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

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...

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Published in:The journal of physical chemistry letters 2023-08, Vol.14 (30), p.6840-6849
Main Authors: Zhang, Lijun, Ridier, Karl, Horniichuk, Oleksandr Ye, Calvez, Stéphane, Salmon, Lionel, Molnár, Gábor, Bousseksou, Azzedine
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cited_by cdi_FETCH-LOGICAL-a424t-f78bd58bde4f02bb9587db6ee279c20f5bce997d40f82f452d6c7af6dda5dc8e3
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container_end_page 6849
container_issue 30
container_start_page 6840
container_title The journal of physical chemistry letters
container_volume 14
creator Zhang, Lijun
Ridier, Karl
Horniichuk, Oleksandr Ye
Calvez, Stéphane
Salmon, Lionel
Molnár, Gábor
Bousseksou, Azzedine
description 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.
doi_str_mv 10.1021/acs.jpclett.3c01136
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source American Chemical Society:Jisc Collections:American Chemical Society Read & Publish Agreement 2022-2024 (Reading list)
subjects Chemical Sciences
Coordination chemistry
Optics
Physical Insights into Light Interacting with Matter
Physics
title Reversible Switching of Strong Light–Matter Coupling Using Spin-Crossover Molecular Materials
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