Study of the Mechanism and Increasing Crystallinity in the Self-Templated Growth of Ultrathin PbS Nanosheets

Maaike M. van der Sluijs, Bastiaan B.V. Salzmann, Daniel Arenas Esteban, Chen Li, Daen Jannis, Laura C. Brafine, Tim D. Laning, Joost W.C. Reinders, Natalie S.A. Hijmans, Jesper R. Moes, Johan Verbeeck, Sara Bals, Daniel Vanmaekelbergh*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

Abstract

Colloidal 2D semiconductor nanocrystals, the analogue of solid-state quantum wells, have attracted strong interest in material science and physics. Molar quantities of suspended quantum objects with spectrally pure absorption and emission can be synthesized. For the visible region, CdSe nanoplatelets with atomically precise thickness and tailorable emission have been (almost) perfected. For the near-infrared region, PbS nanosheets (NSs) hold strong promise, but the photoluminescence quantum yield is low and many questions on the crystallinity, atomic structure, intriguing rectangular shape, and formation mechanism remain to be answered. Here, we report on a detailed investigation of the PbS NSs prepared with a lead thiocyanate single source precursor. Atomically resolved HAADF-STEM imaging reveals the presence of defects and small cubic domains in the deformed orthorhombic PbS crystal lattice. Moreover, variations in thickness are observed in the NSs, but only in steps of 2 PbS monolayers. To study the reaction mechanism, a synthesis at a lower temperature allowed for the study of reaction intermediates. Specifically, we studied the evolution of pseudo-crystalline templates toward mature, crystalline PbS NSs. We propose a self-induced templating mechanism based on an oleylamine-lead-thiocyanate (OLAM-Pb-SCN) complex with two Pb-SCN units as a building block; the interactions between the long-chain ligands regulate the crystal structure and possibly the lateral dimensions.

Original languageEnglish
Pages (from-to)2988-2998
Number of pages11
JournalChemistry of Materials
Volume35
Issue number7
DOIs
Publication statusPublished - 11 Apr 2023

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