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Interstitial Nature of Mn2+ Doping in 2D Perovskites
- Source :
- ACS Nano, ACS Nano, American Chemical Society, 2021, ⟨10.1021/acsnano.1c09142⟩, ACS Nano, 2021, 15 (12), pp.20550-20561. ⟨10.1021/acsnano.1c09142⟩
- Publication Year :
- 2021
- Publisher :
- American Chemical Society (ACS), 2021.
-
Abstract
- International audience; 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.
- Subjects :
- [PHYS]Physics [physics]
crystal structure
strain mapping
General Engineering
General Physics and Astronomy
doping
02 engineering and technology
010402 general chemistry
021001 nanoscience & nanotechnology
nano X-ray diffraction
01 natural sciences
transition metals
0104 chemical sciences
Condensed Matter::Materials Science
halide perovskites
[CHIM]Chemical Sciences
Condensed Matter::Strongly Correlated Electrons
General Materials Science
0210 nano-technology
density functional theory
ComputingMilieux_MISCELLANEOUS
Subjects
Details
- ISSN :
- 1936086X and 19360851
- Volume :
- 15
- Database :
- OpenAIRE
- Journal :
- ACS Nano
- Accession number :
- edsair.doi.dedup.....7fb873d58a2dff0e456e2fd87919e500