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Title: Shape Dependence of Pressure-Induced Phase Transition in CdS Semiconductor Nanocrystals

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.0c01906· OSTI ID:1722885
 [1]; ORCiD logo [2];  [1];  [1];  [2];  [2];  [2];  [3];  [2];  [4];  [4];  [4];  [5]; ORCiD logo [1]; ORCiD logo [6]
  1. Department of Chemistry and Chemical Biology, University of New Mexico, Albuquerque, New Mexico 87131, United States
  2. Sandia National Laboratories, Albuquerque, New Mexico 87123, United States
  3. Nevada National Security Site, New Mexico Operations-Sandia, Albuquerque, New Mexico 87123, United States
  4. HPCAT, X-ray Science Division, Argonne National Laboratories, Lemont, Illinois 60439, United States
  5. National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, New York 11973, United States
  6. Sandia National Laboratories, Albuquerque, New Mexico 87123, United States;Department of Chemical and Biological Engineering, University of New Mexico, Albuquerque, New Mexico 87131, United States;Center for Integrated Nanotechnology, Sandia National Laboratories, Albuquerque, New Mexico 87123, United States

Understanding structural stability and phase transformation of nanoparticles under high pressure is of great scientific interest, as it is one of the crucial factors for design, synthesis, and application of materials. Even though high-pressure research on nanomaterials has been widely conducted, their shape-dependent phase transition behavior still remains unclear. Examples of phase transitions of CdS nanoparticles are very limited, despite the fact that it is one of the most studied wide band gap semiconductors. Here we have employed in-situ synchrotron wide-angle X-ray scattering (WAXS) and transmission electron microscopy (TEM) to investigate the high-pressure behaviors of CdS nanoparticles as a function of particle shapes. We observed that CdS nanoparticles transform from wurtzite to rocksalt phase at elevated pressure in comparison to their bulk counterpart. Phase transitions also vary with particle shape—rod-shaped particles show a partially reversible phase transition and the onset of the structural phase transition pressure decreases with decreasing surface-to-volume ratios, while spherical particles undergo irreversible phase transition with relatively low phase transition pressure. Additionally, TEM images of spherical particles exhibited sintering-induced morphology change after high-pressure compression. Calculations of the bulk modulus reveals that spheres are more compressible than rods in the wurtzite phase. These results indicate that the shape of the particle plays an important role in determining their high-pressure properties. Our study provides important insights into understanding of the phase-structure-property relationship, guiding future design and synthesis of nanoparticles for promising applications.

Research Organization:
Nevada National Security Site/Mission Support and Test Services LLC (NNSS/MSTS), North Las Vegas, NV (United States); Las Vegas, NV (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Programs (DP)
DOE Contract Number:
CHE-1904659; P20GM103451; DENA0003624
OSTI ID:
1722885
Report Number(s):
DOE/NV/03624-0711; STIP WF - 19404929
Journal Information:
Journal of the American Chemical Society, Vol. 142, Issue 14; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English