Many-Body Quantum Chemistry on Massively Parallel Computers

Abstract

The deployment of many-body quantum chemistry methods onto massively parallel high-performance computing (HPC) platforms is reviewed. The particular focus is on highly accurate methods that have become popular in predictive description of chemical phenomena, such as the coupled-cluster method. The account of relevant literature is preceded by a discussion of the modern and near-future HPC landscape and the relevant computational traits of the many-body methods, in their canonical and reduced-scaling formulations, that underlie the challenges in their HPC realization.

A Perspective on Sustainable Computational Chemistry Software Development and Integration

“…The implementation of the resulting tensor algebra on a distributed partitioned global address space (PGAS) runtime Global Arrays (GA) was also compiler-generated. In addition to many improvements and generalizations (SMITH, SMITH3) of TCE, a major refinement of its ideas is becoming possible by decoupling of the high-level operator algebra and tensor algebra layers, the latter including components for optimization (e.g., factorization) of the algebra of symmetric tensors and its implementation using generic tensor frameworks (including distributed and heterogeneous). − Similar high-level abstractions can be found in other areas of electronic structure, e.g., tensor network computation and DFT …”

Tensor Hypercontraction Form of the Perturbative Triples Energy in Coupled-Cluster Theory

“…Coupled-cluster (CC) theory , is one of the most important advances of modern quantum chemistry, allowing for a polynomial-time evaluation of the electronic energies and wave function of a molecule, as a size-extensive alternative to truncated configuration interaction (CI) methods. , Truncated CC methods also avoid the intractable superexponential scaling of full configuration interaction (FCI), yielding reasonable and chemically accurate relative energies compared to both the FCI limit and to experimental results, especially in the context of CCSD­(T), also known as the “gold standard” method in computational quantum chemistry . The tractability and accuracy of CC methods make the development of efficient CC methods crucial for the future of quantum chemistry, as evaluation of accurate energies and wave functions is made possible for larger and more complex systems through hardware advances such as massively parallel computing − and GPUs. − …”

Cluster-in-Molecule Local Correlation Method for Dispersion Interactions in Large Systems and Periodic Systems

“…For example, for molecular systems, the second-order Mo̷ ller-Plesset perturbation theory (MP2) scales as O(N 5 ), where N is a measure of molecular size. The coupled cluster singles and doubles (CCSD) and CCSD with perturbative triple excitation [CCSD(T)] scale as O(N 6 ) and O(N 7 ), respectively. The steep scaling arises from the adoption of canonical molecular orbitals (CMOs) in solving the corresponding electron correlation equations, in which the correlation between any occupied orbital pairs cannot be neglected.…”