A spectral scheme for Kohn-Sham density functional theory of clusters. Starting from the observation that one of the most successful methods for solving the Kohn-Sham equations for periodic systems - the plane-wave method - is a spectral method based on eigenfunction expansion, we formulate a spectral method designed towards solving the Kohn-Sham equations for clusters. This allows for efficient calculation of the electronic structure of clusters (and molecules) with high accuracy and systematic convergence properties without the need for any artificial periodicity. The basis functions in this method form a complete orthonormal set and are expressible in terms of spherical harmonics and spherical Bessel functions. Computation of the occupied eigenstates of the discretized Kohn-Sham Hamiltonian is carried out using a combination of preconditioned block eigensolvers and Chebyshev polynomial filter accelerated subspace iterations. Several algorithmic and computational aspects of the method, including computation of the electrostatics terms and parallelization are discussed. We have implemented these methods and algorithms into an efficient and reliable package called ClusterES (Cluster Electronic Structure). A variety of benchmark calculations employing local and non-local pseudopotentials are carried out using our package and the results are compared to the literature. Convergence properties of the basis set are discussed through numerical examples. Computations involving large systems that contain thousands of electrons are demonstrated to highlight the efficacy of our methodology. The use of our method to study clusters with arbitrary point group symmetries is briefly discussed.

References in zbMATH (referenced in 10 articles , 1 standard article )

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  1. Yu, Hsuan Ming; Banerjee, Amartya S.: Density functional theory method for twisted geometries with application to torsional deformations in group-IV nanotubes (2022)
  2. Temizer, İ.: Radial and three-dimensional nonlocal pseudopotential calculations in gradient-corrected Kohn-Sham density functional theory based on higher-order finite element methods (2021)
  3. Xu, Nan; Doerschuk, Peter: Computation of real-valued basis functions which transform as irreducible representations of the polyhedral groups (2021)
  4. Temizer, İ.; Motamarri, P.; Gavini, V.: NURBS-based non-periodic finite element framework for Kohn-Sham density functional theory calculations (2020)
  5. Feng, Fan; Plucinsky, Paul; James, Richard D.: Phase transformations and compatibility in helical structures (2019)
  6. Bodroski, Zarko; Vukmirović, Nenad; Skrbic, Srdjan: Gaussian basis implementation of the charge patching method (2018)
  7. Pérez-Jordá, José M.: Fast solution of Schrödinger’s equation using linear combinations of plane waves (2017)
  8. Banerjee, Amartya S.; Suryanarayana, Phanish: Cyclic density functional theory: a route to the first principles simulation of bending in nanostructures (2016)
  9. Teng, Zhongming; Zhou, Yunkai; Li, Ren-Cang: A block Chebyshev-Davidson method for linear response eigenvalue problems (2016)
  10. Banerjee, Amartya S.; Elliott, Ryan S.; James, Richard D.: A spectral scheme for Kohn-Sham density functional theory of clusters (2015)