Interstitial Nature of Mn2+ Doping in 2D Perovskites

Torma, Andrew J.; Li, Wenbin; Zhang, Hao; Tu, Qing; Klepov, Vladislav V.; Brennan, Michael C.; McCleese, Christopher L.; Krzyaniak, Matthew D.; Wasielewski, Michael R.; Katan, Claudine; Even, Jacky; Holt, Martin V.; Grusenmeyer, Tod A.; Jiang, Jie; Pachter, Ruth; Kanatzidis, Mercouri G.; Blancon, Jean-Christophe; Mohite, Aditya D.

doi:10.1021/acsnano.1c09142

Title: Interstitial Nature of Mn²⁺ Doping in 2D Perovskites

Journal Article · Thu Dec 09 00:00:00 EST 2021 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.1c09142· OSTI ID:1883353

Torma, Andrew J. ^[1]; Li, Wenbin ^[1]; Zhang, Hao ^[1];

^[2];

^[3]; Brennan, Michael C. ^[4]; McCleese, Christopher L. ^[5];

^[3];

^[6];

^[6]; Holt, Martin V. ^[7];

^[4]; Jiang, Jie ^[4];

^[4];

^[3]; Blancon, Jean-Christophe ^[1];

^[1]

Rice Univ., Houston, TX (United States)
Texas A & M Univ., College Station, TX (United States)
Northwestern Univ., Evanston, IL (United States)
Air Force Research Lab. (AFRL), Wright-Patterson AFB, OH (United States)
Air Force Research Lab. (AFRL), Wright-Patterson AFB, OH (United States); General Dynamics Information Technology, Dayton, OH (United States)
Univ. of Rennes (France); Centre National de la Recherche Scientifique (CNRS) (France)
Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials

Halide perovskites doped with magnetic impurities (such as the transition metals Mn²⁺, Co²⁺, Ni²⁺) are being explored for a wide range of applications beyond photovoltaics, such as spintronic devices, stable light-emitting diodes, single-photon emitters, and magneto-optical devices. However, despite several recent studies, there is no consensus on whether the doped magnetic ions will predominantly replace the octahedral B-site metal via substitution or reside at interstitial defect sites. Here, by performing correlated nanoscale X-ray microscopy, spatially and temporally resolved photoluminescence measurements, and magnetic force microscopy on the inorganic 2D perovskite Cs₂PbI₂Cl₂, we show that doping Mn²⁺ into the structure results in a lattice expansion. The observed lattice expansion contrasts with the predicted contraction expected to arise from the B-site metal substitution, thus implying that Mn²⁺ does not replace the Pb²⁺ sites. Photoluminescence and electron paramagnetic resonance measurements confirm the presence of Mn²⁺ in the lattice, while correlated nano-XRD and X-ray fluorescence track the local strain and chemical composition. Density functional theory calculations predict that Mn²⁺ atoms reside at the interstitial sites between two octahedra in the triangle formed by one Cl^– and two I^– atoms, which results in a locally expanded structure. These measurements show the fate of the transition metal dopants, the local structure, and optical emission when they are doped at dilute concentrations into a wide band gap semiconductor.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Science Foundation (NSF); Institut Universitaire de France; US Army Research Office (ARO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); US Air Force Office of Scientific Research (AFOSR)

Grant/Contract Number:: AC02-06CH11357; NSF 20-587; SC0012541; FG02-99ER14999; FA8650-16-D-5402-0001

OSTI ID:: 1883353

Journal Information:: ACS Nano, Vol. 15, Issue 12; ISSN 1936-0851

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
density functional theory
strain mapping
crystal structure
doping
halide perovskites
nano X-ray diffraction
transition metals

Title: Interstitial Nature of Mn2+ Doping in 2D Perovskites

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Title: Interstitial Nature of Mn²⁺ Doping in 2D Perovskites