相关论文: Analytical nuclear gradients for the range-separat…
An accurate determination of the electron correlation energy is essential for describing the structure, stability, and function in a wide variety of systems, ranging from gas-phase molecular assemblies to condensed matter and…
Recent work has shown that a fully many-body treatment of noncovalent interactions, such as that given by the method of many-body dispersion (MBD), is vital to accurately modeling the structure and energetics of many molecular systems with…
Van der Waals (vdW) interactions are essential for describing molecules and materials, from drug design and catalysis to battery applications. These omnipresent interactions must also be accurately included in machine-learned force fields.…
A common approach to modeling dispersion interactions and overcoming the inaccurate description of long-range correlation effects in electronic structure calculations is the use of pairwise-additive potentials, as in the…
Many-body dispersion (MBD) is a powerful framework to treat van der Waals (vdW) dispersion interactions in density-functional theory and related atomistic modeling methods. Several independent implementations of MBD with varying degree of…
Using a Deep Neuronal Network model (DNN) trained on the large ANI-1 data set of small organic molecules, we propose a transferable density-free many-body dispersion model (DNN-MBD). The DNN strategy bypasses the explicit Hirshfeld…
A correct description of electronic exchange and correlation effects for molecules in contact with extended (metal) surfaces is a challenging task for first-principles modeling. In this work we demonstrate the importance of collective van…
The dispersion component of the van der Waals (vdW) interaction in low-dimensional metals is known to exhibit anomalous "Type-C non-additivity" [Int. J. Quantum Chem. 114, 1157 (2014)]. This causes dispersion energy behavior, at…
Noncovalent van der Waals (vdW) interactions are responsible for a wide range of phenomena in matter. Popular density-functional methods that treat vdW interactions use disparate physical models for these intricate forces, and as a result…
Polymorphs in molecular crystals are often very close in energy, yet they may possess markedly different physical and chemical properties. The understanding and prediction of polymorphism is of paramount importance for a variety of…
We introduce an electron-photon exchange-correlation functional for quantum electrodynamical density-functional theory (QEDFT). The approach, photon MBD (pMBD), is inspired by the many-body dispersion (MBD) method for weak intermolecular…
We introduce a system-independent method to derive effective atomic C$_6$ coefficients and polarizabilities in molecules and materials purely from charge population analysis. This enables the use of dispersion-correction schemes in…
Multi-configurational wave functions are known to describe electronic structure across a Born-Oppenheimer surface qualitatively correct. However, for quantitative reaction energies, dynamical correlation originating from the many…
The many-body dispersion (MBD) framework is a successful approach for modeling the long-range electronic correlation energy and optical response of systems with thousands of atoms. Inspired by field theory, here we develop a…
We estimate polarizabilities of atoms in molecules without electron density, using a Voronoi tesselation approach instead of conventional density partitioning schemes. The resulting atomic dispersion coefficients are calculated, as well as…
Accurate prediction of many-body dispersion (MBD) interactions is essential for understanding the van der Waals forces that govern the behavior of many complex molecular systems. However, the high computational cost of MBD calculations…
We extend our recently proposed Deep Learning-aided many-body dispersion (DNN-MBD) model to quadrupole polarizability (Q) terms using a generalized Random Phase Approximation (RPA) formalism, thus enabling the inclusion of van der Waals…
This paper presents an approach for obtaining accurate interaction energies at the DFT level for systems where dispersion interactions are important. This approach combines Becke and Johnson's [J. Chem. Phys. 127, 154108 (2007)] method for…
We present a structured force reformulation of the many-body dispersion (MBD) model that enables a physically consistent decomposition of forces into pairwise components. By introducing a many-body correlation matrix that scales…
The accuracy of applying density functional theory to noncovalent interactions is hindered by errors arising from low-density regions of interaction-induced change in the density gradient, error compensation between correlation and exchange…