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    The GW approximation in many-body perturbation theory can yield unphysical results for molecular systems. Different algorithms for solving the quasiparticle equation lead to discontinuities in calculated energies.

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    Area of Science:

    • Computational chemistry
    • Condensed matter physics
    • Quantum mechanics

    Background:

    • The GW approximation is a powerful tool for calculating electronic properties of materials.
    • Accurate prediction of molecular properties requires reliable computational methods.
    • Self-consistent solutions are crucial for the validity of theoretical predictions.

    Purpose of the Study:

    • To investigate unphysical irregularities in the GW approximation for molecular systems.
    • To analyze the dependence of GW calculations on the quasiparticle self-consistent equation solver.
    • To identify the origin and implications of discontinuities in quasiparticle energies.

    Main Methods:

    • Application of the GW approximation within many-body perturbation theory.
    • Analysis of partially self-consistent GW schemes.
    • Investigation of quasiparticle (QP) equation solution algorithms.
    • Examination of occupied, virtual, and frontier orbitals in diatomic molecules.

    Main Results:

    • Unphysical discontinuities observed in experimentally measurable quantities.
    • QP solution dependence on the chosen self-consistent algorithm.
    • Each self-energy branch corresponds to a distinct QP solution.
    • "Ripple" effects: discontinuities in one QP energy induce smaller discontinuities in others.
    • Multisolution behavior is more probable for frontier orbitals with small HOMO-LUMO gaps.

    Conclusions:

    • Partially self-consistent GW schemes can lead to unphysical results.
    • Algorithm choice significantly impacts QP energy calculations.
    • Understanding these discontinuities is vital for accurate theoretical predictions in molecular systems.