Related papers: Paying attention to long-range electron correlatio…
An outstanding challenge in chemical computation is the many-electron problem where computational methodologies scale prohibitively with system size. The energy of any molecule can be expressed as a weighted sum of the energies of…
The electronic charge density plays a central role in determining the behavior of matter at the atomic scale, but its computational evaluation requires demanding electronic-structure calculations. We introduce an atom-centered,…
Accurate ab-initio prediction of electronic energies is very expensive for macromolecules by explicitly solving post-Hartree-Fock equations. We here exploit the physically justified local correlation feature in compact basis of small…
Encoding the electronic structure of molecules using 2-electron reduced density matrices (2RDMs) as opposed to many-body wave functions has been a decades-long quest as the 2RDM contains sufficient information to compute the exact molecular…
Energy decomposition analysis (EDA) based on absolutely localized molecular orbitals provides detailed insights into intermolecular bonding by decomposing the total molecular binding energy into physically meaningful components. Here, we…
We introduce a local machine-learning method for predicting the electron densities of periodic systems. The framework is based on a numerical, atom-centred auxiliary basis, which enables an accurate expansion of the all-electron density in…
Machine learning is rapidly accelerating materials and chemical discovery, but most current models target energies, forces, or selected molecular properties rather than the underlying many-body electronic structure. Learning…
Electron correlation effects are essential for an accurate ab initio description of molecules. A quantitative a priori knowledge of the single- or multi-reference nature of electronic structures as well as of the dominant contributions to…
The electron density of a molecule or material has recently received major attention as a target quantity of machine-learning models. A natural choice to construct a model that yields transferable and linear-scaling predictions is to…
Methods for estimating the correlation energy of molecules and other electronic systems are discussed based on the assumption that the correlation energy can be partitioned between atomic regions. In one method, the electron density is…
We present an efficient \textit{ab initio} method for calculating the electronic structure and total energy of strongly correlated electron systems. The method extends the traditional Gutzwiller approximation for one-particle operators to…
The predictive accuracy of Machine Learning (ML) models of molecular properties depends on the choice of the molecular representation. Based on the postulates of quantum mechanics, we introduce a hierarchy of representations which meet…
The computational prediction of the structure and stability of hybrid organic-inorganic interfaces provides important insights into the measurable properties of electronic thin film devices, coatings, and catalyst surfaces and plays an…
We demonstrate a machine learning based approach which can learn the time-dependent electronic excitation dynamics of small molecules subjected to ion irradiation. Ensembles of recurrent neural networks are trained on data generated by…
Multi-configurational approaches yield universal wave function parameterizations that can qualitatively well describe electronic structures along reaction pathways. For quantitative results, multi-reference perturbation theory is required…
A ubiquitous approach to obtain transferable machine learning-based models of potential energy surfaces for atomistic systems is to decompose the total energy into a sum of local atom-centred contributions. However, in many systems…
We propose machine learning (ML) models to predict the electron density -- the fundamental unknown of a material's ground state -- across the composition space of concentrated alloys. From this, other physical properties can be inferred,…
Electron density is a fundamental quantity, which can in principle determine all ground state electronic properties of a given system. Although machine learning (ML) models for electron density based on either an atom-centered basis or a…
In principle, many-electron correlation energy can be precisely computed from a reduced Wigner distribution function ($\mathcal{W}$) thanks to a universal functional transformation ($\mathcal{F}$), whose formal existence is akin to that of…
Ab initio electronic structure methods give accurate results for small systems, but do not scale well to large systems. Chemical insight tells us that molecular functional groups will behave approximately the same way in all molecules,…