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Published May 3, 2024 | Version v1
Journal article Open

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

Creators

  • 1. Arizona State University
  • 2. University of California, Berkeley
  • 3. University of Chicago
  • 4. Brookhaven National Laboratory
  • 5. SLAC National Accelerator Laboratory

Description

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 situ 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.

Files

PhysRevResearch.6.023119.pdf

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Additional details

Identifiers

DOI
10.1103/PhysRevResearch.6.023119
Other
oai:uchicago.tind.io:11763

Funding

U.S. Department of Energy
DE-SC0019375
U.S. Department of Energy
DE-AC02-76SF00515
U.S. Department of Energy
DE-SC0012704
National Science Foundation
DGE1106400
Arnold O. Beckman Postdoctoral Fellowship in Chemical Sciences
Arnold O. Beckman Postdoctoral Fellowship in Chemical Sciences
National Defense
Science and Engineering Graduate Fellowship
University of California, Berkeley
Philomathia Graduate Student Fellowship
David and Lucile Packard Foundation
Fellowship for Science and Engineering
Camille and Henry Dreyfus Foundation
Teacher-Scholar Award

UChicago Information

Division(s)
Physical Sciences Division, Pritzker School of Molecular Engineering
Department(s)
Chemistry
Center(s) or Institute(s)
James Franck Institute