@article{2c2c1b7daa9944b09d4b837d4b71e8ed,
title = "Stochastic evaluation of four-component relativistic second-order many-body perturbation energies: A potentially quadratic-scaling correlation method",
abstract = "A second-order many-body perturbation correction to the relativistic Dirac-Hartree-Fock energy is evaluated stochastically by integrating 13-dimensional products of four-component spinors and Coulomb potentials. The integration in the real space of electron coordinates is carried out by the Monte Carlo (MC) method with the Metropolis sampling, whereas the MC integration in the imaginary-time domain is performed by the inverse-cumulative distribution function method. The computational cost to reach a given relative statistical error for spatially compact but heavy molecules is observed to be no worse than cubic and possibly quadratic with the number of electrons or basis functions. This is a vast improvement over the quintic scaling of the conventional, deterministic second-order many-body perturbation method. The algorithm is also easily and efficiently parallelized with 92% strong scalability going from 64 to 4096 processors.",
author = "Cruz, {J. C{\'e}sar} and Jorge Garza and Takeshi Yanai and So Hirata",
note = "J. C. Cruz acknowledges CONACYT for the scholarship 620190. T. Yanai acknowledges JSPS KAKENHI (Grant Nos. 21H01881 and 21K18931) for financial support. S. Hirata acknowledges the Center for Scalable, Predictive methods for Excitation and Correlated phenomena (SPEC), which is funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, as a part of the Computational Chemical Sciences Program. S. Hirata also acknowledges the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (Grant No. DE-SC0006028). This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231 using NERSC Award No. m3196 (2022). The initial phase of this work was performed at Institute for Molecular Science, Okazaki, Japan.",
year = "2022",
month = jun,
day = "14",
doi = "10.1063/5.0091973",
language = "English (US)",
volume = "156",
journal = "Journal of Chemical Physics",
issn = "0021-9606",
publisher = "American Institute of Physics",
number = "22",
}