A Linear-Scaling Integral-Direct Explicitly Correlated Second-Order Møller–Plesset Approach
Mihály Kállay, Péter R. Nagy, Bence Ladóczki, Dávid Mester
TL;DR
This paper introduces a new method for calculating electron correlations in large molecules efficiently, enabling accurate results for systems with hundreds of atoms.
Contribution
A linear-scaling, integral-direct, local MP2-F12 approach that enables explicitly correlated calculations for large systems.
Findings
The method recovers at least 99.9% of the canonical MP2-F12 correlation energy.
Reaction energies have a mean error of less than 1 kJ/mol.
The approach successfully computed a system with 644 atoms, the largest for explicitly correlated calculations.
Abstract
We present an integral-direct, iteration-free, linear-scaling, local explicitly correlated second-order Møller–Plesset (MP2-F12) approach, extending our previous local MP2 method [J. Chem. Theory Comput. 2016, 12, 4897]. The correlation contributions for individual electron pairs are computed within domains defined by the corresponding localized orbitals, while the correlation energies of spatially distant electron pairs are determined via multipole expansions. All the various types of integrals are computed and transformed directly, thereby precluding the need for integral storage and yielding asymptotically constant memory as well as negligible disk I/O demand. Another competitive advantage is the implementation of the 2B MP2-F12 ansatz, the most complete one so far with local approximations, enabling excellent basis set convergence even with double-ζ basis sets. Our validation…
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Taxonomy
TopicsAdvanced Chemical Physics Studies · Molecular spectroscopy and chirality · Protein Structure and Dynamics