The realization of efficient optical devices depends on the ability to harness strong nonlinearities, which are challenging to achieve with standard photonic systems. Exciton-polaritons formed in hybrid organic-inorganic perovskites offer a promising alternative, exhibiting strong interactions at room temperature (RT). Despite recent demonstrations showcasing a robust nonlinear response, further progress is hindered by an incomplete understanding of the microscopic mechanisms governing polariton interactions in perovskite-based strongly coupled systems. Here, we investigate the nonlinear properties of quasi-2D dodecylammonium lead iodide perovskite (n3-C12) crystals embedded in a planar microcavity. Polarization-resolved pump-probe measurements reveal the contribution of indirect exchange interactions assisted by dark states formation. Additionally, we identify a strong dependence of the unique spin-dependent interaction of polaritons on sample detuning. The results are pivotal for the advancement of polaritonics, and the tunability of the robust spin-dependent anisotropic interaction in n3-C12 perovskites makes this material a powerful choice for the realization of polaritonic circuits.
Origin of Exciton–Polariton Interactions and Decoupled Dark States Dynamics in 2D Hybrid Perovskite Quantum Wells
Fieramosca, Antonio
Primo
;Mastria, Rosanna;Dominici, Lorenzo;Polimeno, Laura;Pugliese, Marco;Prontera, Carmela Tania;De Marco, Luisa;Maiorano, Vincenzo;Todisco, Francesco;Ballarini, Dario;De Giorgi, Milena;Gigli, Giuseppe;Sanvitto, Daniele
2024
Abstract
The realization of efficient optical devices depends on the ability to harness strong nonlinearities, which are challenging to achieve with standard photonic systems. Exciton-polaritons formed in hybrid organic-inorganic perovskites offer a promising alternative, exhibiting strong interactions at room temperature (RT). Despite recent demonstrations showcasing a robust nonlinear response, further progress is hindered by an incomplete understanding of the microscopic mechanisms governing polariton interactions in perovskite-based strongly coupled systems. Here, we investigate the nonlinear properties of quasi-2D dodecylammonium lead iodide perovskite (n3-C12) crystals embedded in a planar microcavity. Polarization-resolved pump-probe measurements reveal the contribution of indirect exchange interactions assisted by dark states formation. Additionally, we identify a strong dependence of the unique spin-dependent interaction of polaritons on sample detuning. The results are pivotal for the advancement of polaritonics, and the tunability of the robust spin-dependent anisotropic interaction in n3-C12 perovskites makes this material a powerful choice for the realization of polaritonic circuits.File | Dimensione | Formato | |
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