<i>Ab initio</i>
 self-energy embedding for the photoemission spectra of NiO and MnO

Iskakov, Sergei; Yeh, Chia-Nan; Gull, Emanuel; Zgid, Dominika

doi:10.1103/physrevb.102.085105

Cited by 52 publications

(66 citation statements)

References 108 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Although our basis sets were tested using MP2, they will be valuable in work using more accurate ab initio correlated methods, such as coupled-cluster theory, [7][8][9]11,12,29 auxiliary field quantum Monte Carlo, 28,[88][89][90][91] or quantum embedding approaches. [92][93][94][95][96][97][98][99][100] In particular, our basis sets remain to be tested on three-dimensional metals, where MP2 is inapplicable. 101 Reliable and standardized Gaussian basis sets for periodic systems also call for the development of optimized auxiliary basis sets for density fitting.…”

Section: Discussionmentioning

confidence: 99%

Correlation-consistent Gaussian basis sets for solids made simple

Ye,

Berkelbach

2021

Preprint

View full text Add to dashboard Cite

The rapidly growing interest in simulating condensed-phase materials using quantum chemistry methods calls for a library of high-quality Gaussian basis sets suitable for periodic calculations. Unfortunately, most standard Gaussian basis sets commonly used in molecular simulation show significant linear dependencies when used in close-packed solids, leading to severe numerical issues that hamper the convergence to the complete basis set (CBS) limit, especially in correlated calculations. In this work, we revisit Dunning's strategy for construction of correlation-consistent basis sets and examine the relationship between accuracy and numerical stability in periodic settings. Specifically, we find that limiting the number of primitive functions avoids the appearance of problematic small exponents while still providing smooth convergence to the CBS limit. As an example, we generate double-, triple-, and quadruple-zeta correlation-consistent Gaussian basis sets for periodic calculations with Goedecker-Teter-Hutter (GTH) pseudopotentials. Our basis sets cover the main-group elements from the first three rows of the periodic table. We verify the fast and reliable convergence to the CBS limit in both Hartree-Fock and post-Hartree-Fock (MP2) calculations, using a diverse test set of 19 semiconductors and insulators.

show abstract

Section: Discussionmentioning

confidence: 99%

Correlation-consistent Gaussian basis sets for solids made simple

Ye,

Berkelbach

2021

Preprint

View full text Add to dashboard Cite

show abstract

“…Following the computational setup in Ref. [58], we choose fcc NiO with lattice constant a = 4.1705Å at temperature T ∼ 451 K (β = 700 E −1 h ). The unit cell is doubled along the [111] direction to capture the antiferromagnetic ordering, which contains two nickel atoms and two oxygen atoms.…”

Section: Realistic Impurity: Seet For Niomentioning

confidence: 99%

“…Noninteracting impurity propagators are generated from a converged GW simulation of the complete unit cell following the SEET framework (for details of the computational setup, see Ref. [58]).…”

Section: Realistic Impurity: Seet For Niomentioning

confidence: 99%

“…As a benchmark, we compare our CDet impurity solver to the ED [78] results used in Ref. [58]. ED requires the discretization of the continuous bath spectrum and its approximation by a few states.…”

Section: Realistic Impurity: Seet For Niomentioning

confidence: 99%

“…Applications to molecular systems therefore form an ideal test bed for impurity solver methods of this type. We complete our benchmark by applying the impurity solver to an impurity generated by a self-energy embedding calculation of antiferromagnetic solid NiO [58].…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Diagrammatic Monte Carlo method for impurity models with general interactions and hybridizations

Wallerberger

Gull

2020

Phys. Rev. Research

Self Cite

View full text Add to dashboard Cite

We present a diagrammatic Monte Carlo method for quantum impurity problems with general interactions and general hybridization functions. Our method uses a recursive determinant scheme to sample diagrams for the scattering amplitude. Unlike in other methods for general impurity problems, an approximation of the continuous hybridization function by a finite number of bath states is not needed and accessing low temperatures does not incur an exponential cost. We test the method for the example of molecular systems, where we systematically vary temperature, interatomic distance, and basis set size. We further apply the method to an impurity problem generated by a self-energy embedding calculation of correlated antiferromagnetic NiO. We find that the method is ideal for quantum impurity problems with a large number of orbitals but only moderate correlations.

show abstract