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Starting-point-independent quantum Monte Carlo calculations of iron oxide

Journal Article · · Physical Review. B
 [1];  [2];  [1];  [1];  [2];  [3];  [4];  [1]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  2. Univ. of California, Berkeley, CA (United States)
  3. Univ. of Washington, Seattle, WA (United States)
  4. Carnegie Inst. of Science, Washington, DC (United States)
+ Show Author Affiliations

Quantum Monte Carlo (QMC) methods are useful for studies of strongly correlated materials because they are many body in nature and use the physical Hamiltonian. Typical calculations assume as a starting point a wave function constructed from single-particle orbitals obtained from one-body methods, e.g., density functional theory. However, mean-field-derived wave functions can sometimes lead to systematic QMC biases if the mean-field result poorly describes the true ground state. In this study, we examine the accuracy and flexibility of QMC trial wave functions using variational and fixed-node diffusion QMC estimates of the total spin density and lattice distortion of antiferromagnetic iron oxide (FeO) in the ground state B1 crystal structure. We found that for relatively simple wave functions the predicted lattice distortion was controlled by the choice of single-particle orbitals used to construct the wave function, rather than by subsequent wave function optimization techniques within QMC. By optimizing the orbitals with QMC, we then demonstrate starting-point independence of the trial wave function with respect to the method by which the orbitals were constructed by demonstrating convergence of the energy, spin density, and predicted lattice distortion for two qualitatively different sets of orbitals. The results suggest that orbital optimization is a promising method for accurate many-body calculations of strongly correlated condensed phases.

Research Organization:
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF); European Research Council (ERC)
Grant/Contract Number:
AC04-94AL85000; NA0003525
OSTI ID:
1721602
Report Number(s):
SAND--2020-9953J; 690740
Journal Information:
Physical Review. B, Journal Name: Physical Review. B Journal Issue: 15 Vol. 102; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
antiferromagnetism
electronic structure
first-principles calculations
magnetoelastic effect