Gaussian-based quasiparticle self-consistent GW for periodic systems.

Area of Science:

• Computational materials science
• Condensed matter physics
• Quantum chemistry

Background:

• Accurate prediction of electronic properties is crucial for materials design.
• Traditional methods like G0W0 exhibit dependence on density functional approximations.
• Strongly correlated materials pose significant challenges for electronic structure calculations.

Purpose of the Study:

• To present a novel quasiparticle self-consistent GW (QSGW) implementation for periodic systems.
• To benchmark the QSGW implementation against established methods and materials.
• To assess the performance of QSGW in predicting spectral properties of semiconductors and transition metal oxides.

Main Methods:

• Developed a QSGW approach using crystalline Gaussian basis sets.
• Employed a full-frequency analytic continuation GW scheme with Brillouin zone sampling.
• Utilized Gaussian density fitting and finite size corrections for calculations.

Main Results:

• QSGW implementation shows systematic overestimation of band gaps in tested materials.
• QSGW eliminates dependence on the choice of density functionals.
• Achieved more consistent spectral property predictions compared to G0W0 across various solids.

Conclusions:

• The developed QSGW method provides a robust and consistent approach for electronic structure calculations.
• QSGW offers a promising alternative to G0W0, especially for strongly correlated systems.
• This work enables the application of QSGW in ab initio quantum embedding for solid-state materials.