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Pask, John

Publications and source records attributed to Pask, John.

3 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

SPARC-X: Quantum simulations at extreme scale - reactive dynamics from first principles

We have developed the massively parallel electronic structure code SPARC-X: a computational framework for performing Kohn-Sham Density Functional Theory (DFT) calculations that can scale linearly with the number of atoms in the system, while being able to leverage petascale and emerging exascale parallel computers to study chemical phenomena at unprecedented length and time scales. SPARC-X exploits a recent breakthrough in electronic structure methodologies: systematically improvable, strictly local, orthonormal, discontinuous real-space bases that efficiently and systematically capture the local chemistry of the system. With further adaptation using new machine-learning techniques and the use of the massively parallel Spectral Quadrature (SQ) electronic structure method, the algorithmic complexity and prefactor associated with DFT calculations involving semilocal as well as hybrid functionals are dramatically reduced. Using petascale computational resources, SPARC-X enables quantum mechanical simulations at length and time scales previously accessible only by empirical approaches, e.g., 1,000,000 atoms for a few picoseconds using semilocal functionals or 1,000 atoms for a few picoseconds using hybrid functionals. Using exascale resources, the sizes and times targeted are two orders of magnitude larger. Such a capability has applications in a wide variety of chemical sciences, including reactive interfaces where large length- and/or long time-scales are needed and traditional force fields fail. This is particularly important in dynamic catalysis, where bond breaking and formation must be understood in detail. We developed, tested, and employed the SPARC-X framework to understand the photocatalytic properties of TiO 2 nanoparticles, revealing finite size effects that cannot be captured with standard model systems or functionals. This integrated development and application strategy ensures that SPARC-X remains a robust, efficient, and scalable software package for quantum simulations on current petascale and emerging exascale computing resources.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Spectral-partitioned Kohn-Sham density functional theory

Here we introduce a general, variational scheme for systematic approximation of a given Kohn-Sham free-energy functional by partitioning the density matrix into distinct spectral domains, each of which may be spanned by an independent diagonal representation without requirement of mutual orthogonality. It is shown that by generalizing the entropic contribution to the free energy to allow for independent representations in each spectral domain, the free energy becomes an upper bound to the exact (unpartitioned) Kohn-Sham free energy, attaining this limit as the representations approach Kohn-Sham eigenfunctions. A numerical procedure is devised for calculation of the generalized entropy associated with spectral partitioning of the density matrix. The result is a powerful framework for Kohn-Sham calculations of systems whose occupied subspaces span multiple energy regimes. As a case in point, we apply the proposed framework to warm- and hot-dense matter described by finite-temperature density functional theory, where at high energies the density matrix is represented by that of the free-electron gas, while at low energies it is variationally optimized. We derive expressions for the spectral-partitioned Kohn-Sham Hamiltonian, atomic forces, and macroscopic stresses within the projector-augmented wave (PAW) and the norm-conserving pseudopotential methods. It is demonstrated that at high temperatures, spectral partitioning facilitates accurate calculations at dramatically reduced computational cost. Moreover, as temperature is increased, fewer exact Kohn-Sham states are required for a given accuracy, leading to further reductions in computational cost. Finally, it is shown that standard multiprojector expansions of electronic orbitals within atomic spheres in the PAW method lack sufficient completeness at high temperatures. Spectral partitioning provides a systematic solution for this fundamental problem.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗