Downfolding from Ab Initio to Interacting Model Hamiltonians: Comprehensive Analysis and Benchmarking of the DFT+cRPA Approach

Abstract

Model Hamiltonians are regularly derived from first-principles data to describe correlated matter. However, the standard methods for this contain a number of largely unexplored approximations. For a strongly correlated impurity model system, here we carefully compare a standard downfolding technique with the best possible ground-truth estimates for charge-neutral excited state energies and wavefunctions using state-of-the-art first-principles many-body wave function approaches. To this end, we use the vanadocene molecule and analyze all downfolding aspects, including the Hamiltonian form, target basis, double counting correction, and Coulomb interaction screening models. We find that the choice of target-space basis functions emerges as a key factor for the quality of the downfolded results, while orbital-dependent double counting correction diminishes the quality. Background screening to the Coulomb interaction matrix elements primarily affects crystal-field excitations. Our benchmark uncovers the relative importance of each downfolding step and offers insights into the potential accuracy of minimal downfolded model Hamiltonians

15 pages (+8 pages Supplemental Material), 10 figures

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• From Polyhedra to Crystals: A Graph-Theoretic Framework for Crystal Structure Generation
• Ground-State-Based Model Reduction with Unitary Circuits
• Theory of ab initio downfolding with arbitrary range electron-phonon coupling
• Quantitative Description of Strongly Correlated Materials by Combining Downfolding Techniques and Tensor Networks
• Bridging constrained random-phase approximation and linear response theory for computing Hubbard parameters
• Engineering Hubbard models with gated two-dimensional moiré systems