相关论文: Multicomponent CASSCF Revisited: Large Active Spac…
The time-dependent restricted-active-space self-consistent-field singles (TD-RASSCF-S) method is presented for investigating TD many-electron dynamics in atoms and molecules. Adopting the SCF notion from the muticonfigurational TD…
Large-scale density functional theory (DFT) calculations provide a powerful tool to investigate the atomic and electronic structure of materials with complex structures. This article reviews a large-scale DFT calculation method, the…
In the near future, material and drug design may be aided by quantum computer assisted simulations. These have the potential to target chemical systems intractable by the most powerful classical computers. However, the resources offered by…
Multipole moments are the first order responses of the energy to spatial derivatives of the electric field strength. The quality of density functional theory (DFT) prediction of molecular multipole moments thus characterizes errors in…
The accurate resolution of the chemical properties of strongly correlated systems, such as biradicals, requires the use of electronic structure theories that account for both multi-reference as well as dynamic correlation effects. A variety…
Fragmentation methods applied to multireference wave functions constitute a road towards the application of highly accurate ab initio wave function calculations to large molecules and solids. However, it is important for reproducibility and…
We present unrestricted Hartree Fock method coupled with configuration interaction (CI) method (URHF-CI) suitable for the calculation of ground and excited states of large number of electrons localized by complex gate potentials in…
Silicon quantum computing has the potential to revolutionize technology with capabilities to solve real-life problems that are computationally complex or even intractable for modern computers [1] by offering sufficient high quality qubits…
Analytic energy gradients are presented for a variational two-electron reduced-density-matrix-driven complete active space self-consistent field (v2RDM-CASSCF) procedure that employs the density-fitting (DF) approximation to the…
The symmetry-projected Hartree--Fock ansatz for the electronic structure problem can efficiently account for static correlation in molecules, yet it is often unable to describe dynamic correlation in a balanced manner. Here, we consider a…
The localized active space self consistent field (LASSCF) method factorizes a complete active space (CAS) wave function into an antisymmetrized product of localized active space wave function fragments. Correlation between fragments is then…
Donor-based quantum devices in silicon are attractive platforms for universal quantum computing and analog quantum simulations. The nearly-atomic precision in dopant placement promises great control over the quantum properties of these…
Chemical accuracy serves as an important metric for assessing the effectiveness of the numerical method in Kohn--Sham density functional theory. It is found that to achieve chemical accuracy, not only the Kohn--Sham wavefunctions but also…
HF-DFT, the practice of evaluating approximate density functionals on Hartree-Fock densities, has long been used in testing density functional approximations. Density-corrected DFT (DC-DFT) is a general theoretical framework for identifying…
In this paper, we study the nuclear gradients of heat bath configuration interaction self-consistent field (HCISCF) wave functions and use them to optimize molecular geometries for various molecules. We show that the HCISCF nuclear…
Computation of electronic spectra is one of the most important applications of methods capturing static electron correlation, including complete-active-space self-consistent field (CASSCF) and post-CASSCF theories. Performance of these…
A second-order many-body perturbation correction to the relativistic Dirac-Hartree-Fock energy is evaluated stochastically by integrating 13-dimensional products of four-component spinors and Coulomb potentials. The integration in the real…
With tens of petaflops supercomputers already in operation and exaflops machines expected to appear within the next 10 years, efficient parallel computational methods are required to take advantage of such extreme-scale machines. In this…
Efficiently recovering dynamic correlation in strongly correlated systems without incurring prohibitive computational costs remains a central challenge in quantum chemistry. In this Perspective, we review and benchmark methods capable of…
Coupled cluster calculations are traditionally performed over Hartree-Fock reference orbitals (HF-CC methodology). However, it has been repeatedly argued in the literature that the use of a Kohn-Sham reference (KS-CC methodology) might…