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- Chang, Yueqing, et al.
(författare)
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Downfolding from ab initio to interacting model Hamiltonians : comprehensive analysis and benchmarking of the DFT+cRPA approach
- 2024
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Ingår i: npj Computational Materials. - 2057-3960. ; 10:1
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Tidskriftsartikel (refereegranskat)abstract
- Model Hamiltonians are regularly derived from first principles 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 wave functions 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 corrections diminish the quality. Background screening of 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.
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| 2. |
- Schobert, Arne, et al.
(författare)
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Ab initio electron-lattice downfolding : Potential energy landscapes, anharmonicity, and molecular dynamics in charge density wave materials
- 2024
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Ingår i: SciPost Physics. - 2542-4653. ; 16:2
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Tidskriftsartikel (refereegranskat)abstract
- The interplay of electronic and nuclear degrees of freedom presents an outstanding problem in condensed matter physics and chemistry. Computational challenges arise especially for large systems, long time scales, in nonequilibrium, or in systems with strong correlations. In this work, we show how downfolding approaches facilitate complexity reduction on the electronic side and thereby boost the simulation of electronic properties and nuclear motion—in particular molecular dynamics (MD) simulations. Three different downfolding strategies based on constraining, unscreening, and combinations thereof are benchmarked against full density functional calculations for selected charge density wave (CDW) systems, namely 1H-TaS2, 1T-TiSe2, 1H-NbS2, and a one-dimensional carbon chain. We find that the downfolded models can reproduce potential energy surfaces on supercells accurately and facilitate computational speedup in MD simulations by about five orders of magnitude in comparison to purely ab initio calculations. For monolayer 1H-TaS2 we report classical and path integral replica exchange MD simulations, revealing the impact of thermal and quantum fluctuations on the CDW transition.
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