Theory of Nonlinear Excitonic Response of Hybrid Organic Perovskites in the Regime of Strong Light-Matter Coupling

A. D. Belogur, D. A. Baghdasaryan, I. V. Iorsh, I. A. Shelykh, V. Shahnazaryan*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

We present a quantitative study of the nonlinear optical response of layered perovskites placed inside planar photonic microcavities in the regime of strong light-matter coupling, when excitonic and photonic modes hybridize and give rise to cavity polaritons. Two sources of nonlinearity are specified, the saturation of the excitonic transition with increase of the optical pump and Coulomb interaction between the excitons. It is demonstrated that a peculiar form of the interaction potential, specific to the multilayer structure of organic perovskites, is responsible for the substantial increase of the exciton binding energy and Rabi splitting with respect to conventional semiconductor systems. This results in a dominant contribution of the Rabi splitting quench effect in the nonlinear optical response. Moreover, due to the tightly bound character of excitons, the density of Mott transition is essentially higher, allowing extremely large polariton blueshifts of about 20 meV to be reached, which is an order of magnitude higher than in conventional semiconductors.

Original languageEnglish
Article number044048
JournalPhysical Review Applied
Volume17
Issue number4
DOIs
Publication statusPublished - Apr 2022

Bibliographical note

Funding Information:
This work is supported by the RA Science Committee and Russian Foundation for Basic Research (RF) in the frames of the joint research project SCS 20RF-048 and RFBR 20-52-05005 accordingly. I.A.S. and V.S. acknowledge support from the Icelandic Research Fund (project “Hybrid polaritonics”). V.S. thanks the University of Iceland for the hospitality. The work was financially supported by the Program Priority 2030. I.V.I. thanks the Russian Foundation for Basic Research (project 20-02-00084).

Publisher Copyright:
© 2022 American Physical Society.

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