Extensions of the siesta dft code for simulation of molecules

We describe extensions to the siesta density functional theory (dft) code [30], for the simulation of isolated molecules and their absorption spectra. The extensions allow for: - Use of a multi-grid solver for the Poisson equation on a finite dft mesh. Non-periodic, Dirichlet boundary conditions are computed by expansion of the electric multipoles over spherical harmonics. - Truncation of a molecular system by the method of design atom pseudo- potentials of Xiao and Zhang[32]. - Electrostatic potential fitting to determine effective atomic charges. - Derivation of electronic absorption transition energies and oscillator stren- gths from the raw spectra produced by a recently described, order O(N3), time-dependent dft code[21]. The code is furthermore integrated within siesta as a post-processing option

ELSI: A Unified Software Interface for Kohn-Sham Electronic Structure Solvers

Solving the electronic structure from a generalized or standard eigenproblem is often the bottleneck in large scale calculations based on Kohn-Sham density-functional theory. This problem must be addressed by essentially all current electronic structure codes, based on similar matrix expressions, and by high-performance computation. We here present a unified software interface, ELSI, to access different strategies that address the Kohn-Sham eigenvalue problem. Currently supported algorithms include the dense generalized eigensolver library ELPA, the orbital minimization method implemented in libOMM, and the pole expansion and selected inversion (PEXSI) approach with lower computational complexity for semilocal density functionals. The ELSI interface aims to simplify the implementation and optimal use of the different strategies, by offering (a) a unified software framework designed for the electronic structure solvers in Kohn-Sham density-functional theory; (b) reasonable default parameters for a chosen solver; (c) automatic conversion between input and internal working matrix formats, and in the future (d) recommendation of the optimal solver depending on the specific problem. Comparative benchmarks are shown for system sizes up to 11,520 atoms (172,800 basis functions) on distributed memory supercomputing architectures.Comment: 55 pages, 14 figures, 2 table

Computation- and Space-Efficient Implementation of SSA

The computational complexity of different steps of the basic SSA is discussed. It is shown that the use of the general-purpose "blackbox" routines (e.g. found in packages like LAPACK) leads to huge waste of time resources since the special Hankel structure of the trajectory matrix is not taken into account. We outline several state-of-the-art algorithms (for example, Lanczos-based truncated SVD) which can be modified to exploit the structure of the trajectory matrix. The key components here are hankel matrix-vector multiplication and hankelization operator. We show that both can be computed efficiently by the means of Fast Fourier Transform. The use of these methods yields the reduction of the worst-case computational complexity from O(N^3) to O(k N log(N)), where N is series length and k is the number of eigentriples desired.Comment: 27 pages, 8 figure