Pseudodiagonalization Method for Accelerating Nonlinear Subspace Diagonalization in Density Functional Theory

Shah, Shikhar; Suryanarayana, Phanish; Chow, Edmond

doi:10.1021/acs.jctc.2c00166

Pseudodiagonalization Method for Accelerating Nonlinear Subspace Diagonalization in Density Functional Theory

Journal Article · Tue May 24 00:00:00 EDT 2022 · Journal of Chemical Theory and Computation

DOI:https://doi.org/10.1021/acs.jctc.2c00166· OSTI ID:1988390

^[1]; Suryanarayana, Phanish ^[2]; ^[2]

Georgia Institute of Technology, Atlanta, GA (United States); Georgia Institute of Technology
Georgia Institute of Technology, Atlanta, GA (United States)

In density functional theory, each self-consistent field (SCF) nonlinear step updates the discretized Kohn-Sham orbitals by solving a linear eigenvalue problem. The concept of pseudodiagonalization is to solve this linear eigenvalue problem approximately, and specifically utilizing a method involving a small number of Jacobi rotations that takes advantage of the good initial guess to the solution given by the approximation to the orbitals from the previous SCF iteration. The approximate solution to the linear eigenvalue problem can be very rapid, particularly for those steps near SCF convergence. Here, we adapt pseudodiagonalization to finite-temperature and metallic systems, where partially-occupied orbitals must be individually resolved with some accuracy. We apply pseudodiagonalization to the subspace eigenvalue problem that arises in Chebyshev-filtered subspace iteration. In tests on metallic and other systems for a range of temperatures, we show that pseudodiagonalization achieves similar rates of SCF convergence to exact diagonalization.

View Accepted Manuscript (DOE)

Research Organization:: Georgia Institute of Technology, Atlanta, GA (United States). Georgia Tech Research Institute

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019410

OSTI ID:: 1988390

Alternate ID(s):: OSTI ID: 1977928

Journal Information:: Journal of Chemical Theory and Computation, Journal Name: Journal of Chemical Theory and Computation Journal Issue: 6 Vol. 18; ISSN 1549-9618

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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