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Title: Dielectric screening and vacancy formation for large neutral and charged Si n H m ( n > 1500 ) nanocrystals using real-space pseudopotentials

Abstract

A commonly used procedure for computing the properties of defects in crystalline materials is to consider a large supercell that includes the defect of interest. This is a straightforward technique as standard energy band codes can be used for such computations. For neutral defects, the only impediment of such an approach is to avoid defect-defect interactions between adjoining cells. However, this procedure can be complex if the defect of interest is charged as the system at large contains Coulombic divergences. Moreover, some have recently argued that the conventional definition of formation energies for charged defects cannot be reconciled with statistical mechanics. Here, we focus on an alternative approach. We consider large nanocrystals wherein a charged defect can be placed. Since the system is confined, a charged defect within the nanocrystal does not result in a Coulombic divergence. The chief impediment is computational, i.e., while no defect-defect or Coulombic divergences are present, the nanocrystal must be sufficiently large to allow the system to properly replicate a bulklike configuration. With the development of new algorithms and hardware advances, computations for systems of sufficient size to address this issue are feasible. In particular, we solve the Kohn-Sham equation in real space using pseudopotential-density-functionalmore » theory for large silicon nanocrystals, which contain thousands of atoms. Further, we focus on (i) the screening of a point charge and (ii) the formation of a charged vacancy in hydrogen-terminated silicon nanocrystals. This approach allows us to examine the role of quantum confinement in addition to exploring the bulk limit. Comparisons to other methods confirm the viability of this approach.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]
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  1. Univ. of Texas, Austin, TX (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Center for Computational Study of Excited State Phenomena in Energy Materials (C2SEPEM)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)
OSTI Identifier:
1982837
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 6; Journal Issue: 5; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Materials Science; Point defects

Citation Formats

Liao, Timothy, Liou, Kai-Hsin, and Chelikowsky, James R. Dielectric screening and vacancy formation for large neutral and charged SinHm (n>1500) nanocrystals using real-space pseudopotentials. United States: N. p., 2022. Web. doi:10.1103/physrevmaterials.6.054603.
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Liao, Timothy, Liou, Kai-Hsin, & Chelikowsky, James R. Dielectric screening and vacancy formation for large neutral and charged SinHm (n>1500) nanocrystals using real-space pseudopotentials. United States. https://doi.org/10.1103/physrevmaterials.6.054603
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Liao, Timothy, Liou, Kai-Hsin, and Chelikowsky, James R. Tue . "Dielectric screening and vacancy formation for large neutral and charged SinHm (n>1500) nanocrystals using real-space pseudopotentials". United States. https://doi.org/10.1103/physrevmaterials.6.054603. https://www.osti.gov/servlets/purl/1982837.
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@article{osti_1982837,
title = {Dielectric screening and vacancy formation for large neutral and charged SinHm (n>1500) nanocrystals using real-space pseudopotentials},
author = {Liao, Timothy and Liou, Kai-Hsin and Chelikowsky, James R.},
abstractNote = {A commonly used procedure for computing the properties of defects in crystalline materials is to consider a large supercell that includes the defect of interest. This is a straightforward technique as standard energy band codes can be used for such computations. For neutral defects, the only impediment of such an approach is to avoid defect-defect interactions between adjoining cells. However, this procedure can be complex if the defect of interest is charged as the system at large contains Coulombic divergences. Moreover, some have recently argued that the conventional definition of formation energies for charged defects cannot be reconciled with statistical mechanics. Here, we focus on an alternative approach. We consider large nanocrystals wherein a charged defect can be placed. Since the system is confined, a charged defect within the nanocrystal does not result in a Coulombic divergence. The chief impediment is computational, i.e., while no defect-defect or Coulombic divergences are present, the nanocrystal must be sufficiently large to allow the system to properly replicate a bulklike configuration. With the development of new algorithms and hardware advances, computations for systems of sufficient size to address this issue are feasible. In particular, we solve the Kohn-Sham equation in real space using pseudopotential-density-functional theory for large silicon nanocrystals, which contain thousands of atoms. Further, we focus on (i) the screening of a point charge and (ii) the formation of a charged vacancy in hydrogen-terminated silicon nanocrystals. This approach allows us to examine the role of quantum confinement in addition to exploring the bulk limit. Comparisons to other methods confirm the viability of this approach.},
doi = {10.1103/physrevmaterials.6.054603},
journal = {Physical Review Materials},
number = 5,
volume = 6,
place = {United States},
year = {Tue May 31 00:00:00 EDT 2022},
month = {Tue May 31 00:00:00 EDT 2022}
}
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