Hot electrons and singlet-fission dark excitons modulate strong-coupling conditions in metal-organic optical microcavities
arxiv(2024)
摘要
Polaritons, formed as a result of strong mixing between light and matter, are
promising for numerous applications including organic solar cells, optical
logic gates, and qubits. In low-Q organic optical microcavities, polaritonic
signatures due to strong hybridization between photons and Frenkel excitons
were found to decay together with the dynamics of dark excitons. A conundrum,
however, remained whether dark excitons modulate exciton-photon coupling
strength. It also remained unclear how dark excitons in the organic layer and
hot electrons in the metal layers contribute to shaping the long-lived optical
response at the energies of the hybrid states. Here, we identified that due to
delocalization of polaritons over both organic and metal layers, they are
sensitive to the effects of both dark excitons and hot electrons. We observed
that the dynamics of dark excitons modulate exciton-photon strong coupling
(Rabi energy). The role of metal layers is to contribute absorptive components
near the energies of the polaritonic branches; contributions from hot electrons
have also been detected. These and other mechanistic insights into the dynamics
of strong-coupling conditions were supported by theoretical analysis based on
non-Hermitian Hamiltonian mechanics, axially-resolved transfer-matrix
simulations, global analysis of pump-probe spectra, and statistical correlation
analysis. The developed methodology can be applied to other microcavity
structures. Our findings pave the way for disentangling pure polaritonic
effects from other excitations in organic and metal layers, with the ultimate
aim of achieving photonic control over photophysical and photochemical
processes.
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