Second-Order Møller–Plesset Perturbation Theory in the Condensed Phase: An Efficient and Massively Parallel Gaussian and Plane Waves Approach


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Date

2012-11-13

Publication Type

Journal Article

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Abstract

A novel algorithm, based on a hybrid Gaussian and plane waves (GPW) approach, is developed for the canonical second-order Møller–Plesset perturbation energy (MP2) of finite and extended systems. The key aspect of the method is that the electron repulsion integrals (ia|λσ) are computed by direct integration between the products of Gaussian basis functions λσ and the electrostatic potential arising from a given occupied-virtual pair density ia. The electrostatic potential is obtained in a plane waves basis set after solving the Poisson equation in Fourier space. In particular, for condensed phase systems, this scheme is highly efficient. Furthermore, our implementation has low memory requirements and displays excellent parallel scalability up to 100 000 processes. In this way, canonical MP2 calculations for condensed phase systems containing hundreds of atoms or more than 5000 basis functions can be performed within minutes, while systems up to 1000 atoms and 10 000 basis functions remain feasible. Solid LiH has been employed as a benchmark to study basis set and system size convergence. Lattice constants and cohesive energies of various molecular crystals have been studied with MP2 and double-hybrid functionals.

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published

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Volume

8 (11)

Pages / Article No.

4177 - 4188

Publisher

American Chemical Society

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03947 - VandeVondele, Joost (ehemalig) check_circle

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