Atomic Alignment in PbS Nanocrystal Superlattices with Compact Inorganic Ligands via Reversible Oriented Attachment of Nanocrystals

Nanocrystals (NCs) serve as versatile building blocks for the creation of functional materials with NC self-assembly offering opportunities to enable novel material properties. Here, we demonstrate that PbS NCs functionalized with strongly negatively charged metal chalcogenide complex (MCC) ligands, such as Sn 2 S 6 4– and AsS 4 3–, can self-assemble into all-inorganic superlattices with both long-range superlattice translational and atomic-lattice orientational order. Structural characterizations reveal that the NCs adopt an unexpected edge-to-edge alignment, and numerical simulation clarifies that orientational order is thermodynamically stabilized by many-body ion correlations originating from the dense electrolyte. Furthermore, we show that the superlattices of Sn 2 S 6 4– -functionalized PbS NCs can be fully disassembled back into the colloidal state, which is highly unusual for orientationally attached superlattices with atomic-lattice alignment. The reversible oriented attachment of NCs, enabling their dynamic assembly and disassembly into effectively single-crystalline superstructures, offers a pathway toward designing reconfigurable materials with adaptive and controllable electronic and optoelectronic properties.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2026-06-16
DOI
https://doi.org/10.1021/jacs.6c00744
Primary Topic
Quantum Dots Synthesis And Properties
Type
article
Field-Weighted Citation Impact
0.00

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article

Atomic Alignment in PbS Nanocrystal Superlattices with Compact Inorganic Ligands via Reversible Oriented Attachment of Nanocrystals

Sadegh Yazdi, Zirui Zhou, Richard D. Schaller, Naomi S. Ginsberg et al.
Journal of the American Chemical Society
Quantum Dots Synthesis And Properties
article

Atomic Alignment in PbS Nanocrystal Superlattices with Compact Inorganic Ligands via Reversible Oriented Attachment of Nanocrystals

Sadegh Yazdi, Zirui Zhou, Richard D. Schaller, Naomi S. Ginsberg, Xiaoben Zhang, Vivian R. K. Wall, Dmitri V. Talapin, Saghar Rezaie, Aditya Singh, Ahhyun Jeong, Justin C. Ondry, Josh Portner, David T. Limmer, Junhong Chen, Zehan Mi, Ye Ji Kim, Youssef Tazoui
article en

Abstract

Nanocrystals (NCs) serve as versatile building blocks for the creation of functional materials with NC self-assembly offering opportunities to enable novel material properties. Here, we demonstrate that PbS NCs functionalized with strongly negatively charged metal chalcogenide complex (MCC) ligands, such as Sn 2 S 6 4– and AsS 4 3–, can self-assemble into all-inorganic superlattices with both long-range superlattice translational and atomic-lattice orientational order. Structural characterizations reveal that the NCs adopt an unexpected edge-to-edge alignment, and numerical simulation clarifies that orientational order is thermodynamically stabilized by many-body ion correlations originating from the dense electrolyte. Furthermore, we show that the superlattices of Sn 2 S 6 4– -functionalized PbS NCs can be fully disassembled back into the colloidal state, which is highly unusual for orientationally attached superlattices with atomic-lattice alignment. The reversible oriented attachment of NCs, enabling their dynamic assembly and disassembly into effectively single-crystalline superstructures, offers a pathway toward designing reconfigurable materials with adaptive and controllable electronic and optoelectronic properties.

Journal of the American Chemical Society
Argonne National Laboratory (US), Energy Institute (GB), Lawrence Berkeley National Laboratory (US), University of Colorado Boulder (US), University of Colorado System (US), University of Chicago (US), Directorate of Health (IS), MSSCORPS (Taiwan) (TW), Division of Materials Research (US), Kavli Energy NanoScience Institute (US), NOAA Chemical Sciences Laboratory (US), Center for Nanoscale Materials, University of California, Berkeley (US)
National Science Foundation, University of Chicago, Kwanjeong Educational Foundation, Basic Energy Sciences, Air Force Office of Scientific Research, National Science Foundation Graduate Research Fellowship Program
Openalex Percentile: Top 14%
Quantum Dots Synthesis And Properties
DOISourceOpenAlex
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