Dynamic Nanocrystal Superlattices with Thermally Triggerable Lubricating Ligands

Ning, Yifan; Yang, Shengsong; Yang, Dai-Bei; Cai, Yi-Yu; Xu, Jun; Li, Ruipeng; Zhang, Yugang; Kagan, Cherie R.; Saven, Jeffery G.; Murray, Christopher B.

doi:10.1021/jacs.3c10706

Title: Dynamic Nanocrystal Superlattices with Thermally Triggerable Lubricating Ligands

Journal Article · 31 January 2024 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.3c10706 · OSTI ID:2372683

^[1];

^[1]; Yang, Dai-Bei ^[1]; Cai, Yi-Yu ^[1]; Xu, Jun ^[1]; Li, Ruipeng ^[2];

^[3];

^[1];

^[1]; Murray, Christopher B. ^[1]

Univ. of Pennsylvania, Philadelphia, PA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

The size-dependent and collective physical properties of nanocrystals (NCs) and their self-assembled superlattices (SLs) enable the study of mesoscale phenomena and the design of metamaterials for a broad range of applications. However, the limited mobility of NC building blocks in dried NCSLs often hampers the potential for employing postdeposition methods to produce high-quality NCSLs. In this study, we present tailored promesogenic ligands that exhibit a lubricating property akin to thermotropic liquid crystals. The lubricating ability of ligands is thermally triggerable, allowing the dry solid NC aggregates deposited on the substrates with poor ordering to be transformed into NCSLs with high crystallinity and preferred orientations. The interplay between the dynamic behavior of NCSLs and the molecular structure of the ligands is elucidated through a comprehensive analysis of their lubricating efficacy using both experimental and simulation approaches. Coarse-grained molecular dynamic modeling suggests that a shielding layer from mesogens prevents the interdigitation of ligand tails, facilitating the sliding between outer shells and consequently enhancing the mobility of NC building blocks. Further, the dynamic organization of NCSLs can also be triggered with high spatial resolution by laser illumination. The principles, kinetics, and utility of lubricating ligands could be generalized to unlock stimuli-responsive metamaterials from NCSLs and contribute to the fabrication of NCSLs.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704; SC0019282

OSTI ID:: 2372683

Report Number(s):: BNL--225688-2024-JAAM

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 6 Vol. 146; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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