Integral-Direct and Parallel Implementation of the CCSD(T) Method: Algorithmic Developments and Large-Scale Applications

A completely integral-direct, disk I/O, and network traffic
economic
coupled-cluster singles, doubles, and perturbative triples [CCSD­(T)]
implementation has been developed relying on the density-fitting approximation.
By fully exploiting the permutational symmetry, the presented algorithm
is highly operation count and memory-efficient. Our measurements demonstrate
excellent strong scaling achieved via hybrid MPI/OpenMP parallelization
and a highly competitive, 60–70% utilization of the theoretical
peak performance on up to hundreds of cores. The terms whose evaluation
time becomes significant only for small- to medium-sized examples
have also been extensively optimized. Consequently, high performance
is also expected for systems appearing in extensive data sets used,
e.g., for density functional or machine learning parametrizations,
and in calculations required for certain reduced-cost or local approximations
of CCSD­(T), such as in our local natural orbital scheme [LNO-CCSD­(T)].
The efficiency of this implementation allowed us to perform some of
the largest CCSD­(T) calculations ever presented for systems of 31–43
atoms and 1037–1569 orbitals using only four to eight many-core
CPUs and 1–3 days of wall time. The resulting 13 correlation
energies and the 12 corresponding reaction energies and barrier heights
are added to our previous benchmark set collecting reference CCSD­(T)
results of molecules at the applicability limit of current implementations.