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Intermolecular vibrational energy transfer enabled by microcavity strong light–matter coupling

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Science  08 May 2020:
Vol. 368, Issue 6491, pp. 665-667
DOI: 10.1126/science.aba3544

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Atypical vibrational interactions

Vibrational energy transfer (VET) between solute molecules is generally unfavorable in liquids because of weak intermolecular forces. Xiang et al. measured the two-dimensional infrared spectrum of a molecular mixture, W(CO)6 and W(13CO)6, with saturated concentrations in a binary solvent embedded in an optical microcavity. This experiment showed that the VET between the asymmetric stretch vibrations of two solute molecules is enhanced via polaritonic intermediate states formed by a strong coupling with the cavity mode. The efficiency is modulated by the cavity lifetime, which provides an opportunity to control the VET process in the liquid phase. This could lead to various practical implementations.

Science, this issue p. 665

Abstract

Selective vibrational energy transfer between molecules in the liquid phase, a difficult process hampered by weak intermolecular forces, is achieved through polaritons formed by strong coupling between cavity photon modes and donor and acceptor molecules. Using pump-probe and two-dimensional infrared spectroscopy, we found that the excitation of the upper polariton, which is composed mostly of donors, can efficiently relax to the acceptors within ~5 picoseconds. The energy-transfer efficiency can be further enhanced by increasing the cavity lifetime, suggesting that the energy transfer is a polaritonic process. This vibrational energy-transfer pathway opens doors for applications in remote chemistry, sensing mechanisms, and vibrational polariton condensation.

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