4.8 Article

Anisotropic Transient Disordering of Colloidal, Two-Dimensional CdSe Nanoplatelets upon Optical Excitation

Journal

NANO LETTERS
Volume 21, Issue 3, Pages 1288-1294

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.0c03958

Keywords

Nanoplatelets; nonequilibrium phenomena; transient heating; X-ray diffraction; anisotropic disordering

Funding

  1. National Science Foundation [1629383, 1808590]
  2. National Science Foundation Graduate Research Fellowship Program [DGE1842165]
  3. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DEFG02-99ER14999, DE-AC02-06CH11357]
  4. 3M Graduate Research Fellowship
  5. Ryan Fellowship
  6. Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facilities [DE-AC02-06CH11357]
  7. Ultrafast Initiative of the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, through Argonne National Laboratory [DEAC02-06CH11357]
  8. Northwestern University
  9. E.I. DuPont de Nemours Co.
  10. Dow Chemical Company
  11. Division Of Chemistry
  12. Direct For Mathematical & Physical Scien [1808590] Funding Source: National Science Foundation
  13. Division Of Materials Research
  14. Direct For Mathematical & Physical Scien [1629383] Funding Source: National Science Foundation

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Time-resolved X-ray diffraction study reveals that photoexcitation induces greater out-of-plane disordering in 4 and 5 monolayer NPLs, while 3 ML NPLs display the opposite behavior. In comparison, disordering in zero-dimensional CdSe nanocrystals is isotropic and recovery is faster. These findings support the superior performance of NPLs in optoelectronic applications.
Nanoplatelets (NPLs)-colloidally synthesized, spatially anisotropic, two-dimensional semiconductor quantum wells-are of intense interest owing to exceptionally narrow transition line widths, coupled with solution processability and bandgap tunability. However, given large surface areas and undercoordinated bonding at facet corners and edges, excitation under sufficient intensities may induce anisotropic structural instabilities that impact desired properties. We employ time-resolved X-ray diffraction to study the crystal structure of CdSe NPLs in response to optical excitation. Photoexcitation induces greater out-of-plane than in-plane disordering in 4 and 5 monolayer (ML) NPLs, while 3 ML NPLs display the opposite behavior. Recovery dynamics suggest that out-of-plane cooling slightly outpaces in-plane cooling in 5 ML NPLs with recrystallization occurring on indistinguishable time scales. In comparison, for zero-dimensional CdSe nanocrystals, disordering is isotropic and recovery is faster. These results favor the use of NPLs in optoelectronic applications, where they are likely to exhibit superior performance over traditional, zero-dimensional nanocrystals.

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