MP2- and RPA-Based Ab Initio Molecular Dynamics and Monte Carlo Sampling
Nonlocal correlation methods based on wave function theory are developed for application to condensed matter systems. These methods include MP2 and direct-RPA theory as well as double-hybrid functionals. Analytic gradients and stress tensors for MP2 theory in the gamma point approximation have been developed. Sampling complex systems at ambient temperature, for example, liquid water, becomes possible with efficient algorithms for massively parallel computers. Results show a qualitative improvement over standard local density functionals as well as hybrid functionals.
This research was partly supported by NCCR MARVEL, funded by the Swiss National Science Foundation. We acknowledge that the results of this research have been achieved using the PRACE Research Infrastructure resource Hermit based in Germany at Stuttgart (HLRS). Additional calculations were enabled by the Swiss National Supercomputer Centre (CSCS).
- Dunning TH (1989) Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen. J Chem Phys 90:1007–1023Google Scholar
- Hobbs P (1974) Ice physics. Clarendon Press, OxfordGoogle Scholar
- Schmidt J, VandeVondele J, Kuo IFW, Sebastiani D, Siepmann JI, Hutter J, Mundy CJ (2009) Isobaric–isothermal molecular dynamics simulations utilizing density functional theory: an assessment of the structure and density of water at near–ambient conditions. J Phys Chem B 113:11959–11964CrossRefGoogle Scholar