Interpretation of multiple solutions in fully iterative GF2 and GW schemes using local analysis of two-particle density matrices
| Autor: | Dominika Zgid, Pavel Pokhilko |
|---|---|
| Rok vydání: | 2021 |
| Předmět: |
Physics
Chemical Physics (physics.chem-ph) General Physics and Astronomy FOS: Physical sciences Charge (physics) Function (mathematics) Computational Physics (physics.comp-ph) Resonance (particle physics) Condensed Matter - Other Condensed Matter symbols.namesake Local analysis Simple (abstract algebra) Physics - Chemical Physics symbols Condensed Matter::Strongly Correlated Electrons Statistical physics Symmetry breaking Physical and Theoretical Chemistry Hamiltonian (quantum mechanics) Physics - Computational Physics Spin-½ Other Condensed Matter (cond-mat.other) |
| DOI: | 10.48550/arxiv.2104.12751 |
| Popis: | Due to the presence of non-linear equations, iterative Green’s function methods can result in multiple different solutions even for simple molecular systems. In contrast to the wave-function methods, a detailed and careful analysis of such molecular solutions was not performed before. In this work, we use two-particle density matrices to investigate local spin and charge correlators that quantify the charge resonance and covalent characters of these solutions. When applied within the unrestricted orbital set, spin correlators elucidate the broken symmetry of the solutions, containing necessary information for building effective magnetic Hamiltonians. Based on GW and GF2 calculations of simple molecules and transition metal complexes, we construct Heisenberg Hamiltonians, four-spin-four-center corrections, and biquadratic spin–spin interactions. These Hamiltonian parameterizations are compared to previous wave-function calculations. |
| Databáze: | OpenAIRE |
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