Correlation effects in MgO and CaO: Cohesive energies and lattice constants

Doll, K.; Dolg, Michael; Stoll, Hermann

doi:10.1103/physrevb.54.13529

Cited by 61 publications

(37 citation statements)

References 45 publications

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“…Because the calculated cohesive energy is about 93% of the experimental value for all substances, the correlation contributions are stronger in the more covalent substances and from heavier elements. This is supported by the results of Doll et al [33][34][35][36][37] for the fully ionic alkali halides and alkali-earth oxides, where the HF contribution to the cohesion is about 70%. For the semiconductors we have substances, e.g.…”

Section: Cohesive Energy Of Polar Semiconductorssupporting

confidence: 74%

“…But of course a combination of the method of increments with the local correlation method of Pulay is possible to reduce the computational effort even further [31,32]. The focus of this review lies on the method of increments and its application to ground-state properties of various material classes: From insulators [33][34][35][36][37] over semiconductors [20,21,[38][39][40][41][42] to metals [22,43,44], from strongly bound ionic or covalent systems to weakly bound van der Waals solids [45][46][47], from large molecules [31,48] over polymers [49][50][51][52][53][54][55][56] to three-dimensional solids, from weakly correlated systems to strongly correlated ones such as transition-metal oxides [57,58] and rare-earth nitrides and oxides [59][60][61]. The generalisation to metals is discussed for the example of solid mercury [44,62] and the inclusion of multi-reference treatments for strongly correlated systems is presented for a one-dimensional lithium chain [43].…”

Section: Introductionmentioning

confidence: 98%

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The method of increments—a wavefunction-based ab initio correlation method for solids

2006

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An overview of wavefunction-based correlation methods generalised for the application to solids is presented. Those methods based on a preceding Hartree-Fock treatment explicitly calculate the many-body wavefunction in contrast to the density-functional theory which relies on the ground-state density of the system. This review focus on the so-called method of increments where the correlation energy of the solid is expanded in terms of localised orbitals or of a group of localised orbitals. The method of increments is applied to a great variety of materials, from covalent semiconductors to ionic insulators, from large band-gap materials like diamond to the half-metal -tin, from large molecules like fullerenes over polymers, graphite to three-dimensional solids. Rare-gas crystals where the binding is van der Waals like are treated as well as solid mercury, where the metallic binding is entirely due to correlation. Strongly correlated systems are examined and the correlation driven metal-insulator transition is described at an ab initio level.

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Section: Cohesive Energy Of Polar Semiconductorssupporting

confidence: 74%

Section: Introductionmentioning

confidence: 98%

The method of increments—a wavefunction-based ab initio correlation method for solids

2006

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“…Until now the ground state correlation energies of graphite and diamond, 30,31 of group-IV semiconductors, [32][33][34] III-V and II-VI semiconductors, 33,35-37 oxides such as MgO, rutile (TiO 2 ) or even NiO, [38][39][40][41] light and heavy alkali halides up to AuCl, [42][43][44] GdN, 45 hydro borates, 46 bulk LiH and LiH chains, 47,48 trans-polyacethylene, 49,50 and rare gas crystals 51,52 were estimated. But an application of the incremental method to a chemically more challenging system like a semiconducting polymer with an aromatic system is still missing.…”

Section: Introductionmentioning

confidence: 99%

Quantum chemical ab initio calculations of correlation effects in complex polymers: Poly(para-phenylene)

Willnauer

Birkenheuer

2004

The Journal of Chemical Physics

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Different quantum chemical approaches to the ground state correlation energy per unit cell of infinite poly(para-phenylene) (PPP) chains are presented. PPP is an organic polymer with interesting optical properties, due to its conjugated, aromatic pi system. The inclusion of correlation effects is crucial for a sound quantum chemical description of such a system. The correlation calculations were performed on the coupled cluster with single and double excitations (CCSD) level of theory using Dunning's spd correlation consistent polarized valence double-zeta basis sets. The correlation energy per unit cell is determined by means of the incremental method, which comprises series of CCSD calculations with partial excitation spaces. The resulting correlation energy per unit cell of PPP is -21.797 eV and compares well with that obtained by a simple but much more demanding cluster convergence approach (-21.775 eV). In addition, the accuracy and performance of the incremental scheme is discussed with respect to full CCSD benchmark calculations on PPP oligomers. Two variants are considered, the conventional one based on bond-type local units, and an extended one based on natural chemical subunits. Whereas it is difficult to reach "chemical" accuracy with the first variant, the second variant allows an accurate and efficient treatment with only a few individual CCSD calculations for a polymer with an aromatic pi system such as PPP.

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“…1-4 However, the problem of an ab initio treatment of electron correlations in these systems has only partially been solved. 5 The incremental method [6][7][8][9][10][11][12][13][14][15] combines HF calculations for periodic systems with correlation calculations on corresponding finite clusters. In a series of papers, this computational scheme has proven to be an accurate method for the computation of cohesive properties of semiconductors [6][7][8][9][10][11][12] as well as ionic solids.…”

Section: Introductionmentioning

confidence: 99%

Ab initioapproach to cohesive properties of GdN

et al. 1998

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We apply ab initio quantum-chemical methods to calculate correlation effects on cohesive properties of GdN, thereby extending the recently proposed incremental method to rare-earth compounds. Our calculated values are in reasonable agreement with the experimental cohesive energy ͑86.0%͒ and the experimental lattice constant ͑102.0%͒. Furthermore, we calculate a bulk modulus of 140.3 GPa. Taking into account estimates for the effect of a better basis both at the one-particle level and at the many-particle level, we even reach 98.5% of the experimental cohesive energy and 101.3% of the experimental lattice constant. For this estimate, we obtain a bulk modulus of 163.8 GPa. ͓S0163-1829͑98͒07304-4͔

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Correlation effects in MgO and CaO: Cohesive energies and lattice constants

Cited by 61 publications

References 45 publications

The method of increments—a wavefunction-based ab initio correlation method for solids

The method of increments—a wavefunction-based ab initio correlation method for solids

Quantum chemical ab initio calculations of correlation effects in complex polymers: Poly(para-phenylene)

Ab initioapproach to cohesive properties of GdN

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