Journal
CHEMISTRY OF MATERIALS
Volume 30, Issue 18, Pages 6400-6409Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.8b02657
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Funding
- start-up grant of Syracuse University
- NSF MRSEC program [DMR-1719875]
- National Institutes of Health Grant [NIH/NIBIB R010EB00315]
- National Science Foundation [DMR-1708617]
- DOE Office of Science [DE-AC02-06CH11357]
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The introduction of dopants plays a key role in the physical properties of semiconductors for optoelectronic applications. However, doping is generally challenging for nanocrystals (NCs), especially for two-dimensional (2D) NCs, due to the self-annealing effect and high surface energies required for dopant addition. Here, we report an efficient doping strategy for Mn-doped 2D CsPbCl3 (i.e., Mn:CsPbCl3) nanoplatelets (NPLs) through a postsynthetic solvothermal process. While the original lightly doped 2D Mn:CsPbCl3 NPLs were obtained from growth doping, higher Mn doping efficiencies were achieved through diffusion doping under pressure-mediated solvothermal conditions, resulting in enhanced Mn photoluminescence (PL). Surprisingly, a new CsMnCl3 phase with complete dopant substitution by spinodal decomposition was observed with extended solvothermal treatment, which is confirmed by powder X-ray diffraction, X-ray absorption fine structure, and electron paramagnetic resonance. Compared with Mn:CsPbCl3 NPLs, the pure CsMnCl3 NPLs give rise to shorter Mn PL lifetime, which is consistent with the short Mn-Mn distance within CsMnCl3 NPLs. This work provides an efficient strategy for doping inside NCs as well as new insights on the dopant concentration-dependent structural and optical properties of perovskite NCs.
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