Electron correlation in solids via density embedding theory

被引:77
作者
Bulik, Ireneusz W. [1 ]
Chen, Weibing [1 ]
Scuseria, Gustavo E. [1 ,2 ]
机构
[1] Rice Univ, Dept Chem, Houston, TX 77005 USA
[2] Rice Univ, Dept Phys & Astron, Houston, TX 77005 USA
关键词
BODY PERTURBATION-THEORY; LOCALIZED WANNIER FUNCTIONS; MOLECULAR-ORBITAL METHODS; HEXAGONAL BORON-NITRIDE; COUPLED-CLUSTER THEORY; CORRELATION-ENERGY; NUMERICAL APPLICATION; LINEAR COMBINATION; FUNCTIONAL THEORY; WAVE-FUNCTION;
D O I
10.1063/1.4891861
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Density matrix embedding theory [G. Knizia and G. K.-L. Chan, Phys. Rev. Lett. 109, 186404 (2012)] and density embedding theory [I. W. Bulik, G. E. Scuseria, and J. Dukelsky, Phys. Rev. B 89, 035140 (2014)] have recently been introduced for model lattice Hamiltonians and molecular systems. In the present work, the formalism is extended to the ab initio description of infinite systems. An appropriate definition of the impurity Hamiltonian for such systems is presented and demonstrated in cases of 1, 2, and 3 dimensions, using coupled cluster theory as the impurity solver. Additionally, we discuss the challenges related to disentanglement of fragment and bath states. The current approach yields results comparable to coupled cluster calculations of infinite systems even when using a single unit cell as the fragment. The theory is formulated in the basis of Wannier functions but it does not require separate localization of unoccupied bands. The embedding scheme presented here is a promising way of employing highly accurate electronic structure methods for extended systems at a fraction of their original computational cost. (C) 2014 AIP Publishing LLC.
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页数:10
相关论文
共 61 条
[1]   ON THE INFLUENCE OF NITROGEN PRESSURE ON THE ORDERING OF HEXAGONAL BORON-NITRIDE [J].
ANDREEV, YG ;
LUNDSTROM, T .
JOURNAL OF ALLOYS AND COMPOUNDS, 1994, 216 (01) :L5-L7
[2]  
[Anonymous], 1994, International Series of Monographs on Chemistry
[3]  
[Anonymous], LECT NOTES CHEM
[4]   Atomic orbital Laplace-transformed second-order Moller-Plesset theory for periodic systems [J].
Ayala, PY ;
Kudin, KN ;
Scuseria, GE .
JOURNAL OF CHEMICAL PHYSICS, 2001, 115 (21) :9698-9707
[5]   Perspective: Fifty years of density-functional theory in chemical physics [J].
Becke, Axel D. .
JOURNAL OF CHEMICAL PHYSICS, 2014, 140 (18)
[6]  
Booth G. H., ARXIV13092320V1
[7]   Towards an exact description of electronic wavefunctions in real solids [J].
Booth, George H. ;
Grueneis, Andreas ;
Kresse, Georg ;
Alavi, Ali .
NATURE, 2013, 493 (7432) :365-370
[8]   Density matrix embedding from broken symmetry lattice mean fields [J].
Bulik, Ireneusz W. ;
Scuseria, Gustavo E. ;
Dukelsky, Jorge .
PHYSICAL REVIEW B, 2014, 89 (03)
[9]   Noncollinear density functional theory having proper invariance and local torque properties [J].
Bulik, Ireneusz W. ;
Scalmani, Giovanni ;
Frisch, Michael J. .
PHYSICAL REVIEW B, 2013, 87 (03)
[10]   Perspective on density functional theory [J].
Burke, Kieron .
JOURNAL OF CHEMICAL PHYSICS, 2012, 136 (15)