Koopmans' condition for density-functional theory

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	Koopmans' condition for density-functional theory
	Dabo, Ismaila ; Ferretti, Andrea ; Poilvert, Nicolas ; Li, Yanli ; Marzari, Nicola ; Cococcioni, Matteo ; Li YL(李艳丽)
刊名	http://dx.doi.org/10.1103/PhysRevB.82.115121
	2010-09-23
关键词	SHAM ORBITAL ENERGIES IONIZATION-POTENTIALS MOLECULAR-DYNAMICS DERIVATIVE DISCONTINUITIES EXCHANGE VALENCE TEMPERATURE EXCITATIONS ADSORPTION SYSTEMS
英文摘要	MURI [DAAD 19-03-1-016]; University of Minnesota; French National Agency of Research [ANR 06-CIS6-014]; NSF [EAR-0810272]; Abu Dhabi-Minnesota Institute for Research Excellence; DOE [SciDAC DE-FC02-06ER25794, DE-FG02-05ER15728, DE-FG02-05ER46253]; MIT-ISN; In approximate Kohn-Sham density-functional theory, self-interaction manifests itself as the dependence of the energy of an orbital on its fractional occupation. This unphysical behavior translates into qualitative and quantitative errors that pervade many fundamental aspects of density-functional predictions. Here, we first examine self-interaction in terms of the discrepancy between total and partial electron removal energies, and then highlight the importance of imposing the generalized Koopmans' condition-that identifies orbital energies as opposite total electron removal energies-to resolve this discrepancy. In the process, we derive a correction to approximate functionals that, in the frozen-orbital approximation, eliminates the unphysical occupation dependence of orbital energies up to the third order in the single-particle densities. This non-Koopmans correction brings physical meaning to single-particle energies; when applied to common local or semilocal density functionals it provides results that are in excellent agreement with experimental data-with an accuracy comparable to that of GW many-body perturbation theory-while providing an explicit total energy functional that preserves or improves on the description of established structural properties.
语种	英语
出版者	PHYS REV B
内容类型	期刊论文
源URL	[http://dspace.xmu.edu.cn/handle/2288/91597]
专题	物理技术－已发表论文
推荐引用方式 GB/T 7714	Dabo, Ismaila,Ferretti, Andrea,Poilvert, Nicolas,et al. Koopmans' condition for density-functional theory[J]. http://dx.doi.org/10.1103/PhysRevB.82.115121,2010.
APA	Dabo, Ismaila.,Ferretti, Andrea.,Poilvert, Nicolas.,Li, Yanli.,Marzari, Nicola.,...&李艳丽.(2010).Koopmans' condition for density-functional theory.http://dx.doi.org/10.1103/PhysRevB.82.115121.
MLA	Dabo, Ismaila,et al."Koopmans' condition for density-functional theory".http://dx.doi.org/10.1103/PhysRevB.82.115121 (2010).