Tunable Broad Light Emission from 3D “Hollow” Bromide Perovskites through Defect Engineering

Spanopoulos, Ioannis; Hadar, Ido; Ke, Weijun; Guo, Peijun; Mozur, Eve M.; Morgan, Emily; Wang, Shuxin; Zheng, Ding; Padgaonkar, Suyog; Manjunatha Reddy, G. N.; Weiss, Emily A.; Hersam, Mark C.; Seshadri, Ram; Schaller, Richard D.; Kanatzidis, Mercouri G.

doi:10.1021/jacs.1c01727

Tunable Broad Light Emission from 3D “Hollow” Bromide Perovskites through Defect Engineering

Journal Article · Tue Apr 27 00:00:00 EDT 2021 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.1c01727· OSTI ID:1864311

^[1]; ^[1]; ^[1]; ^[2]; ^[3]; ^[3]; Wang, Shuxin ^[3]; Zheng, Ding ^[1]; Padgaonkar, Suyog ^[1]; ^[4]; ^[1]; ^[1]; ^[3]; Schaller, Richard D. ^[1]; ^[1]

Northwestern Univ., Evanston, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Univ. of California, Santa Barbara, CA (United States)
Univ. Lille (France)

We report hybrid halide perovskites consisting of corner-sharing metal halide octahedra and small cuboctahedral cages filled with counter cations have proven to be prominent candidates for many high-performance optoelectronic devices. The stability limits of their three-dimensional perovskite framework are defined by the size range of the cations present in the cages of the structure. In some cases, the stability of the perovskite-type structure can be extended even when the counterions violate the size and shape requirements, as is the case in the so-called "hollow" perovskites. In this work, we engineered a new family of 3D highly defective yet crystalline "hollow" bromide perovskites with general formula (FA)_1-x(en)_x(Pb)_1-0.7x(Br)_3-0.4x (FA = formamidinium (FA⁺), en = ethylenediammonium (en²⁺), x = 0-0.44). Pair distribution function analysis shed light on the local structural coherence, revealing a wide distribution of Pb-Pb distances in the crystal structure as a consequence of the Pb/Br-deficient nature and en inclusion in the lattice. By manipulating the number of Pb/Br vacancies, we finely tune the optical properties of the pristine FAPbBr₃ by blue shifting the band gap from 2.20 to 2.60 eV for the x = 0.42 en sample. A most unexpected outcome was that at x > 0.33 en incorporation, the material exhibits strong broad light emission (1% photoluminescence quantum yield (PLQY)) that is maintained after exposure to air for more than a year. This is the first example of strong broad light emission from a 3D hybrid halide perovskite, demonstrating that meticulous defect engineering is an excellent tool for customizing the optical properties of these semiconductors.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: European Union; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0012541

OSTI ID:: 1864311

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 18 Vol. 143; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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