A comparison between the one- and two-step spin-orbit coupling approaches based on the ab initio Density Matrix Renormalization Group
arXiv:2207.02435 · doi:10.1063/5.0107805
Abstract
The efficient and reliable treatment of both spin-orbit coupling (SOC) and electron correlation is essential for understanding f-element chemistry. We analyze two approaches to the problem, the one-step approach where both effects are treated simultaneously, and the two-step state interaction approach. We report an implementation of the ab initio density matrix renormalization group (DMRG) with a one-step treatment of the SOC effect which can be compared to prior two-step treatments on an equal footing. Using a dysprosium octahedral complex and bridged dimer as benchmark systems, we identify characteristics of problems where the one-step approach is beneficial for obtaining the low-energy spectrum.
arXiv comment9 pages, 4 figures
References in corpus (31)
- Recent developments in the PySCF program package
- Heat-bath Configuration Interaction: An efficient selected CI algorithm inspired by heat-bath sampling
- Semistochastic Heat-bath Configuration Interaction method: selected configuration interaction with semistochastic perturbation theory
- Quantum Monte Carlo method using phase-free random walks with Slater determinants
- The Density Matrix Renormalization Group in Chemistry and Molecular Physics: Recent Developments and New Challenges
- The density matrix renormalization group for ab initio quantum chemistry
- Spin-orbit excitation energies, anisotropic exchange, and magnetic phases of honeycomb RuCl3
- A spin-adapted Density Matrix Renormalization Group algorithm for quantum chemistry
- Controlling the accuracy of the density matrix renormalization group method: The Dynamical Block State Selection approach
- Quantum information analysis of electronic states at different molecular structures
- Cheap and near exact CASSCF with large active spaces
- An Efficient Matrix Product Operator Representation of the Quantum-Chemical Hamiltonian
- CheMPS2: a free open-source spin-adapted implementation of the density matrix renormalization group for ab initio quantum chemistry
- Ab initio computations of molecular systems by the auxiliary-field quantum Monte Carlo method
- Excited states using semistochastic heat-bath configuration interaction
- Spin-adapted Matrix Product States and Operators
- Auxiliary-field quantum Monte Carlo calculations of molecular systems with a Gaussian basis
- Low communication high performance ab initio density matrix renormalization group algorithms
- Four-Component Density Matrix Renormalization Group
- Phaseless auxiliary-field quantum Monte Carlo calculations with planewaves and pseudopotentials--applications to atoms and molecules
- Targeted Excited State Algorithms
- Systematic electronic structure in the cuprate parent state from quantum many-body simulations
- A General Automatic Method for Optimal Construction of Matrix Product Operators Using Bipartite Graph Theory
- Excited state calculations using phaseless auxiliary-field quantum Monte Carlo: potential energy curves of low lying C2 singlet states
- Eliminating spin contamination in auxiliary-field quantum Monte Carlo: realistic potential energy curve of F2
- One-step treatment of spin-orbit coupling and electron correlation in large active spaces
- Density matrices in full configuration interaction quantum Monte Carlo: Excited states, transition dipole moments and parallel distribution
- A nonorthogonal state-interaction approach for matrix product state wave functions
- Electron paramagnetic resonance g-tensors from state interaction spin-orbit coupling density matrix renormalization group
- SOiCI and iCISO: Combining iterative configuration interaction with spin-orbit coupling in two ways
- Ab initio Calculations in Atoms, Molecules, and Solids, Treating Spin-Orbit Coupling and Electron Interaction on Equal Footing