Motional Narrowing through Photonic Exchange: Rational Suppression of Excitonic Disorder from Molecular Cavity Polariton Formation

Motional Narrowing through Photonic Exchange: Rational Suppression of Excitonic Disorder from Molecular Cavity Polariton Formation

Maximizing the coherence between the constituents of molecular materials remains a crucial goal toward the implementation of these systems into everyday optoelectronic technologies. Here we experimentally assess the ability of strong light–matter coupling in the collective limit to reduce energetic...

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Bibliographic Details
Published in:The journal of physical chemistry letters Vol. 15; no. 9; pp. 2405 - 2418
Main Authors: Wanasinghe, Sachithra T., Gjoni, Adelina, Burson, Wade, Majeski, Caris, Zaslona, Bradley, Rury, Aaron S.
Format: Journal Article
Language:English
Published: United States American Chemical Society 07-03-2024
Subjects:
Letter
Physical Insights into Light Interacting with Matter
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Summary:Maximizing the coherence between the constituents of molecular materials remains a crucial goal toward the implementation of these systems into everyday optoelectronic technologies. Here we experimentally assess the ability of strong light–matter coupling in the collective limit to reduce energetic disorder using porphyrin-based chromophores in Fabry–Pérot (FP) microresonator structures. Following characterization of cavity polaritons formed from chemically distinct porphyrin dimers, we find that the peaks corresponding to the lower polariton (LP) state in each sample do not possess widths consistent with conventional theories. We model the behavior of the polariton peak widths effectively using the results of spectroscopic theory. We correlate differences in the suppression of excitonic energetic disorder between our samples with microscopic light–matter interactions and propose that the suppression stems from photonic exchange. Our results demonstrate that cavity polariton formation can suppress disorder and show researchers how to design coherence into hybrid molecular material systems.
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USDOE
SC-0022134
ISSN:1948-7185
1948-7185
DOI:10.1021/acs.jpclett.3c03217