Quantification of Exciton Fine Structure Splitting in a Two-Dimensional Perovskite Compound

Posmyk, Katarzyna; Zawadzka, Natalia; Dyksik, Mateusz; Surrente, Alessandro; Maude, Duncan K.; Kazimierczuk, Tomasz; Babiński, Adam; Molas, Maciej R.; Paritmongkol, Watcharaphol; Mączka, Mirosław; Tisdale, William A.; Płochocka, Paulina; Baranowski, Michał

doi:10.1021/acs.jpclett.2c00942

Quantification of Exciton Fine Structure Splitting in a Two-Dimensional Perovskite Compound

Journal Article · Fri May 13 00:00:00 EDT 2022 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.2c00942· OSTI ID:1904339

^[1]; Zawadzka, Natalia ^[2]; ^[3]; ^[4]; Maude, Duncan K. ^[5]; ^[2]; ^[2]; ^[2]; ^[6]; ^[7]; ^[6]; ^[3]; ^[4]

Wroclaw Univ. of Science and Technology (Poland); OSTI
Univ. of Warsaw (Poland)
Univ. of Toulouse (France); Wroclaw Univ. of Science and Technology (Poland)
Wroclaw Univ. of Science and Technology (Poland)
Univ. of Toulouse (France)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Polish Academy of Sciences (PAS), Wroclaw (Poland). Institute of Low Temperature and Structure Research

Applications of two-dimensional (2D) perovskites have significantly outpaced the understanding of many fundamental aspects of their photophysics. The optical response of 2D lead halide perovskites is dominated by strongly bound excitonic states. However, a comprehensive experimental verification of the exciton fine structure splitting and associated transition symmetries remains elusive. Here we employ low temperature magneto-optical spectroscopy to reveal the exciton fine structure of (PEA)₂PbI₄ (here PEA is phenylethylammonium) single crystals. We observe two orthogonally polarized bright in-plane free exciton (FX) states, both accompanied by a manifold of phonon-dressed states that preserve the polarization of the corresponding FX state. Introducing a magnetic field perpendicular to the 2D plane, we resolve the lowest energy dark exciton state, which although theoretically predicted, has systematically escaped experimental observation (in Faraday configuration) until now. These results corroborate standard multiband, effective-mass theories for the exciton fine structure in 2D perovskites and provide valuable quantification of the fine structure splitting in (PEA)₂PbI₄.

View Accepted Manuscript (DOE)

Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Centre Poland; Ministry of Science and Higher Education, Poland

Grant/Contract Number:: SC0019345

OSTI ID:: 1904339

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 20 Vol. 13; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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