Adiabatic-connection fluctuation-dissipation density-functional theory based on range separation

Adiabatic-Connection-Fluctuation-Dissipation approach to the long-range behavior of the exchange-correlation energy at metal surfaces: A numerical study for jellium slabs

A still open issue in many-body theory is the asymptotic behavior of the exchange-correlation energy and potential in the vacuum region of a metal surface. Here we report a numerical study of the position-dependent exchange-correlation energy for jellium slabs, as obtained by combining the formally exact adiabatic-connection-fluctuation-dissipation theorem with either time-dependent density-functional theory or an inhomogeneous Singwi-Tosi-Land-Sjölander approach. We find that the inclusion of correlation allows to obtain well-converged semi-infinite-jellium results (independent of the slab th…

Efficient and accurate calculation of exact exchange and RPA correlation energies in the Adiabatic-Connection Fluctuation-Dissipation theory

Recently there has been a renewed interest in the calculation of exact-exchange and RPA correlation energies for realistic systems. These quantities are main ingredients of the so-called EXX/RPA+ scheme which has been shown to be a promising alternative approach to the standard LDA/GGA DFT for weakly bound systems where LDA and GGA perform poorly. In this paper, we present an efficient approach to compute the RPA correlation energy in the framework of the Adiabatic-Connection Fluctuation-Dissipation formalism. The method is based on the calculation of a relatively small number of eigenmodes of…

Energy Dissipation during Diffusion at Metal Surfaces: Disentangling the Role of Phonons vs. Electron-Hole Pairs

Helium spin echo experiments combined with ab initio-based Langevin molecular dynamics simulations are used to quantify the adsorbate-substrate coupling during the thermal diffusion of Na atoms on Cu(111). An analysis of trajectories within the local density friction approximation allows the contribution from electron-hole pair excitations to be separated from the total energy dissipation. Despite the minimal electronic friction coefficient of Na and the relatively small mass mismatch to Cu promoting efficient phononic dissipation, about $(20\pm5)\%$ of the total energy loss is attributable to…

铁电软模的非绝热动力学

Non adiabatic dynamics of the ferroelectric soft mode

本研究通过时间分辨二次谐波生成和泵-探测反射率，揭示了SnTe中非绝热铁电软模的动力学行为，展示了极化和晶格运动的非线性耦合及时间尺度分离效应。

Adiabatic-connection fluctuation-dissipation DFT for the structural properties of solids-the renormalized ALDA and electron gas kernels

We present calculations of the correlation energies of crystalline solids and isolated systems within the adiabatic-connection fluctuation-dissipation formulation of density-functional theory. We perform a quantitative comparison of a set of model exchange-correlation kernels originally derived for the homogeneous electron gas (HEG), including the recently-introduced renormalized adiabatic local-density approximation (rALDA) and also kernels which (a) satisfy known exact limits of the HEG, (b) carry a frequency dependence or (c) display a 1/$k^2$ divergence for small wavevectors. After general…

Accurate Total Energies from the Adiabatic-Connection Fluctuation-Dissipation Theorem

In the context of inhomogeneous one-dimensional finite systems, recent numerical advances [Phys. Rev. B 103, 125155 (2021)] allow us to compute the exact coupling-constant dependent exchange-correlation kernel $f^λ_\text{xc}(x,x',ω)$ within linear response time-dependent density functional theory. This permits an improved understanding of ground-state total energies derived from the adiabatic-connection fluctuation-dissipation theorem (ACFDT). We consider both `one-shot' and `self-consistent' ACFDT calculations, and demonstrate that chemical accuracy is reliably preserved when the frequency de…