Regularized second-order correlation methods for extended systems.

Second-order Møller-Plesset perturbation theory (MP2) constitutes the simplest form of many-body wavefunction theory and often provides a good compromise between efficiency and accuracy. There are, however, well-known limitations to this approach. In particular, MP2 is known to fail or diverge for some prototypical condensed matter systems like the homogeneous electron gas (HEG) and to overestimate dispersion-driven interactions in strongly polarizable systems.

Physisorption of Water on Graphene: Subchemical Accuracy from Many-Body Electronic Structure Methods.

Wet carbon interfaces are ubiquitous in the natural world and exhibit anomalous properties, which could be exploited by emerging technologies. However, progress is limited by lack of understanding at the molecular level. Remarkably, even for the most fundamental system (a single water molecule interacting with graphene), there is no consensus on the nature of the interaction.

Reaction energetics of hydrogen on Si(100) surface: A periodic many-electron theory study.

We report on a many-electron wavefunction theory study for the reaction energetics of hydrogen dissociation on the Si(100) surface. We demonstrate that quantum chemical wavefunction based methods using periodic boundary conditions can predict chemically accurate results for the activation barrier and the chemisorption energy in agreement with experimental findings. These highly accurate results for the reaction energetics enable a deeper understanding of the underlying physical mechanism and make it possible to benchmark widely used density functional theory methods.

Properties of the water to boron nitride interaction: From zero to two dimensions with benchmark accuracy.

Molecular adsorption on surfaces plays an important part in catalysis, corrosion, desalination, and various other processes that are relevant to industry and in nature. As a complement to experiments, accurate adsorption energies can be obtained using various sophisticated electronic structure methods that can now be applied to periodic systems. The adsorption energy of water on boron nitride substrates, going from zero to 2-dimensional periodicity, is particularly interesting as it calls for an accurate treatment of polarizable electrostatics and dispersion interactions, as well as posing a practical challenge to experiments and electronic structure methods.