Related papers: Orbital optimization of large active spaces via AI…
It is shown that a prechosen set of occupied/virtual valence/core atomic/fragmental orbitals can be transformed to an equivalent set of localized occupied/virtual pre-molecular orbitals (pre-LMO), which can then be taken as probes to select…
We present an approach for the calculation of spin density distributions for molecules that require very large active spaces for a qualitatively correct description of their electronic structure. Our approach is based on the density-matrix…
Accurate electronic structure calculations are essential in modern materials science, but strongly correlated systems pose a significant challenge due to their computational cost. Traditional methods, such as complete active space…
The implementation of an efficient self-consistent field (SCF) method including both scalar relativistic effects and spin-orbit interaction in density functional theory (DFT) is presented. We make use of Gaussian-type orbitals (GTOs) and…
We present an efficient implementation of the Density Matrix Renormalization Group (DMRG) algorithm that includes an optimal ordering of the proton and neutron orbitals and an efficient expansion of the active space utilizing various…
Full configuration interaction (FCI) solvers are limited to small basis sets due to their expensive computational costs. An optimal orbital selection for FCI (OptOrbFCI) is proposed to boost the power of existing FCI solvers to pursue the…
The increasing availability of GPUs for scientific computing has prompted interest in accelerating quantum chemical calculations through their use. The complexity of integral kernels for high angular momentum basis functions however often…
Evaluating high-dimensional integrals via deep hierarchical recurrences is a dominant cost in quantum chemistry. While CPUs manage these efficiently, GPUs suffer a critical mismatch: limited per-thread memory is quickly overwhelmed by an…
We present a general approach to converge excited state solutions to any quantum chemistry orbital optimization process, without the risk of variational collapse. The resulting Square Gradient Minimization (SGM) approach only requires…
During the past 15 years, the density matrix renormalization group (DMRG) has become increasingly important for ab initio quantum chemistry. Its underlying wavefunction ansatz, the matrix product state (MPS), is a low-rank decomposition of…
The general procedure underlying Hartree-Fock and Kohn-Sham density functional theory calculations consists in optimizing orbitals for a self-consistent solution of the Roothaan-Hall equations in an iterative process. It is often ignored…
The emergence of artificial intelligence (AI) accelerators like NVIDIA Tensor Cores offers new opportunities to speed up tensor-heavy scientific computations. However, applying them to quantum chemistry is challenging due to strict accuracy…
Sequential robot manipulation tasks require finding collision-free trajectories that satisfy geometric constraints across multiple object interactions in potentially high-dimensional configuration spaces. Solving these problems in real-time…
This work presents a novel approach to distribute orbitals into subspaces within electron-pairing-based natural orbital functionals (NOFs). This approach modifies the coupling between weakly and strongly occupied orbitals by applying an…
Natural orbital functional (NOF) theory offers a promising approach for studying strongly correlated systems at an affordable computational cost, with an accuracy comparable to highly demanding wavefunction-based methods. However, its…
We present GridFF, an efficient method for simulating molecules on rigid substrates, derived from techniques used in protein-ligand docking in biochemistry. By projecting molecule-substrate interactions onto precomputed spatial grids with…
We have devised and implemented a local ab initio Density Matrix Renormalization Group (DMRG) algorithm to describe multireference nondynamic correlations in large systems. For long molecules that are extended in one of their spatial…
In this paper, we analyze the numerical aspects of the inherently multi-reference density matrix renormalization group (DMRG) calculations on top of the periodic Kohn-Sham density functional theory (DFT) using the complete active space…
A new large-scale parallel multiconfigurational self-consistent field (MCSCF) implementation in the open-source NWChem computational chemistry code is presented. The generalized active space (GAS) approach is used to partition large…
A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…