Particle-particle ladder based basis-set corrections applied to atoms and molecules using coupled-cluster theory.

  title={Particle-particle ladder based basis-set corrections applied to atoms and molecules using coupled-cluster theory.},
  author={Andreas Irmler and Andreas Gr{\"u}neis},
  journal={The Journal of chemical physics},
  volume={151 10},
We investigate the basis-set convergence of electronic correlation energies calculated using coupled cluster theory and a recently proposed finite basis-set correction technique. The correction is applied to atomic and molecular systems and is based on a diagrammatically decomposed coupled cluster singles and doubles (CCSD) correlation energy. Only the second-order energy and the particle-particle ladder term are corrected for their basis-set incompleteness error. We present absolute… 

Figures and Tables from this paper

A basis-set error correction based on density-functional theory for strongly correlated molecular systems.

The key result of this study is that the explicit dependence on the on-top pair density allows one to completely remove the dependence on any form of spin polarization without any significant loss of accuracy.

Dynamical correlation energy of metals in large basis sets from downfolding and composite approaches.

This work describes how high-energy excitations treated by MP2 can be "downfolded" into a low-energy active space to be treated by CCSD, and test the composite approach with the direct random-phase approximation used in place of MP2, yielding a method that is typically (but not always) more cost effective due to the smaller number of orbitals that need to be included in the more expensive C CSD calculation.

Accelerating the convergence of auxiliary-field quantum Monte Carlo in solids with optimized Gaussian basis sets.

This work investigates the use of optimized correlation-consistent Gaussian basis sets for the study of insulating solids with auxiliary-field quantum Monte Carlo (AFQMC) and finds that these optimized basis sets yield the most consistent results as a function of volume.

Basis set truncation corrections for improved frozen natural orbital CCSD(T) energies

A number of approaches are proposed and assessed to reduce the frozen natural orbital (FNO) truncation error of coupled-cluster singles and doubles with perturbative triples [CCSD(T)] energies. The

Power Laws Used to Extrapolate the Coupled Cluster Correlation Energy to the Thermodynamic Limit.

An analysis of the transition structure factor showing that N-1 still applies to large system sizes and that the apparent N- 1/3 power law occurs only at low N is provided.

Surface science using coupled cluster theory via local Wannier functions and in-RPA-embedding: The case of water on graphitic carbon nitride.

A plane-wave based implementation to obtain intrinsic atomic orbitals and Wannier functions for arbitrary localization potentials is presented and fragment size convergence for a range of approximate many-electron perturbation theories is discussed.

Abstract Applications of Coupled Cluster Theory to Models of Extended Systems of Fermions

Applications of Coupled Cluster Theory to Models of Extended Systems of Fermions James Michael Callahan This thesis describes the application of coupled-cluster theory to model systems of metallic

Double hybrid DFT calculations with Slater type orbitals

For conformers of organic molecules and noncovalent interactions where very high accuracy is required for qualitatively correct results, DHs provide only small improvements over hybrids, while they still excel in thermochemistry, kinetics, transition metal chemistry and the description of strained organic systems.

Towards Pair Atomic Density Fitting for Correlation Energies with Benchmark Accuracy

Pair atomic density fitting (PADF) has been identified as a promising strategy to reduce the scaling with system size of quantum chemical methods for the calculation of the correlation energy like

A Density-Based Basis-Set Correction for Wave Function Theory.

A universal density-based basis-set incompleteness correction that can be applied to any wave function method and which allows us to obtain CCSD(T) atomization and correlation energies near the CBS limit for the G2 set of molecules with compact Gaussian basis sets.



A complete basis set model chemistry. I. The total energies of closed‐shell atoms and hydrides of the first‐row elements

The major source of errror in most ab initio calculations of molecular energies is the truncation of the one‐electron basis set. A complete basis set model chemistry is defined to include corrections

Explicitly Correlated Coupled-Cluster Theory

The theoretical prediction of molecular energies and properties to chemical accuracy is often achieved using coupled-cluster methods and large orbital basis sets. Through recent advances in F12

Convergence of many-body wave-function expansions using a plane-wave basis: From homogeneous electron gas to solid state systems

Using the finite simulation-cell homogeneous electron gas (HEG) as a model, we investigate the convergence of the correlation energy to the complete-basis-set (CBS) limit in methods utilizing

Correlation problems in atomic and molecular systems III. Rederivation of the coupled-pair many-electron theory using the traditional quantum chemical methodst†‡§

The equations of the coupled-pair many-electron theory (CPMET) for the closed shell systems are rederived both in the spin-orbital and orbital forms without the use of second quantization, Wick's

Coupled cluster channels in the homogeneous electron gas.

Numerical evidence is presented which shows that methods based on this renormalisation have convergent energies in the thermodynamic limit including mosaic-only CCD, which is just a renormalised MP2, which all other methods including only a single channel appear to yield divergent energies.

Explicitly correlated coupled-cluster singles and doubles method based on complete diagrammatic equations.

The CCSD-R12 correlation energies presented here for selected systems using the Slater-type correlation function can, therefore, serve as benchmarks for rigorous assessment of other approximate CC-R 12 methods.

Benchmarks of improved complete basis set extrapolation schemes designed for standard CCSD(T) atomization energies.

  • D. Feller
  • Chemistry
    The Journal of chemical physics
  • 2013
Simple modifications of complete basis set extrapolation formulas chosen from the literature are examined to reproduce a diverse set of 183 reference atomization energies derived primarily from very large basis set standard, frozen core coupled-cluster singles, doubles plus perturbative triples with the aug-cc-pVnZ basis sets.

CCSD(T)/CBS atomic and molecular benchmarks for H through Ar.

These CBS limits can now be used as benchmarks to calibrate more approximate calculations using smaller basis sets, and the sequence of basis sets provides data on convergence patterns for each component of the correlation energy.

Communications: Explicitly correlated second-order Møller-Plesset perturbation method for extended systems.

A formalism for the second-order Møller-Plesset perturbation method employing basis functions that depend explicitly on electron-electron distances (the MP2-R12 or F12 method) is derived and