Joint approximate diagonalization approach to quasiparticle self-consistent GW calculations.

Area of Science:

• Quantum Chemistry
• Computational Physics
• Materials Science

Background:

• Quasiparticle self-consistent GW (qsGW) is a key method for electronic structure calculations.
• Standard qsGW approximations can limit accuracy.
• Accurate prediction of electronic properties is crucial for materials design.

Purpose of the Study:

• To develop an alternative, more accurate qsGW calculation route.
• To investigate the impact of using the full dynamical self-energy.
• To explore density matrix construction for improved accuracy.

Main Methods:

• Joint approximate diagonalization of one-body GW Green's functions.
• Utilizing input quasiparticle energies.
• Comparison with standard qsGW and coupled-cluster methods on the GW100 set.

Main Results:

• The new method achieves 60 meV mean-absolute-error accuracy for ionization potentials on the GW100 set.
• It successfully incorporates the full dynamical self-energy.
• An intermediate scheme between qsGW and scGW shows improved agreement with coupled-cluster results.

Conclusions:

• The proposed alternative route offers a viable and accurate approach to qsGW calculations.
• Employing the full Green's function for density matrix construction yields more accurate results.
• This work advances the accuracy of electronic structure predictions.