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Article Dans Une Revue ACS Nano Année : 2021

Interstitial Nature of Mn 2+ Doping in 2D Perovskites

Qing Tu
Vladislav Klepov
Matthew Krzyaniak
Michael Wasielewski
Claudine Katan
Tod Grusenmeyer
Ruth Pachter
Mercouri Kanatzidis
Jean-Christophe Blancon
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Aditya Mohite

Résumé

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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Dates et versions

hal-03481423 , version 1 (22-02-2022)

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Paternité - Pas d'utilisation commerciale

Identifiants

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Andrew Torma, Wenbin Li, Hao Zhang, Qing Tu, Vladislav Klepov, et al.. Interstitial Nature of Mn 2+ Doping in 2D Perovskites. ACS Nano, 2021, 15 (12), pp.20550-20561. ⟨10.1021/acsnano.1c09142⟩. ⟨hal-03481423⟩
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