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Journal Articles Journal of Physical Chemistry Letters Year : 2023

Reversible Switching of Strong Light–Matter Coupling Using Spin-Crossover Molecular Materials

Abstract

The formation of hybrid light–matter states through the resonant interaction of confined electromagnetic fields with matter excitations has emerged as a fascinating tool for controlling quantum-mechanical states and then manipulating the functionalities and chemical reactivity landscape of molecular materials. Here we report the first observation of switchable strong light–matter coupling involving bistable spin-crossover molecules. Spectroscopic measurements, supported by transfer-matrix and coupled-oscillator simulations, reveal Rabi splitting values of up to 550 meV, which at 15% of the molecular excitation energy enter the regime of ultrastrong coupling. We find that the thermally induced switching of molecules between their low-spin and high-spin states allows fine control of the light–matter hybridization strength, offering the appealing possibility of reversible switching between the ultrastrong- and weak-coupling regimes within a single photonic structure. Through this work, we show that spin-crossover molecular compounds constitute a promising class of active nanomaterials in the burgeoning context of tunable polaritonic devices and polaritonic chemistry.
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Dates and versions

hal-04174168 , version 1 (31-07-2023)

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Lijun Zhang, Karl Ridier, Oleksandr Ye. Horniichuk, Stéphane Calvez, Lionel Salmon, et al.. Reversible Switching of Strong Light–Matter Coupling Using Spin-Crossover Molecular Materials. Journal of Physical Chemistry Letters, 2023, 14 (30), pp.6840-6849. ⟨10.1021/acs.jpclett.3c01136⟩. ⟨hal-04174168⟩
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