Mechanistic Exploration of Dodecanethiol-Treated Colloidal CsPbBr3 Nanocrystals with Photoluminescence Quantum Yields Reaching Near 100%

Md Aslam Uddin, Justin K. Mobley, Abdullah A. Masud, Tuo Liu, Rosemary L. Calabro, Doo Young Kim, Christopher I. Richards, Kenneth R. Graham

Research output: Contribution to journalArticlepeer-review

57 Scopus citations

Abstract

Metal halide perovskite nanocrystals (NCs) are attractive materials for optoelectronics. However, further improvements in stability, reproducibility, and photoluminescence quantum yield (φPL) are essential for enabling future applications. Inadequate surface passivation is a major cause of instability, irreproducibility, and less than unity φPL. Herein, we probe the influence of multiple ligand binding groups on the colloidal stability and φPL of CsPbBr3 nanocrystals (NCs). We find that post-synthetic treatment with dodecanethiol reproducibly yields highly stable NCs with near-unity φPL for a range of synthetic conditions and initial φPL of the as-synthesized NCs. A mechanistic investigation shows that thiol addition leads to thioether formation via the thiol-ene reaction with octadecene, oleic acid, and oleylamine. Both thiolates and thioethers are suspected to bind to undercoordinated Pb atoms on the NC surfaces, and this surface binding can be rapidly accelerated through exposure to blue or UV light. Furthermore, we show that metallic Pb nanoparticles appear in many batches of synthesized CsPbBr3 NCs and that dodecanethiol addition eliminates these metallic Pb particles.

Original languageEnglish
Pages (from-to)18103-18112
Number of pages10
JournalJournal of Physical Chemistry C
Volume123
Issue number29
DOIs
StatePublished - Jul 25 2019

Bibliographical note

Publisher Copyright:
© 2019 American Chemical Society.

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • General Energy
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Fingerprint

Dive into the research topics of 'Mechanistic Exploration of Dodecanethiol-Treated Colloidal CsPbBr3 Nanocrystals with Photoluminescence Quantum Yields Reaching Near 100%'. Together they form a unique fingerprint.

Cite this