Enhancement of DFT-calculations at Petascale: Nuclear Magnetic Resonance, Hybrid Density Functional Theory and Car-Parrinello calculations

TL;DR

This paper enhances the scalability of DFT calculations on petascale supercomputers, enabling large-scale simulations in materials science, chemistry, and biology by introducing parallelism over electronic bands in Quantum ESPRESSO.

Contribution

It introduces an additional level of parallelism over electronic bands in Quantum ESPRESSO, significantly improving large-system DFT calculations on supercomputers.

Findings

Successful computation of NMR chemical shifts in large biological assemblies

Electronic structure analysis of defected amorphous silica with hybrid functionals

Determination of atomic structures of complex molecules on thousands of CPU cores

Abstract

One of the most promising techniques used for studying the electronic properties of materials is based on Density Functional Theory (DFT) approach and its extensions. DFT has been widely applied in traditional solid state physics problems where periodicity and symmetry play a crucial role in reducing the computational workload. With growing compute power capability and the development of improved DFT methods, the range of potential applications is now including other scientific areas such as Chemistry and Biology. However, cross disciplinary combinations of traditional Solid-State Physics, Chemistry and Biology drastically improve the system complexity while reducing the degree of periodicity and symmetry. Large simulation cells containing of hundreds or even thousands of atoms are needed to model these kind of physical systems. The treatment of those systems still remains a computational challenge even with modern supercomputers. In this paper we describe our work to improve the scalability of Quantum ESPRESSO \cite{Quantum-Espresso} for treating very large cells and huge numbers of electrons. To this end we have introduced an extra level of parallelism, over \emph{\emph{electronic bands}}, in three kernels for solving computationally expensive problems: the Sternheimer equation solver (Nuclear Magnetic Resonance, package QE-GIPAW), the Fock operator builder (electronic ground-state, package PWscf) and most of the Car-Parrinello routines (Car-Parrinello dynamics, package CP). Final benchmarks show our success in computing the Nuclear Magnetic Response (NMR) chemical shift of a large biological assembly, the electronic structure of defected amorphous silica with hybrid exchange-correlation functionals and the equilibrium atomic structure of height Porphyrins anchored to a Carbon Nanotube, on many thousands of CPU cores.