相关论文: Applying the Coupled-Cluster Ansatz to Solids and …
In this tutorial-style review we discuss basic concepts of coupled cluster theory and recent developments that increase its computational efficiency for calculations of molecules, solids and materials in general. We will touch upon the…
Many-electron correlation methods offer a systematic approach to predicting material properties with high precision. However, practically attaining accurate ground-state properties for bulk metals presents significant challenges. In this…
Metallic solids are a challenging target for wavefunction-based electronic structure theories and have not been studied in great detail by such methods. Here, we use coupled-cluster theory with single and double excitations (CCSD) to study…
First-principles calculations are a cornerstone of modern surface science and heterogeneous catalysis. However, accurate reaction energies and barrier heights are frequently inaccessible due to the approximations demanded by the large…
Coupled-cluster theory with single, double, and perturbative triple excitations (CCSD(T)) -- often considered the "gold standard" of main-group quantum chemistry -- is inapplicable to three-dimensional metals due to an infrared divergence,…
Coupled-cluster theories can be used to compute ab initio electronic correlation energies of real materials with systematically improvable accuracy. However, the widely-used coupled cluster singles and doubles plus perturbative triples…
We discuss diagrammatic modifications to the coupled cluster doubles (CCD) equations, wherein different groups of terms out of rings, ladders, crossed-rings and mosaics can be removed to form approximations to the coupled cluster method, of…
We present an ab-initio study of boron nitride as well as carbon allotropes. Their relative thermodynamic stabilities and structural phase transitions from low- to high-density phases are investigated. Pressure-temperature phase diagrams…
We use density functional theory (DFT) to investigate the electronic structure and chemical properties of gold nanoparticles. Different structural families of clusters are compared. For up to 60 atoms we optimize structures using DFT-based…
Efficient mixing and pumping of liquids at the microscale is a technology that is still to be optimized. The combination of an AC electric field with a small temperature gradient leads to a strong electro-thermal flow that can be used for…
Coupled cluster theory is one of the most accurate electronic structure methods for predicting ground and excited state chemistry. However, the presence of numerical artifacts at electronic degeneracies, such as complex energies, has made…
Computationally efficient and accurate quantum mechanical approximations to solve the many-electron Schr\"odinger equation are at the heart of computational materials science. In that respect the coupled cluster hierarchy of methods plays a…
In classical computational chemistry, the coupled-cluster ansatz is one of the most commonly used $ab~initio$ methods, which is critically limited by its non-unitary nature. The unitary modification as an ideal solution to the problem is,…
A first-principles study of the adsorption of a single water molecule on a layer of graphitic carbon nitride employing an embedding approach is presented. The embedding approach involves an algorithm to obtain localized Wannier orbitals of…
We present a comparative study of metal-organic interface properties obtained from dispersion corrected density functional theory calculations based on two different approaches: the periodic slab supercell technique and cluster models with…
The structure of oxide-supported metal nanoclusters plays an essential role in their sharply enhanced catalytic activity over bulk metals. Simulations provide the atomic-scale resolution needed to understand these systems. However, the…
We present a general theory to treat periodic solids with quantum-chemistry methods. It relies on two main developments: 1) the modeling of a solid as a Clifford torus which is a torus that is both periodic and flat and 2) the introduction…
We present an efficient implementation of ab initio many-body quantum embedding and local correlation methods for infinite periodic systems through translational symmetry adapted interpolative separable density fitting, an approach which…
Introducing an active space approximation is inevitable for the quantum computations of chemical systems. However, this approximation ignores the electron correlations related to non-active orbitals. Here, we propose a computational method…
Precise parameter estimation plays a central role in science and technology. The statistical error in estimation can be decreased by repeating measurement, leading to that the resultant uncertainty of the estimated parameter is proportional…