相关论文: Automatic code generation enables nuclear gradient…

We examine aspects of the computation of finite element matrices and vectors which are made possible by automated code generation. Given a variational form in a syntax which resembles standard mathematical notation, the low-level computer…

We present second-order molecular cluster perturbation theory (MCPT(2)), a linear scaling methodology to calculate arbitrarily large systems with explicit calculation of individual wavefunctions in a coupled-cluster framework. This new…

We report an implementation of self-consistent Green's function many-body theory within a second-order approximation (GF2) for application with molecular systems. This is done by iterative solution of the Dyson equation expressed in matrix…

Computing atomic-scale properties of chemically disordered materials requires an efficient exploration of their vast configuration space. Traditional approaches such as Monte Carlo or Special Quasirandom Structures either entail sampling an…

Electric field-assisted chemistry has attracted much attention in recent years, particularly in the context of oriented external electric fields for controlling molecular structure and reactivity. Such fields have been explored in a wide…

In earlier work [J. Chem. Phys. 144, 064102 (2016)], we introduced a time-dependent formulation of the second-order N-electron valence perturbation theory (t-NEVPT2) which (i) had a lower computational scaling than the usual…

In the near future, material and drug design may be aided by quantum computer assisted simulations. These have the potential to target chemical systems intractable by the most powerful classical computers. However, the resources offered by…

We present a measurement-cost efficient implementation of Strongly-Contracted $N$-Electron Valence Perturbation Theory (SC-NEVPT2) for use on near-term quantum devices. At the heart of our algorithm we exploit the properties of adaptive…

The quantum capacitance model is applied to obtain an exact solution for the space-resolved carrier density in a multigated doped graphene sheet at zero temperature, with quantum correction arising from the finite electron capacity of the…

The efficiency of the recently proposed iCIPT2 [iterative configuration interaction (iCI) with selection and second-order perturbation theory (PT2); J. Chem. Theory Comput. 16, 2296 (2020)] for strongly correlated electrons is further…

Despite recent advances, systematic quantitative treatment of the electron correlation problem in extended systems remains a formidable task. Systematically improvable Green's function methods capable of quantitatively describing weak and…

The development of a novel exact two-component (X2C) scheme with the inclusion of the picture-change correction for the fluctuation potential, the X2Ccorr scheme, is reported, hereby establishing a hierarchy of X2C schemes with systematic…

Computation of electronic spectra is one of the most important applications of methods capturing static electron correlation, including complete-active-space self-consistent field (CASSCF) and post-CASSCF theories. Performance of these…

A doped semiconductor double-quantum-dot molecule is proposed as a qubit realization. The quantum information is encoded in the electron spin, thus benefiting from the long relevant decoherence times; the enhanced flexibility of the…

Atomic-scale phase-field modeling formulates the probability densities of atomic vibrations as Gaussian distributions and derives a free energy functional using variational Gaussian theory and interatomic potentials. This framework permits…

Embedding techniques allow the efficient description of correlations within localized fragments of large molecular systems, while accounting for their environment at a lower level of theory. We introduce FragPT2: a novel embedding framework…

Machine learning is employed to build an energy density functional for self-bound nuclear systems for the first time. By learning the kinetic energy as a functional of the nucleon density alone, a robust and accurate orbital-free density…

A recently developed finite element approach for fully numerical atomic structure calculations [S. Lehtola, Int. J. Quantum Chem. 119, e25945 (2019)] is extended to the description of atoms with spherically symmetric densities via…

We present a novel scheme to accurately predict atomic forces as vector quantities, rather than sets of scalar components, by Gaussian Process (GP) Regression. This is based on matrix-valued kernel functions, on which we impose the…

We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled…