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Pressure Induced Assembly and Coalescence of Lead Chalcogenide Nanocrystals

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.0c13350· OSTI ID:1774185
 [1];  [2];  [2];  [2];  [2];  [2];  [3];  [3];  [3];  [4];  [5]
  1. Univ. of New Mexico, Albuquerque, NM (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States)
  5. Univ. of New Mexico, Albuquerque, NM (United States); Univ. of Connecticut, Storrs, CT (United States)
We report here pressure induced nanocrystal coalescence of ordered lead chalcogenide nanocrystal arrays into one dimensional (1D) and 2D nanostructures. In particular, atomic crystal phase transitions and mesoscale coalescence of PbS and PbSe nanocrystals have been observed and monitored in-situ respectively by wide- and small-angle synchrotron X-ray scattering techniques. At the atomic scale, both nanocrystals underwent reversible structural transformations from cubic to orthorhombic at significantly higher pressures than those for the corresponding bulk materials. At the mesoscale, PbS nanocrystal arrays displayed a superlattice transformation from face-centered cubic to lamellar structures, while no clear mesoscale lattice transformation was observed for PbSe nanocrystal arrays. Intriguingly, transmission electron microscopy (TEM) showed that the applied pressure forced both spherical nanocrystals to coalesce into single crystalline 2D nanosheets and 1D nanorods. Our results confirm that pressure can be used as a straightforward approach to manipulate the interparticle spacing and engineer nanostructures with specific morphologies, and therefore provide insights into the design and functioning of new semiconductor nanocrystal structures under high-pressure conditions.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1774185
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 7 Vol. 143; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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