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Title: Understanding radiative transitions and relaxation pathways in plexcitons
Authors: Finkelstein-Shapiro, Daniel
Mante, Pierre-Adrien
Sarısözen, Sema
Wittenbecher, Lukas
Minda, Iulia
Balcı, Sinan
Pullerits, Tonu
Keywords: Cavity quantum electrodynamics
Excitation energy dissipation
Molecular aggregates
Issue Date: 2021
Publisher: Cell Press
Abstract: Molecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of polaritonic light-matter states, called plexcitons. Such systems are tunable, scalable, easy to synthesize, and offer sub-wavelength confinement, all while giving access to the ultrastrong light-matter coupling regime, promising a plethora of applications. However, the complexity of these materials prevented the understanding of their excitation and relaxation phenomena. Here, we follow the relaxation pathways in plexcitons and conclude that while the metal destroys the optical coherence, the molecular aggregate coupled to surface processes significantly contributes to the energy dissipation. We use two-dimensional electronic spectroscopy with theoretical modeling to assign the different relaxation processes to either molecules or metal nanoparticle. We show that the dynamics beyond a few femtoseconds has to be considered in the language of hot electron distributions instead of the accepted lower and upper polariton branches and establish the framework for further understanding.
ISSN: 2451-9294
Appears in Collections:Chemistry / Kimya
Photonics / Fotonik
Scopus İndeksli Yayınlar Koleksiyonu / Scopus Indexed Publications Collection
WoS İndeksli Yayınlar Koleksiyonu / WoS Indexed Publications Collection

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