In situ coherent x-ray scattering reveals polycrystalline structure and discrete annealing events in strongly coupled nanocrystal superlattices

Hurley, Matthew J.; Tanner, Christian P. N.; Portner, Joshua; Utterback, James K.; Coropceanu, Igor; Das, Avishek; Slivka, Joseph D.; Fluerasu, Andrei; Sun, Yanwen; Song, Sanghoon; Hamerlynck, Leo M.; Miller, Alexander H.; Bhattacharyya, Priyadarshini; Talapin, Dmitri V.; Williams, Garth J.; Ginsberg, Naomi S.; Teitelbaum, Samuel W.

doi:10.1103/PhysRevResearch.6.023119

Title: In situ coherent x-ray scattering reveals polycrystalline structure and discrete annealing events in strongly coupled nanocrystal superlattices

Journal Article · 03 May 2024 · Physical Review Research

DOI: https://doi.org/10.1103/PhysRevResearch.6.023119 · OSTI ID:2345789

; Tanner, Christian P. N.; Portner, Joshua;

; Coropceanu, Igor;

; Slivka, Joseph D.; Fluerasu, Andrei; Sun, Yanwen;

; Hamerlynck, Leo M.; Miller, Alexander H.;

; Talapin, Dmitri V.;

;

Solution-phase bottom up self-assembly of nanocrystals into superstructures such as ordered superlattices is an attractive strategy to generate functional materials of increasing complexity, including very recent advances that incorporate strong interparticle electronic coupling. While the self-assembly kinetics in these systems have been elucidated and related to the product characteristics, the weak interparticle bonding interactions suggest the superstructures formed could continue to order within the solution long after the primary nucleation and growth have occurred, even though the mechanism of annealing remains to be elucidated. Here, we use a combination of Bragg coherent diffractive imaging and x-ray photon correlation spectroscopy to create real-space maps of supercrystalline order along with a real-time view of the strain fluctuations in aging strongly coupled nanocrystal superlattices while they remain suspended and immobilized in solution. By combining the results, we deduce that the self-assembled superstructures are polycrystalline, initially comprising multiple nucleation sites, and that shear avalanches at grain boundaries continue to increase crystallinity long after growth has substantially slowed. This multimodal approach should be generalizable to characterize a breadth of materials in their native chemical environments, thus extending the reach of high-resolution coherent x-ray characterization to the benefit of a much wider range of physical systems. Published by the American Physical Society 2024

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Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019375; AC02-76SF00515; SC0012704

OSTI ID:: 2345789

Journal Information:: Physical Review Research, Journal Name: Physical Review Research Journal Issue: 2 Vol. 6; ISSN PPRHAI; ISSN 2643-1564

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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