4.6 Article

Ultrafast Coherence Delocalization in Real Space Simulated by Polaritons

期刊

ADVANCED OPTICAL MATERIALS
卷 10, 期 5, 页码 -

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adom.202102237

关键词

2D infrared spectra; coherence; hyperspectral imaging; molecular vibrational polaritons; quantum simulation; vibrational strong coupling

资金

  1. NSF CAREER Award [DMR1848215]
  2. Alfred P. Sloan Research Fellowship [FG-2020-12845]
  3. National Science Foundation [ECCS-1542148]
  4. UCSD
  5. Roger Tsien Fellowship from the Department of Chemistry and Biochemistry at UC San Diego

向作者/读者索取更多资源

Coherence delocalization has been studied on a coupled-cavity molecular polariton platform using ultrafast two-dimensional infrared hyperspectral imaging. Unidirectional coherence delocalization has been observed in frequency and real space. The dissipation of delocalized photon from high-energy to low-energy modes enables this directionality. Experiments further show that only energetically nearby polaritons can form coherences that survive long-range environmental fluctuations.
Coherence delocalization has been investigated on a coupled-cavity molecular polariton platform in time, frequency, and spatial domains, enabled by ultrafast two-dimensional infrared hyperspectral imaging. Unidirectional coherence delocalization (coherence prepared in one cavity transferred to another cavity) has been observed in frequency and real space. This directionality is enabled by the dissipation of delocalized photon from high-energy to low-energy modes, described by Lindblad dynamics. Further experiments show that when coherences are directly prepared between polaritons from different cavities, only energetically nearby polaritons can form coherences that survive the long-range environmental fluctuation. Together with the Lindblad dynamics, this result implies that coherences delocalize through a one-step mechanism where photons transfer from one cavity to another, shedding light to coherence evolution in natural and artificial quantum systems. This new optical platform based on molecular vibrational polariton thus demonstrates a way of combining photon and molecular modes to simulate coherence dynamics in the infrared regime.

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