Related papers: The Variationally Fitted Electron-Electron Potenti…
In biological and synthetic materials, many important processes involve charges that are present in a medium with spatially varying dielectric permittivity. To accurately understand the role of electrostatic interactions in such systems, it…
For the theoretical understanding of the reactivity of complex chemical systems accurate relative energies between intermediates and transition states are required. Despite its popularity, density functional theory (DFT) often fails to…
A self-consistent calculation scheme for correlated electron systems is created based on the density-functional theory (DFT). Our scheme is a multi-reference DFT (MR-DFT) calculation in which the electron charge density is reproduced by an…
We introduce an orbital free electron density functional approximation based on alchemical perturbation theory. Given convergent perturbations of a suitable reference system, the accuracy of popular self-consistent Kohn-Sham density…
The present study aims at further development of covariant energy density functionals (CEDFs) towards more accurate description of binding energies across the nuclear chart. For the first time, infinite basis corrections to binding energies…
The calculation of electron-phonon (e-ph) coupling from first principles is a topic of great interest in materials science, offering a robust, non-empirical framework to understand and predict a wide range of physical phenomena. While…
The self consistent version of the density functional theory (DFT) is presented, which allows to calculate the ground state and dynamic properties of finite multi-electron systems such as atoms, molecules and clusters. The exact functional…
Density functional theory (DFT) is an exact alternative formulation of quantum mechanics, in which it is possible to calculate the total energy, the spin and the charge density of many-electron systems in the ground state. In practice, it…
We develop a variational formalism in order to study the structure of low energy spectra of frustrated quantum spin systems. It is first applied to trial wavefunctions of ladders with one spin-1/2 on each site. We determine energy minima of…
The reported new algorithm determines the exact exchange potential v_x in a iterative way using energy and orbital shifts (ES, OS) obtained - with finite-difference formulas - from the solutions (occupied orbitals and their energies) of the…
The treatment of atomic anions with Kohn-Sham density functional theory (DFT) has long been controversial since the highest occupied molecular orbital (HOMO) energy, $E_{HOMO}$, is often calculated to be positive with most approximate…
The superposition of atomic potentials (SAP) approach has recently been shown to be a simple and efficient way to initialize electronic structure calculations [S. Lehtola, J. Chem. Theory Comput. 15, 1593 (2019)]. Here, we study the…
We present a critical analysis of the popular fragment-orbital density-functional theory (FO-DFT) scheme for the calculation of electronic coupling values. We discuss the characteristics of different possible formulations or 'flavors' of…
We investigate the feasibility of early fault-tolerant quantum algorithms focusing on ground-state energy estimation problems. In particular, we examine the computation of the cumulative distribution function (CDF) of the spectral measure…
Discontinuous changes in the electronic structure upon infinitesimal changes to the Hamiltonian are demonstrated. Remarkably, these are revealed in one and two electron molecular systems if the realm of the nuclear charge is extended to be…
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…
Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…
The present work proposes to use density-functional theory (DFT) to correct for the basis-set error of wave-function theory (WFT). One of the key ideas developed here is to define a range-separation parameter which automatically adapts to a…
Understanding strongly correlated systems is essential for advancing quantum chemistry and materials science, yet conventional methods like Density Functional Theory (DFT) often fail to capture their complex electronic behavior. To address…
We derive the variational formulation of a gradient damage model by applying the energetic formulation of rate-independent processes and obtain a regularized formulation of fracture. The model exhibits different behavior at traction and…