Understanding Radiative Transitions and Relaxation Pathways in Plexcitons
| Autor: | Lukas Wittenbecher, Sinan Balci, Donatas Zigmantas, Sema Sarisozen, Tõnu Pullerits, Iulia Minda, Daniel Finkelstein-Shapiro, Pierre-Adrien Mante |
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| Jazyk: | angličtina |
| Rok vydání: | 2020 |
| Předmět: |
General Chemical Engineering
FOS: Physical sciences Physics::Optics 02 engineering and technology 010402 general chemistry 01 natural sciences Biochemistry Electron spectroscopy Physics - Chemical Physics Materials Chemistry Polariton Radiative transfer Environmental Chemistry Plasmon Chemical Physics (physics.chem-ph) Physics Plasmonic nanoparticles Quantum Physics Biochemistry (medical) General Chemistry 021001 nanoscience & nanotechnology 0104 chemical sciences Coupling (physics) Chemical physics Relaxation (physics) Quantum Physics (quant-ph) 0210 nano-technology Coherence (physics) |
| Popis: | Molecular aggregates on plasmonic nanoparticles have emerged as attractive systems for the studies of cavity quantum electrodynamics. They are highly tunable, scalable, easy to synthesize and offer sub-wavelength confinement, all while giving access to the ultrastrong light-matter coupling regime at room temperature and promising a plethora of applications. However, the complexity of both the molecular aggregate and plasmonic nanoparticle introduces many more processes affecting the excitation and its relaxation, than are present in atom-cavity systems. Here, we follow the complex relaxation pathways of the photoexcitation of such hybrid systems and conclude that while the metal is responsible for destroying the coherence of the excitation, the molecular aggregate significantly participates in dissipating the energy. We rely on two-dimensional electronic spectroscopy in a combined theory-experiment approach, which allows us to ascribe the different timescales of relaxation to processes inside the molecules or the metal nanoparticle. We show that the dynamics beyond a few femtoseconds has to be cast in the language of hot electron distributions and excitons instead of the accepted lower and upper polariton branches, and furthermore set the framework for delving deeper into the photophysics of excitations that could be used in hot electron transfer, for example to drive photocatalytic reactions. revised simulations and interpretation |
| Databáze: | OpenAIRE |
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