Dynamics of self-hybridized exciton–polaritons in 2D halide perovskites

Journal Article · 31 December 2023 · Light, Science & Applications

DOI: https://doi.org/10.1038/s41377-023-01334-9 · OSTI ID:2274717

Anantharaman, Surendra B.; Lynch, Jason; Stevens, Christopher E. ; Munley, Christopher; Li, Chentao ; Hou, Jin ; Zhang, Hao; Torma, Andrew; Darlington, Thomas ; Coen, Francis; Li, Kevin; Majumdar, Arka ; Schuck, P. James; Mohite, Aditya; Harutyunyan, Hayk; Hendrickson, Joshua R. ; Jariwala, Deep

Abstract Excitons, bound electron–hole pairs, in two-dimensional hybrid organic inorganic perovskites (2D HOIPs) are capable of forming hybrid light-matter states known as exciton-polaritons (E–Ps) when the excitonic medium is confined in an optical cavity. In the case of 2D HOIPs, they can self-hybridize into E–Ps at specific thicknesses of the HOIP crystals that form a resonant optical cavity with the excitons. However, the fundamental properties of these self-hybridized E–Ps in 2D HOIPs, including their role in ultrafast energy and/or charge transfer at interfaces, remain unclear. Here, we demonstrate that >0.5 µm thick 2D HOIP crystals on Au substrates are capable of supporting multiple-orders of self-hybridized E–P modes. These E–Ps have high Q factors (>100) and modulate the optical dispersion for the crystal to enhance sub-gap absorption and emission. Through varying excitation energy and ultrafast measurements, we also confirm energy transfer from higher energy E–Ps to lower energy E–Ps. Finally, we also demonstrate that E–Ps are capable of charge transport and transfer at interfaces. Our findings provide new insights into charge and energy transfer in E–Ps opening new opportunities towards their manipulation for polaritonic devices.

• Research Organization: Columbia University, New York, NY (United States); Emory University, Atlanta, GA (United States)
• Sponsoring Organization: Air Force Office of Scientific Research (AFOSR); Air Force Research Laboratory; Army Research Office; National Nanotechnology Coordinated Infrastructure Program; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
• Grant/Contract Number: SC0019443; SC0020101
• OSTI ID: 2274717
• Journal Information: Light, Science & Applications, Journal Name: Light, Science & Applications Journal Issue: 1 Vol. 13; ISSN 2047-7538
• Publisher: Nature Publishing GroupCopyright Statement
• Country of Publication: United Kingdom
• Language: English