Angular-Momentum-Dependent Orbital-Free Density Functional Theory

作     者：Youqi Ke Florian Libisch Junchao Xia Lin-Wang Wang Emily A. Carter 

作者机构：Department of Mechanical and Aerospace Engineering Program in Applied and Computational Mathematics and Andlinger Center for Energy and the Environment Princeton University Princeton New Jersey 08544 USA Material Science Division Lawrence Berkeley National Laboratory Berkeley California 94720 USA 

出 版 物：《Physical Review Letters》 (Phys Rev Lett)

年 卷 期：2013年第111卷第6期

页      面：066402-066402页

核心收录：

学科分类：07[理学] 0702[理学-物理学] 

基　　金：Office of Naval Research 

主　　题：DENSITY functional theory ELECTRON density KINETIC energy PSEUDOPOTENTIAL method TRANSITION metal compounds ELECTRON-ion collisions 

摘      要：Orbital-free (OF) density functional theory (DFT) directly solves for the electron density rather than the wave function of many electron systems, greatly simplifying and enabling large scale first principles simulations. However, the required approximate noninteracting kinetic energy density functionals and local electron-ion pseudopotentials severely restrict the general applicability of conventional OFDFT. Here, we present a new generation of OFDFT called angular-momentum-dependent (AMD)-OFDFT to harness the accuracy of Kohn-Sham DFT and the simplicity of OFDFT. The angular momenta of electrons are explicitly introduced within atom-centered spheres so that the important ionic core region can be accurately described. In addition to conventional OF total energy functionals, we introduce a crucial nonlocal energy term with a set of AMD energies to correct errors due to the kinetic energy density functional and the local pseudopotential. We find that our AMD-OFDFT formalism offers substantial improvements over conventional OFDFT, as we show for various properties of the transition metal titanium.