Temperature-Driven Transformation of CsPbBr 3 Nanoplatelets into Mosaic Nanotiles in Solution through Self-Assembly

Dang, Zhiya; Dhanabalan, Balaji; Castelli, Andrea; Dhall, Rohan; Bustillo, Karen C.; Marchelli, Dorwal; Spirito, Davide; Petralanda, Urko; Shamsi, Javad; Manna, Liberato; Krahne, Roman; Arciniegas, Milena P.

doi:10.1021/acs.nanolett.9b05036

Title: Temperature-Driven Transformation of CsPbBr ₃ Nanoplatelets into Mosaic Nanotiles in Solution through Self-Assembly

Journal Article · Tue Jan 28 00:00:00 EST 2020 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.9b05036· OSTI ID:1766592

; Dhanabalan, Balaji ^[1]; Castelli, Andrea; Dhall, Rohan ^[2]; Bustillo, Karen C. ^[2]; Marchelli, Dorwal; Spirito, Davide; Petralanda, Urko;

;

; Krahne, Roman;

Dipartimento di Chimica e Chimica Industriale, Università degli Studi di Genova, Via Dodecaneso, 31, 16146 Genova, Italy
National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Two-dimensional colloidal halide perovskite nanocrystals are promising materials for light-emitting applications. Recent studies have focused on nanoplatelets that are able to selfassemble and transform on solid substrates. However, the mechanism behind the process and the atomic arrangement of their assemblies remain unclear. Here, we present a detailed analysis of the transformation of self-assembled stacks of CsPbBr₃ nanoplatelets in solution over a period of a few months by using ex situ transmission electron microscopy and surface analysis. We demonstrate that the transformation mechanism can be understood as oriented attachment, proceeding through the following steps: (i) desorption of the ligands from the surfaces of the particles, causing the seamless atomic merging of nanoplatelet stacks into nanobelts; (ii) merging of neighboring nanobelts that form more extended nanoplates; and (iii) attachment of nanobelts and nanoplates, forming objects with an atomic structure that resembles a mosaic made of broken nanotiles. We reveal that aged nanobelts and nanoplates, which are mainly stabilized by amine/ammonium ions, link through a bilayer of CsBr, with the atomic columns of neighboring perovskite lattices shifted by a half-unit-cell, forming Ruddlesden-Popper planar faults. We also show, via in situ monitoring of the nanocrystal photoluminescence combined with transmission electron microscopy analysis, that the transformation is temperature driven and that it can take place within tens of minutes in solution and in spin-coated films. Understanding this process gives crucial information for the design and fabrication of perovskite materials, where control over the type and density of defects is desired, stimulating the development of perovskite nanocrystal structures with tailored electronic properties.

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Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1766592

Alternate ID(s):: OSTI ID: 1815738

Journal Information:: Nano Letters, Journal Name: Nano Letters Vol. 20 Journal Issue: 3; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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59 BASIC BIOLOGICAL SCIENCES
CsPbBr3
perovskite
nanoplatelets
self-assembly
transformations
temperature
transmission electron microscopy

Title: Temperature-Driven Transformation of CsPbBr 3 Nanoplatelets into Mosaic Nanotiles in Solution through Self-Assembly

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Title: Temperature-Driven Transformation of CsPbBr ₃ Nanoplatelets into Mosaic Nanotiles in Solution through Self-Assembly