Extraordinary Interfacial Stitching between Single All-Inorganic Perovskite Nanocrystals

Leyre Gomez*, Junhao Lin, Chris De Weerd, Lucas Poirier, Simon C. Boehme, Elizabeth Von Hauff, Yasufumi Fujiwara, Kazutomo Suenaga, Tom Gregorkiewicz

*Corresponding author for this work

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

All-inorganic cesium lead halide perovskite nanocrystals are extensively studied because of their outstanding optoelectronic properties. Being of a cubic shape and typically featuring a narrow size distribution, CsPbX3 (X = Cl, Br, and I) nanocrystals are the ideal starting material for the development of homogeneous thin films as required for photovoltaic and optoelectronic applications. Recent experiments reveal spontaneous merging of drop-casted CsPbBr3 nanocrystals, which is promoted by humidity and mild-temperature treatments and arrested by electron beam irradiation. Here, we make use of atom-resolved annular dark-field imaging microscopy and valence electron energy loss spectroscopy in a state-of-the-art low-voltage monochromatic scanning transmission electron microscope to investigate the aggregation between individual nanocrystals at the atomic level. We show that the merging process preserves the elemental composition and electronic structure of CsPbBr3 and takes place between nanocrystals of different sizes and orientations. In particular, we reveal seamless stitching for aligned nanocrystals, similar to that reported in the past for graphene flakes. Because the crystallographic alignment occurs naturally in drop-casted layers of CsPbX3 nanocrystals, our findings constitute the essential first step toward the development of large-area nanosheets with band gap energies predesigned by the nanocrystal choice - the gateway to large-scale photovoltaic applications of inorganic perovskites.

Original languageEnglish
Pages (from-to)5984-5991
Number of pages8
JournalACS Applied Materials and Interfaces
Volume10
Issue number6
DOIs
Publication statusPublished - 14 Feb 2018

Funding

C.d.W., L.G., and T.G. acknowledge the Dutch Technology Foundation STW, which is part of the Netherlands Organisation for Scientific Research (NWO) for financial support. J.L. and K.S. work has been financed by JST-ACCEL and JSPS KAKENHI (JP16H06333 and P16823). E.v.H. thanks the Foundation for Fundamental Research on Matter (FOM) (V0714M-13MV60) from the Netherlands Organization for Scientific Research (NWO) for funding. Y.F. and T.G. thank Osaka University for International Joint Research Promotion Program.

FundersFunder number
JST-ACCEL
Japan Society for the Promotion of ScienceJP16H06333, P16823
Stichting voor Fundamenteel Onderzoek der MaterieV0714M-13MV60
Nederlandse Organisatie voor Wetenschappelijk Onderzoek
Stichting voor de Technische Wetenschappen
Osaka University

    Keywords

    • EELS
    • high-resolution TEM
    • inorganic perovskites
    • merging
    • nanocrystals
    • seamless stitching

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