Ligand-induced incompatible curvatures control ultrathin nanoplatelet polymorphism and chirality

• 成果类型: Article
• 署名作者: Monego, Debora; Dutta, Sarit; Grossman, Doron; Krapez, Marion; Bauer, Pierre; Hubley, Austin; Mahler, Benoit; Widmer-Cooper, Asaph; Abecassis, Benjamin
• 署名单位: University of Sydney; University of Sydney; Ecole Normale Superieure de Lyon (ENS de LYON); Centre National de la Recherche Scientifique (CNRS); CNRS - Institute of Chemistry (INC); Institut Polytechnique de Paris; Ecole Polytechnique; Centre National de la Recherche Scientifique (CNRS); Centre National de la Recherche Scientifique (CNRS); Universite Claude Bernard Lyon 1
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-8658
• DOI: 10.1073/pnas.2316299121
• 发表日期: 2024-02-27
• 关键词: cdse nanoplatelets; platelets

摘要

The ability of thin materials to shape-shift is a common occurrence that leads to dynamic pattern formation and function in natural and man-made structures. However, harnessing this concept to rationally design inorganic structures at the nanoscale has remained far from reach due to a lack of fundamental understanding of the essential physical components. Here, we show that the interaction between organic ligands and the nanocrystal surface is responsible for the full range of chiral shapes seen in colloidal nanoplatelets. The adsorption of ligands results in incompatible curvatures on the top and bottom surfaces of the NPL, causing them to deform into helicoids, helical ribbons, or tubes depending on the lateral dimensions and crystallographic orientation of the NPL. We demonstrate that nanoplatelets belong to the broad class of geometrically frustrated assemblies and exhibit one of their hallmark features: a transition between helicoids and helical ribbons at a critical width. The effective curvature (kappa) over bar is the single aggregate parameter that encodes the details of the ligand/surface interaction, determining the nanoplatelets' geometry for a given width and crystallographic orientation. The conceptual framework described here will aid the rational design of dynamic, chiral nanostructures with high fundamental and practical relevance.