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Title: Strongly Quantum Confined Colloidal Cesium Tin Iodide Perovskite Nanoplates: Lessons for Reducing Defect Density and Improving Stability

Journal Article · · Nano Letters
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [4];  [5];  [1]; ORCiD logo [1]; ORCiD logo [6];  [2]; ORCiD logo [7]; ORCiD logo [7]
  1. Univ. of California, Berkeley, CA (United States). Department of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  3. Univ. of California, Berkeley, CA (United States). Department of Chemistry
  4. Univ. of California, Berkeley, CA (United States). Department of Materials Science and Engineering
  5. Univ. of California, Berkeley, CA (United States). Department of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division and Chemical Sciences Division
  6. Univ. of California, Berkeley, CA (United States). Department of Chemistry and Department of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division and Chemical Sciences Division
  7. Univ. of California, Berkeley, CA (United States). Department of Chemistry and Department of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Kavli Energy NanoScience Institute, Berkeley, CA (United States)

We report that within the last several years, metal halide perovskites such as methylammonium lead iodide, CH3NH3PbI3, have come to the forefront of scientific investigation as defect-tolerant, solution-processable semiconductors that exhibit excellent optoelectronic properties. The vast majority of study has focused on Pb-based perovskites, which have limited applications because of their inherent toxicity. To enable the broad application of these materials, the properties of lead-free halide perovskites must be explored. Here, two-dimensional, lead-free cesium tin iodide, (CsSnI3), perovskite nanoplates have been synthesized and characterized for the first time. These CsSnI3 nanoplates exhibit thicknesses of less than 4 nm and exhibit significant quantum confinement with photoluminescence at 1.59 eV compared to 1.3 eV in the bulk. Ab initio calculations employing the generalized gradient approximation of Perdew-Burke-Ernzerhof elucidate that although the dominant intrinsic defects in CsSnI3 do not introduce deep levels inside the band gap, their concentration can be quite high. These simulations also highlight that synthesizing and processing CsSnI3 in Sn-rich conditions can reduce defect density and increase stability, which matches insights gained experimentally. Lastly, this improvement in the understanding of CsSnI3 represents a step toward the broader challenge of building a deeper understanding of Sn-based halide perovskites and developing design principles that will lead to their successful application in optoelectronic devices.

Research Organization:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1465707
Journal Information:
Nano Letters, Vol. 18, Issue 3; Related Information: © 2018 American Chemical Society.; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 96 works
Citation information provided by
Web of Science

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From Nonluminescent to Blue‐Emitting Cs 4 PbBr 6 Nanocrystals: Tailoring the Insulator Bandgap of 0D Perovskite through Sn Cation Doping journal May 2019
0D Cs 3 Cu 2 X 5 (X = I, Br, and Cl) Nanocrystals: Colloidal Syntheses and Optical Properties journal December 2019
Colloidal synthesis of lead-free all-inorganic cesium bismuth bromide perovskite nanoplatelets journal January 2018
Lead‐Free Metal Halide Perovskite Nanocrystals: Challenges, Applications, and Future Aspects journal January 2019
Rich Chemistry in Inorganic Halide Perovskite Nanostructures journal September 2018
Efficient CsSnI 3 -based inorganic perovskite solar cells based on a mesoscopic metal oxide framework via incorporating a donor element journal January 2020
Tin Halide Perovskites: Progress and Challenges journal April 2020
Building bridges between halide perovskite nanocrystals and thin-film solar cells journal January 2018
Lead-free hybrid perovskites for photovoltaics journal January 2018
Synthesis and optical properties of novel mixed‐metal cation CsPb 1− x Ti x Br 3 ‐based perovskite glasses for W‐LED journal August 2019
Lead‐Free Halide Perovskite Nanocrystals: Crystal Structures, Synthesis, Stabilities, and Optical Properties journal January 2020
Bleifreie Halogenid‐Perowskit‐Nanokristalle: Kristallstrukturen, Synthese, Stabilitäten und optische Eigenschaften journal December 2019
Recent advances toward practical use of halide perovskite nanocrystals journal January 2018
Halide Perovskite Nanocrystals for Next‐Generation Optoelectronics journal April 2019