Bright Excitonic Fine Structure in Metal-Halide Perovskites: From Two-Dimensional to Bulk

Posmyk, Katarzyna; Zawadzka, Natalia; Kipczak, Łucja; Dyksik, Mateusz; Surrente, Alessandro; Maude, Duncan K.; Kazimierczuk, Tomasz; Babiński, Adam; Molas, Maciej R.; Bumrungsan, Wakul; Chooseng, Chanisara; Paritmongkol, Watcharaphol; Tisdale, William A.; Baranowski, Michał; Plochocka, Paulina

doi:10.1021/jacs.3c11957

Title: Bright Excitonic Fine Structure in Metal-Halide Perovskites: From Two-Dimensional to Bulk

Journal Article · 07 February 2024 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.3c11957 · OSTI ID:2290432

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^[3]; Maude, Duncan K. ^[4];

^[2]; Babiński, Adam ^[2];

^[2]; Bumrungsan, Wakul ^[5]; Chooseng, Chanisara ^[5];

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Wroclaw University of Science and Technology (Poland); Université Toulouse (France)
University of Warsaw (Poland)
Wroclaw University of Science and Technology (Poland)
Université Toulouse (France)
Vidyasirimedhi Institute of Science and Technology (VISTEC), Rayong (Thailand)
Massachusetts Institute of Technology, Cambridge, MA (United States); Vidyasirimedhi Institute of Science and Technology (VISTEC), Rayong (Thailand)
Massachusetts Institute of Technology, Cambridge, MA (United States)

The optical response of two-dimensional (2D) perovskites, often referred to as natural quantum wells, is primarily governed by excitons, whose properties can be readily tuned by adjusting the perovskite layer thickness. We have investigated the exciton fine structure splitting in the archetypal 2D perovskite (PEA)₂(MA)_n–1PbnI_3n+1 with varying numbers of inorganic octahedral layers n = 1, 2, 3, and 4. We demonstrate that the in-plane excitonic states exhibit splitting and orthogonally oriented dipoles for all confinement regimes. The evolution of the exciton states in an external magnetic field provides further insights into the g-factors and diamagnetic coefficients. With increasing n, we observe a gradual evolution of the excitonic parameters characteristic of a 2D to three-dimensional transition. Our results provide valuable information concerning the evolution of the optoelectronic properties of 2D perovskites with the changing confinement strength.

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Research Organization:: Laboratoire National des Champs Magnetiques Intenses, Toulouse (France)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); MAESTRO; National Science Centre, Poland; Polish National Agency for Academic Exchange

Grant/Contract Number:: SC0019345; 2020/38/A/ST3/00214; 2020/39/D/ST3/03000; 2021/43/D/ST3/01444; BPN/BKK/2021/1/00002/U/00001; 2018/31/B/ST3/02111; 2017/27/B/ST3/00205

OSTI ID:: 2290432

Alternate ID(s):: OSTI ID: 2311091

Journal Information:: Journal of the American Chemical Society, Vol. 146, Issue 7; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Energy
Excitons
Magnetic properties
Optical properties
Perovskites

Title: Bright Excitonic Fine Structure in Metal-Halide Perovskites: From Two-Dimensional to Bulk

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