopy of vibrational polaritons

Xiang, Bo ; Ribeiro, Raphael F. ; Dunkelberger, Adam D. ; Wang, Jiaxi ; Li, Yingmin ; Simpkins, Blake S. ; Owrutsky, Jeffrey C. ; Yuen-Zhou, Joel ; Xiong, Wei

Proceedings of the National Academy of Sciences - PNAS, 2018-05, Vol.115 (19), p.4845-4850 [Periódico revisado por pares]

United States: National Academy of Sciences

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  • Título:
    Two-dimensional infrared spectroscopy of vibrational polaritons
  • Autor: Xiang, Bo ; Ribeiro, Raphael F. ; Dunkelberger, Adam D. ; Wang, Jiaxi ; Li, Yingmin ; Simpkins, Blake S. ; Owrutsky, Jeffrey C. ; Yuen-Zhou, Joel ; Xiong, Wei
  • Assuntos: Anharmonicity ; Coherent light ; Infrared imaging systems ; Infrared spectra ; Infrared spectroscopy ; Organic chemistry ; Photonics ; Physical Sciences ; Polaritons ; Scientific imaging ; Spectroscopy ; Vibration
  • É parte de: Proceedings of the National Academy of Sciences - PNAS, 2018-05, Vol.115 (19), p.4845-4850
  • Notas: ObjectType-Article-1
    SourceType-Scholarly Journals-1
    ObjectType-Feature-2
    content type line 23
    Author contributions: B.X., A.D.D., J.W., Y.L., and W.X. designed research; B.X., A.D.D., J.W., Y.L., and W.X. performed research; B.X., R.F.R., A.D.D., B.S.S., J.C.O., J.Y.-Z., and W.X. analyzed data; R.F.R., A.D.D., B.S.S., J.C.O., J.Y.-Z., and W.X. developed the theoretical model; and B.X., R.F.R., A.D.D., B.S.S., J.C.O., J.Y.-Z., and W.X. wrote the paper.
    Edited by Stephen R. Forrest, University of Michigan, Ann Arbor, MI, and approved March 28, 2018 (received for review December 19, 2017)
  • Descrição: We report experimental 2D infrared (2D IR) spectra of coherent light–matter excitations—molecular vibrational polaritons. The application of advanced 2D IR spectroscopy to vibrational polaritons challenges and advances our understanding in both fields. First, the 2D IR spectra of polaritons differ drastically from free uncoupled excitations and a new interpretation is needed. Second, 2D IR uniquely resolves excitation of hybrid light–matter polaritons and unexpected dark states in a state-selective manner, revealing otherwise hidden interactions between them. Moreover, 2D IR signals highlight the impact of molecular anharmonicities which are applicable to virtually all molecular systems. A quantum-mechanical model is developed which incorporates both nuclear and electrical anharmonicities and provides the basis for interpreting this class of 2D IR spectra. This work lays the foundation for investigating phenomena of nonlinear photonics and chemistry of molecular vibrational polaritons which cannot be probed with traditional linear spectroscopy.
  • Editor: United States: National Academy of Sciences
  • Idioma: Inglês
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