Complete Dopant Substitution by Spinodal Decomposition in Mn-Doped Two-Dimensional CsPbCl3 Nanoplatelets

Li, Zhi-Jun; Hofman, Elan; Davis, Andrew Hunter; Khammang, Alex; Wright, Joshua T.; Dzikovski, Boris; Meulenberg, Robert W.; Zheng, Weiwei

doi:10.1021/acs.chemmater.8b02657

Complete Dopant Substitution by Spinodal Decomposition in Mn-Doped Two-Dimensional CsPbCl₃ Nanoplatelets

Journal Article · Thu Aug 23 00:00:00 EDT 2018 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.8b02657· OSTI ID:1484785

Li, Zhi-Jun ^[1]; Hofman, Elan ^[1]; Davis, Andrew Hunter ^[1]; Khammang, Alex ^[2]; Wright, Joshua T. ^[3]; Dzikovski, Boris ^[4]; Meulenberg, Robert W. ^[2]; ^[1]

Syracuse Univ., NY (United States)
Univ. of Maine, Orono, ME (United States)
Illinois Inst. of Technology, Chicago, IL (United States)
National Biomedical Center for Advanced Electron Spin Resonance Technology, Ithaca, NY (United States)

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. In this paper, 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Science Foundation (NSF); National Institutes of Health (NIH); USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1484785

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 18 Vol. 30; ISSN 0897-4756

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
Doping
Impurities
Ions
Solvothermal reaction
Transition metals