A Guided Stochastic Energy-Domain Formulation of the Second Order Moller-Plesset Perturbation Theory

作者：Ge, Qinghui; Gao, Yi; Baer, Roi; Rabani, Eran; Neuhauser, Daniel^*

来源：Journal of Physical Chemistry Letters, 2014, 5(1): 185-189.

DOI：10.1021/jz402206m

• RESOLUTION
• MOLECULES

We develop an alternative formulation in the energy-domain to calculate the second order Moller-Plesset (MP2) perturbation energies. The approach is based on repeatedly choosing four random energies using a nonseparable guiding function, filtering four random orbitals at these energies, and averaging the resulting Coulomb matrix elements to obtain a statistical estimate of the MP2 correlation energy. In contrast to our time-domain formulation, the present approach is useful for both quantum chemistry and real-space/plane wave basis sets. The scaling of the MP2 calculation is roughly linear with system size, providing a useful tool to study dispersion energies in large systems. This is demonstrated on a structure of 64 fullerenes within the SZ basis as well as on silicon nanocrystals using real-space grids.

• 出版日期2014-1-16
• 单位浙江大学