Related papers: Understanding the core limitations of second-order…
The adiabatic approximation in time-dependent density functional theory (TDDFT) yields reliable excitation spectra with great efficiency in many cases, but fundamentally fails for states of double excitation character. We discuss how…
Density functional calculations for the electronic conductance of single molecules are now common. We examine the methodology from a rigorous point of view, discussing where it can be expected to work, and where it should fail. When…
We discuss energy densities in the strong-interaction limit of density functional theory, deriving an exact expression within the definition (gauge) of the electrostatic potential of the exchange-correlation hole. Exact results for small…
By introducing the self-energy density functionals for the dissipative interactions between the reduced system and its environment, we develop a time-dependent density-functional theory formalism based on an equation of motion for the…
Electron transfer with changing occupation in the 4f subshell poses a considerable challenge for quantitative predictions in quantum chemistry. Using the example of cerium oxide, we identify the main deficiencies of common…
Finite temperature density functional theory requires representations for the internal energy, entropy, and free energy as functionals of the local density field. A central formal difficulty for an orbital-free representation is…
In this work we explore the performance of approximations to electron correlation in reduced density-matrix functional theory (RDMFT) and of approximations to the observables calculated within this theory. Our analysis focuses on the…
The paper is devoted to the study of the twice epi-differentiablity of extended-real-valued functions, with an emphasis on functions satisfying a certain composite representation. This will be conducted under the parabolic regularity, a…
The ability of several density-functional theory (DFT) exchange-correlation functionals to describe hydrogen bonds in small water clusters (dimer to pentamer) in their global minimum energy structures is evaluated with reference to second…
This work is the second in the series "On the performance of QTP functionals applied to second-order response properties." In the first paper (J. Chem. Phys. 162, 054105, 2025), we demonstrated the good performance of Quantum Theory Project…
The exact formulation of multi-configuration density-functional theory (DFT) is discussed in this work. As an alternative to range-separated methods, where electron correlation effects are split in the coordinate space, the combination of…
Potential functional approximations are an intriguing alternative to density functional approximations. The potential functional that is dual to the Lieb density functional is defined and properties given. The relationship between…
Density Functional Theory (DFT) is widely used for atomistic simulations. However, its reach stays limited due to several limitations such as lack of accurate exchange-correlation functional, requirement of costly O(N 3) diagonalization…
Reporting extensions of a recently developed approach to density functional theory with correct long-range be-havior (Phys. Rev. Lett. 94, 043002 (2005)). The central quantities are a splitting functional gamma[n] and a complementary…
Two-dimensional mixtures of dipolar colloidal particles with different dipole moments exhibit extremely rich self-assembly behaviour and are relevant to a wide range of experimental systems, including charged and super-paramagnetic colloids…
Multipole moments are the first order responses of the energy to spatial derivatives of the electric field strength. The quality of density functional theory (DFT) prediction of molecular multipole moments thus characterizes errors in…
An exchange-correlation energy functional $ E_{\mathrm xc} $ and the resultant exchange-correlation potential $ v_{\mathrm xc}({\bf r}) $ in density-functional theory are proposed using orbital-dependent coupling-constant-averaged pair…
DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…
Density functional theory can be extended to excited states by means of a unified variational approach for passive state ensembles. This extension overcomes the restriction of the typical density functional approach to ground states, and…
We study a simple but useful test for neural exchange-correlation (XC) functionals: can a neural model reproduce an established XC functional when it is used self-consistently? We call this test functional cloning. The model is trained at…