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Overlapped embedded fragment stochastic density functional theory for covalently-bonded materials

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.5064472· OSTI ID:1492332
 [1];  [2];  [3];  [4]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. The Hebrew Univ. of Jerusalem, Jerusalem (Israel)
  3. Univ. of California, Los Angeles, CA (United States)
  4. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Tel Aviv Univ., Tel Aviv (Israel)
+ Show Author Affiliations
The stochastic density functional theory (DFT) is a valuable linear-scaling approach to Kohn-Sham DFT that does not rely on the sparsity of the density matrix. Linear (and often sub-linear) scaling is achieved by introducing a controlled statistical error in the density, energy, and forces. The statistical error (noise) is proportional to the inverse square root of the number of stochastic orbitals and thus decreases slowly; however, by dividing the system into fragments that are embedded stochastically, the statistical error can be reduced significantly. This has been shown to provide remarkable results for non-covalently-bonded systems; however, the application to covalently bonded systems had limited success, particularly for delocalized electrons. Here, we show that the statistical error in the density correlates with both the density and the density matrix of the system and propose a new fragmentation scheme that elegantly interpolates between overlapped fragments. In conclusion, we assess the performance of the approach for bulk silicon of varying supercell sizes (up to Ne = 16 384 electrons) and show that overlapped fragments reduce significantly the statistical noise even for systems with a delocalized density matrix.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1492332
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 3 Vol. 150; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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Stochastic embedding DFT: Theory and application to p -nitroaniline in water journal November 2019
Energy window stochastic density functional theory journal September 2019

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