The Surface Chemistry and Structure of Colloidal Lead Halide Perovskite Nanocrystals

Smock, Sara R.; Chen, Yunhua; Rossini, Aaron J.; Brutchey, Richard L.

doi:10.1021/acs.accounts.0c00741

The Surface Chemistry and Structure of Colloidal Lead Halide Perovskite Nanocrystals

Journal Article · Thu Jan 14 23:00:00 EST 2021 · Accounts of Chemical Research

DOI:https://doi.org/10.1021/acs.accounts.0c00741· OSTI ID:1765699

Smock, Sara R. ^[1]; Chen, Yunhua ^[2]; ^[2]; ^[1]

Univ. of Southern California, Los Angeles, CA (United States)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)

Since the initial discovery of colloidal lead halide perovskite nanocrystals, there has been significant interest placed on these semiconductors because of their remarkable optoelectronic properties, including very high photoluminescence quantum yields, narrow size- and composition-tunable emission over a wide color gamut, defect tolerance, and suppressed blinking. These material attributes have made them attractive components for next-generation solar cells, light emitting diodes, low-threshold lasers, single photon emitters, and X-ray scintillators. While a great deal of research has gone into the various applications of colloidal lead halide perovskite nanocrystals, comparatively little work has focused on the fundamental surface chemistry of these materials. While the surface chemistry of colloidal semiconductor nanocrystals is generally affected by their particle morphology, surface stoichiometry, and organic ligands that contribute to the first coordination sphere of their surface atoms, these attributes are markedly different in lead halide perovskite nanocrystals because of their ionicity. Herein, emerging work on the surface chemistry of lead halide perovskite nanocrystals is highlighted, with a particular focus placed on the most-studied composition of CsPbBr₃. We begin with an in-depth exploration of the native surface chemistry of as-prepared, 0-D cuboidal CsPbBr₃ nanocrystals, including an atomistic description of their surface termini, vacancies, and ionic bonding with ligands. We then proceed to discuss various post-synthetic surface treatments that have been developed to increase the photoluminescence quantum yields and stability of CsPbBr₃ nanocrystals, including the use of tetraalkylammonium bromides, metal bromides, zwitterions, and phosphonic acids, and how these various ligands are known to bind to the nanocrystal surface. To underscore the effect of post-synthetic surface treatments on the application of these materials, we focus on lead halide perovskite nanocrystal-based light emitting diodes, and the positive effect of various surface treatments on external quantum efficiencies. We also discuss the current state-of-the-art in the surface chemistry of 1-D nanowires and 2-D nanoplatelets of CsPbBr₃, which are more quantum confined than the corresponding cuboidal nanocrystals but also generally possess a higher defect density because of their increased surface area-to-volume ratios.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; Alfred P. Sloan Foundation

Grant/Contract Number:: SC0006812; SC0006812

OSTI ID:: 1765699

Report Number(s):: IS--J-10,410

Journal Information:: Accounts of Chemical Research, Journal Name: Accounts of Chemical Research Journal Issue: 3 Vol. 54; ISSN 0001-4842

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Crystals
Ligands
Nanocrystals
Nanoparticles
Perovskites

The Surface Chemistry and Structure of Colloidal Lead Halide Perovskite Nanocrystals

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