Tensor Hypercontraction Second-Order Møller–Plesset
Perturbation Theory: Grid Optimization and Reaction Energies
- Publication date
- Publisher
Abstract
We
have recently introduced the tensor hypercontraction (THC) method
for electronic structure, including MP2. Here, we present an algorithm
for THC-MP2 that lowers the memory requirements as well as the prefactor
while maintaining the formal quartic scaling that we demonstrated
previously. We also describe a procedure to optimize quadrature grids
used in grid-based least-squares (LS) THC-MP2. We apply this algorithm
to generate grids for first-row atoms with less than 100 points/atom
while incurring negligible errors in the computed energies. We benchmark
the LS-THC-MP2 method using optimized grids for a wide variety of
tests sets including conformational energies and reaction barriers
in both the cc-pVDZ and cc-pVTZ basis sets. These tests demonstrate
that the THC methodology is not limited to small basis sets and that
it incurs negligible errors in both absolute and relative energies
