相关论文: Automated construction of molecular active spaces …

The selection of a balanced active space is a critical step in multi-reference quantum chemistry calculations, particularly for systems with strong electron correlation. Likewise, active space selection is a key to unlock the potential of…

The accuracy of reaction energy profiles calculated with multi-configurational electronic structure methods and corrected by multi-reference perturbation theory depends crucially on consistent active orbital spaces selected along the…

One of the key challenges of quantum-chemical multi-configuration methods is the necessity to manually select orbitals for the active space. This selection requires both expertise and experience and can therefore impose severe limitations…

We present our implementation autoCAS for fully automated multi-configurational calculations, which we also make available free of charge on our webpages. The graphical user interface of autoCAS connects a general electronic structure…

A widely used strategy to reduce the computational cost in quantum-chemical calculations is to partition the system into an active subsystem, which is the focus of the computational efforts and an environment that is treated at a lower…

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…

The active-space quantum chemical methods could provide very accurate description of strongly correlated electronic systems, which is of tremendous value for natural sciences. The proper choice of the active space is crucial, but a…

ABACUS (Atomic-orbital Based Ab-initio Computation at USTC) is an open-source software for first-principles electronic structure calculations and molecular dynamics simulations. It mainly features density functional theory (DFT) and…

An Adaptive Mesh in Phase Space (AMPS) methodology has been developed for solving multi-dimensional kinetic equations by the discrete velocity method. A Cartesian mesh for both configuration (r) and velocity (v) spaces is produced using a…

We report the derivation and implementation of orbital optimization algorithms for the active space decomposition (ASD) model, which are extensions of complete active space self-consistent field (CASSCF) and its occupation-restricted…

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…

Tracing ultrafast processes induced by interaction of light with matter is often very challenging. In molecular systems, the initially created electronic coherence becomes damped by the slow nuclear rearrangement on a femtosecond timescale…

The ability to understand and engineer molecular structures relies on having accurate descriptions of the energy as a function of atomic coordinates. Here we outline a new paradigm for deriving energy functions of hyperdimensional molecular…

Most modern calculations of many-electron atoms use basis sets of atomic orbitals. An accurate account for the electronic correlations in heavy atoms is very difficult computational problem and optimization of the basis sets can reduce…

Computing accurate rate constants for catalytic events occurring at the surface of a given material represents a challenging task with multiple potential applications in chemistry. To address this question, we propose an approach based on a…

Quantum machine learning -- and specifically Variational Quantum Algorithms (VQAs) -- offers a powerful, flexible paradigm for programming near-term quantum computers, with applications in chemistry, metrology, materials science, data…

Many areas of chemistry are devoted to the challenge of understanding, predicting, and controlling the behavior of strongly localized electrons. Examples include molecular magnetism and luminescence, color centers in crystals,…

We present a new adaptive method for electronic structure calculations based on novel fast algorithms for reduction of multivariate mixtures. In our calculations, spatial orbitals are maintained as Gaussian mixtures whose terms are selected…

We introduce a method for accurate quantum chemical calculations based on a simple variational wave function, defined by a single geminal that couples all the electrons into singlet pairs, combined with a real space correlation factor. The…

Quantum chemical simulations can be greatly accelerated by constructing machine learning potentials, which is often done using active learning (AL). The usefulness of the constructed potentials is often limited by the high effort required…