Elucidating the Role of Antisolvents on the Surface Chemistry and Optoelectronic Properties of CsPbBrxI3-x Perovskite Nanocrystals

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review

1 Scopus Citations
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Author(s)

  • Junzhi Ye
  • Zhenchao Li
  • Dominik J. Kubicki
  • Yunwei Zhang
  • Linjie Dai
  • Clara Otero-Martínez
  • Manuel A. Reus
  • Rakesh Arul
  • Kavya Reddy Dudipala
  • Zahra Andaji-Garmaroudi
  • Yi-Teng Huang
  • Zewei Li
  • Ziming Chen
  • Peter Müller-Buschbaum
  • Samuel D. Stranks
  • Clare P. Grey
  • Jeremy J. Baumberg
  • Neil C. Greenham
  • Lakshminarayana Polavarapu
  • Akshay Rao
  • Robert L. Z. Hoye

Detail(s)

Original languageEnglish
Pages (from-to)12102-12115
Journal / PublicationJournal of the American Chemical Society
Volume144
Issue number27
Online published27 Jun 2022
Publication statusPublished - 13 Jul 2022

Link(s)

Abstract

Colloidal lead-halide perovskite nanocrystals (LHP NCs) have emerged over the past decade as leading candidates for efficient next-generation optoelectronic devices, but their properties and performance critically depend on how they are purified. While antisolvents are widely used for purification, a detailed understanding of how the polarity of the antisolvent influences the surface chemistry and composition of the NCs is missing in the field. Here, we fill this knowledge gap by studying the surface chemistry of purified CsPbBrxI3-x NCs as the model system, which in itself is considered a promising candidate for pure-red light-emitting diodes and top-cells for tandem photovoltaics. Interestingly, we find that as the polarity of the antisolvent increases (from methyl acetate to acetone to butanol), there is a blueshift in the photoluminescence (PL) peak of the NCs along with a decrease in PL quantum yield (PLQY). Through transmission electron microscopy and X-ray photoemission spectroscopy measurements, we find that these changes in PL properties arise from antisolvent-induced iodide removal, which leads to a change in halide composition and, thus, the bandgap. Using detailed nuclear magnetic resonance (NMR) and Fourier-transform infrared spectroscopy (FTIR) measurements along with density functional theory calculations, we propose that more polar antisolvents favor the detachment of the oleic acid and oleylamine ligands, which undergo amide condensation reactions, leading to the removal of iodide anions from the NC surface bound to these ligands. This work shows that careful selection of low-polarity antisolvents is a critical part of designing the synthesis of NCs to achieve high PLQYs with minimal defect-mediated phase segregation.

Research Area(s)

Citation Format(s)

Elucidating the Role of Antisolvents on the Surface Chemistry and Optoelectronic Properties of CsPbBrxI3-x Perovskite Nanocrystals. / Ye, Junzhi; Li, Zhenchao; Kubicki, Dominik J. et al.

In: Journal of the American Chemical Society, Vol. 144, No. 27, 13.07.2022, p. 12102-12115.

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review

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