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Title: Size-dependent lattice dynamics of atomically precise cadmium selenide quantum dots

Abstract

Material properties depend sensitively on the atomic arrangements and atomic bonding, but these are notoriously difficult to measure in nanosized atomic clusters due to the small size of the objects and the challenge of obtaining bulk samples of identical clusters. Here we have combined the recent ability to make gram quantities of identical semiconductor quantum-dot nanoparticles with the ability to measure lattice dynamics on small sample quantities of hydrogenated materials using high energy resolution inelastic x-ray scattering (HERIX), to measure the size-dependence of the phonon density of states (PDOS) in CdSe quantum dots. The fact that we have atomically precise structural models for these nanoparticles allows the calculation of the PDOS using Density Functional Theory (DFT), providing both experimental and theoretical confirmations of the important role that the inertia of the surface capping species plays on determining the lattice dynamics.

Authors:
 [1]; ORCiD logo [2];  [1];  [3];  [1];  [4];  [5];  [5]
  1. Columbia Univ., New York, NY (United States)
  2. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. American Physical Society, Ridge, NY (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States); Miami Univ., Oxford, OH (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1489740
Alternate Identifier(s):
OSTI ID: 1492134; OSTI ID: 1495704
Report Number(s):
BNL-210839-2019-JAAM
Journal ID: ISSN 0031-9007
Grant/Contract Number:  
SC0012704; AC02-06CH11357; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 122; Journal Issue: 2; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Shi, Chenyang, Billinge, Simon J. L., Beecher, Alexander N., Li, Yan, Owen, Jonathan S., Leu, Bogdan M., Said, Ayman H., and Hu, Michael Y. Size-dependent lattice dynamics of atomically precise cadmium selenide quantum dots. United States: N. p., 2019. Web. doi:10.1103/PhysRevLett.122.026101.
Shi, Chenyang, Billinge, Simon J. L., Beecher, Alexander N., Li, Yan, Owen, Jonathan S., Leu, Bogdan M., Said, Ayman H., & Hu, Michael Y. Size-dependent lattice dynamics of atomically precise cadmium selenide quantum dots. United States. doi:10.1103/PhysRevLett.122.026101.
Shi, Chenyang, Billinge, Simon J. L., Beecher, Alexander N., Li, Yan, Owen, Jonathan S., Leu, Bogdan M., Said, Ayman H., and Hu, Michael Y. Mon . "Size-dependent lattice dynamics of atomically precise cadmium selenide quantum dots". United States. doi:10.1103/PhysRevLett.122.026101.
@article{osti_1489740,
title = {Size-dependent lattice dynamics of atomically precise cadmium selenide quantum dots},
author = {Shi, Chenyang and Billinge, Simon J. L. and Beecher, Alexander N. and Li, Yan and Owen, Jonathan S. and Leu, Bogdan M. and Said, Ayman H. and Hu, Michael Y.},
abstractNote = {Material properties depend sensitively on the atomic arrangements and atomic bonding, but these are notoriously difficult to measure in nanosized atomic clusters due to the small size of the objects and the challenge of obtaining bulk samples of identical clusters. Here we have combined the recent ability to make gram quantities of identical semiconductor quantum-dot nanoparticles with the ability to measure lattice dynamics on small sample quantities of hydrogenated materials using high energy resolution inelastic x-ray scattering (HERIX), to measure the size-dependence of the phonon density of states (PDOS) in CdSe quantum dots. The fact that we have atomically precise structural models for these nanoparticles allows the calculation of the PDOS using Density Functional Theory (DFT), providing both experimental and theoretical confirmations of the important role that the inertia of the surface capping species plays on determining the lattice dynamics.},
doi = {10.1103/PhysRevLett.122.026101},
journal = {Physical Review Letters},
number = 2,
volume = 122,
place = {United States},
year = {2019},
month = {1}
}

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Works referenced in this record:

Rapid-acquisition pair distribution function (RA-PDF) analysis
journal, November 2003

  • Chupas, Peter J.; Qiu, Xiangyun; Hanson, Jonathan C.
  • Journal of Applied Crystallography, Vol. 36, Issue 6, p. 1342-1347
  • DOI: 10.1107/S0021889803017564

Projector augmented-wave method
journal, December 1994


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Quantum dot bioconjugates for imaging, labelling and sensing
journal, June 2005

  • Medintz, Igor L.; Uyeda, H. Tetsuo; Goldman, Ellen R.
  • Nature Materials, Vol. 4, Issue 6, p. 435-446
  • DOI: 10.1038/nmat1390

Two-dimensional detector software: From real detector to idealised image or two-theta scan
journal, January 1996

  • Hammersley, A. P.; Svensson, S. O.; Hanfland, M.
  • High Pressure Research, Vol. 14, Issue 4-6, p. 235-248
  • DOI: 10.1080/08957959608201408