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We are proposing a new computational thermochemistry protocol denoted W3 theory, as a successor to W1 and W2 theory proposed earlier [Martin and De Oliveira, J. Chem. Phys. 111, 1843 (1999)]. The new method is both more accurate overall…

Chemical Physics · Physics 2007-05-23 A. Daniel Boese , Mikhal Oren , Onur Atasoylu , Jan M. L. Martin , Mihaly Kallay , Juergen Gauss

In an attempt to improve on our earlier W3 theory [J. Chem. Phys. {\bf 120}, 4129 (2004)] we consider such refinements as more accurate estimates for the contribution of connected quadruple excitations ($\hat{T}_4$), inclusion of connected…

Chemical Physics · Physics 2007-05-23 Amir Karton , Elena Rabinovich , Jan M. L. Martin , Branko Ruscic

The total atomization energy at absolute zero, (TAE$_0$) of benzene, C$_6$H$_6$, was computed fully {\em ab initio} by means of W2h theory as 1306.6 kcal/mol, to be compared with the experimentally derived value 1305.7+/-0.7 kcal/mol. The…

Chemical Physics · Physics 2009-11-07 S. Parthiban , J. M. L. Martin

The performance of two recent {\em ab initio} computational thermochemistry schemes, W1 and W2 theory [J.M.L. Martin and G. de Oliveira, J. Chem. Phys. 111, 1843 (1999}], is assessed for an enlarged sample of thermochemical data consisting…

Chemical Physics · Physics 2009-11-07 S. Parthiban , Jan M. L. Martin

High-accuracy composite wavefunction methods like Weizmann-4 (W4) theory, high-accuracy extrapolated \textit{ab initio} thermochemistry (HEAT), and Feller-Peterson-Dixon (FPD) enable sub-kJ/mol accuracy in gas-phase thermochemical…

Chemical Physics · Physics 2024-04-12 Emmanouil Semidalas , Amir Karton , Jan M. L. Martin

We consider the thermochemical impact of post-CCSD(T) contributions to the total atomization energy (TAE, the sum of all bond energies) of first- and second-row molecules, and specifically their coupling with the subvalence correlation…

The thermochemistry of the carbon clusters C$_n$ (n=2--10) has been revisited by means of W4 theory and W3.2lite theory. Particularly the larger clusters exhibit very pronounced post-CCSD(T) correlation effects. Despite this, our best…

Chemical Physics · Physics 2010-08-26 Amir Karton , Alex Tarnopolsky , Jan M. L. Martin

To follow up on the unexpectedly-good performance of several coupled-cluster models with approximate inclusion of 3-body clusters [J. Chem. Phys. 151, 064102 (2019)] we performed a more complete assessment of the 3CC method [J. Chem. Phys.…

Chemical Physics · Physics 2025-10-13 Nakul Teke , Ajay Melekamburath , Bimal Gaudel , Edward F. Valeev

By judicious use of extrapolations to the 1-particle basis set limit and $n$-particle calibration techniques, total atomization energies of molecules with up to four heavy atoms can be obtained with calibration accuracy (1 kJ/mol or better,…

Chemical Physics · Physics 2007-05-23 Jan M. L. Martin

Accurate thermochemical data with sub-chemical accuracy (within 1 kcal mol$^{-1}$ of the empirical ground truth) are essential for advancing computational chemistry methods. However, existing datasets that reach this level of accuracy…

The inner-shell correlation contributions to the total atomization energies (TAEs) of the W4-17 computational thermochemistry benchmark have been determined at the CCSD(T) level near the basis set limit using several families of core…

Chemical Physics · Physics 2019-05-15 Nitai Sylvetsky , Jan M. L. Martin

This study evaluates the precision of widely recognized quantum chemical methodologies, CCSD(T), DLPNO-CCSD(T) and localized ph-AFQMC, for determining the thermochemistry of main group elements. DLPNO-CCSD(T) and localized ph-AFQMC, which…

The GW approximation of many-body perturbation theory is an accurate method for computing electron addition and removal energies of molecules and solids. In a canonical implementation, however, its computational cost is $O(N^4)$ in the…

Chemical Physics · Physics 2021-04-21 Jan Wilhelm , Dorothea Golze , Leopold Talirz , Jürg Hutter , Carlo A. Pignedoli

We present a basis set correction scheme for the coupled-cluster singles and doubles (CCSD) method. The scheme is based on employing frozen natural orbitals (FNOs) and diagrammatically decomposed contributions to the electronic correlation…

Materials Science · Physics 2021-06-18 Andreas Irmler , Alejandro Gallo , Andreas Grüneis

An extensive analysis has been carried out of the performance of standard families of basis sets with the hierarchy of coupled cluster methods CC2, CCSD, CC3 and CCSDT in computing selected Oxygen, Carbon and Nitrogen K-edge (vertical) core…

Chemical Physics · Physics 2019-08-13 Johanna P. Carbone , Lan Cheng , Rolf H. Myhre , Devin Matthews , Henrik Koch , Sonia Coriani

Obtaining sub-chemical accuracy (1 kJ mol${}^{-1}$) for reaction energies of medium-sized gas-phase molecules is a longstanding challenge in the field of thermochemical modeling. The perturbative triples correction to CCSD, CCSD(T),…

Chemical Physics · Physics 2025-03-26 Tingting Zhao , James H. Thorpe , Devin A. Matthews

An efficiency of the Tucker decomposition of amplitude tensors within the single-reference relativistic coupled cluster method with single and double excitations (RCCSD) was studied in a series of benchmark calculations for (AuCl)$_n$…

Computational Physics · Physics 2025-07-29 Alexander V. Oleynichenko , Artem S. Rumiantsev , Andrei Zaitsevskii , Ephraim Eliav

The study and prediction of chemical reactivity is one of the most important application areas of molecular quantum chemistry. Large-scale, fully error-tolerant quantum computers could provide exact or near-exact solutions to the underlying…

Quantum Physics · Physics 2019-09-12 Michael Kühn , Sebastian Zanker , Peter Deglmann , Michael Marthaler , Horst Weiß

We introduce a method for solving a self consistent electronic calculation within localized atomic orbitals, that allows us to converge to the complete basis set (CBS) limit in a stable, controlled, and systematic way. We compare our…

Strongly Correlated Electrons · Physics 2015-05-19 S. Azadi , C. Cavazzoni , S. Sorella

We present a near-linear scaling formulation of the explicitly-correlated coupled-cluster singles and doubles with perturbative triples method (CCSD(T)$_{\overline{\text{F12}}}$) for high-spin states of open-shell species. The approach is…

Chemical Physics · Physics 2024-07-30 Ashutosh Kumar , Frank Neese , Edward F. Valeev
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