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Isolating Polaritonic 2D-IR Transmission Spectra. | LitMetric

Isolating Polaritonic 2D-IR Transmission Spectra.

J Phys Chem Lett

Department of Chemistry, University of Michigan, 930 North University Avenue, Ann Arbor, Michigan 48109, United States.

Published: November 2021

Strong coupling between vibrational transitions in molecules within a resonant optical microcavity leads to the formation of collective, delocalized vibrational polaritons. There are many potential applications of "polaritonic chemistry", ranging from modified chemical reactivity to quantum information processing. One challenge in obtaining the polaritonic response is removing a background contribution due to the uncoupled molecules that generate an ordinary 2D-IR spectrum whose amplitude is filtered by the polariton transmission spectrum. We show that most features in 2D-IR spectra of vibrational polaritons can be explained by a linear superposition of this background signal and the true polariton response. Through a straightforward correction procedure, in which the filtered bare-molecule 2D-IR spectrum is subtracted from the measured cavity response, we recover the polaritonic spectrum.

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Source
http://dx.doi.org/10.1021/acs.jpclett.1c03198DOI Listing

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