Deciphering between enhanced light emission and absorption in multi-mode porphyrin cavity polariton samples

Odewale, Elizabeth O.; Avramenko, Aleksandr G.; Rury, Aaron S.

doi:10.1515/nanoph-2023-0748

Title: Deciphering between enhanced light emission and absorption in multi-mode porphyrin cavity polariton samples

Journal Article · 14 March 2024 · Nanophotonics (Online)

DOI: https://doi.org/10.1515/nanoph-2023-0748 · OSTI ID:2323969

Odewale, Elizabeth O. ^[1]; Avramenko, Aleksandr G. ^[1];

^[1]

Materials Structural Dynamics Laboratory, Department of Chemistry , 2954 Wayne State University , 48202 , Detroit , MI , USA

Abstract It remains unclear how the collective strong coupling of cavity-confined photons to the electronic transitions of molecular chromophore leverages the distinct properties of the polaritonic constituents for future technologies. In this study, we design, fabricate, and characterize multiple types of Fabry-Pérot (FP) mirco-resonators containing copper(II) tetraphenyl porphyrin (CuTPP) to show how cavity polariton formation affects radiative relaxation processes in the presence of substantial non-Condon vibronic coupling between two of this molecule’s excited electronic states. Unlike the prototypical enhancement of Q state radiative relaxation of CuTPP in a FP resonator incapable of forming polaritons, we find the light emission processes in multimode cavity polariton samples become enhanced for cavity-exciton energy differences near those of vibrations known to mediate non-Condon vibronic coupling. We propose the value of this detuning is consistent with radiative relaxation of Herzberg-Teller polaritons into collective molecular states coupled to the cavity photon coherently. We contrast the feature stemming from light emission from the HT polariton state with those that occur due to polariton-enhanced light absorption. Our results demonstrate the landscape of molecular and photonic interactions enabled by cavity polariton formation using complex chromophores and how researchers can design resonators to leverage these interactions to characterize and control polaritonic properties.

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Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0022134

OSTI ID:: 2323969

Journal Information:: Nanophotonics (Online), Journal Name: Nanophotonics (Online) Journal Issue: 14 Vol. 13; ISSN 2192-8614

Publisher:: Walter de Gruyter GmbHCopyright Statement

Country of Publication:: Germany

Language:: English

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