The zero-order regular approximation for relativistic effects: The effect of spin–orbit coupling in closed shell molecules

Lenthe, Erik van; Snijders, J.G.; Baerends, Evert Jan

doi:10.1063/1.472460

Cited by 1,604 publications

(1,037 citation statements)

References 47 publications

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“…The CCSD(T) calculations were performed with the MOLPRO 2012 program package. [64,65] The spin-orbit calculations were performed with the ADF code [66,67] at the ZORA-spin orbit level [68][69][70][71][72] with the BLYP functional [40,73] and the TZ2P basis set. The calculations were performed on our local (UA and WSU) Opteron-based and Xeonbased Linux clusters.…”

Section: Computationalmentioning

confidence: 99%

Remarkably High Stability of Late Actinide Dioxide Cations: Extending Chemistry to Pentavalent Berkelium and Californium

Dau

Vasiliu

Peterson

et al. 2017

Chemistry A European J

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Section: Computationalmentioning

confidence: 99%

Remarkably High Stability of Late Actinide Dioxide Cations: Extending Chemistry to Pentavalent Berkelium and Californium

Dau

Vasiliu

Peterson

et al. 2017

Chemistry A European J

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“…18,32,38 The relativistic effects are taken into account at the all-electron level with the zero-orderregular approximation (ZORA) approach. [39][40][41][42][43][44] The molecular orbitals (MOs) were expanded in an uncontracted set of Slater-type orbitals (STO), based on a basis set study. This computational approach has been successful to describe the Pt/C and Co/C interactions.…”

Section: Computational Detailsmentioning

confidence: 99%

Influence of Carbon Support on Electronic Structure and Catalytic Activity of Pt Catalysts: Binding to the CO Molecule

2016

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Single-atom catalysts, especially with single Pt atoms, exhibit potentially improved catalytic activity as compared to metal clusters and metal surfaces. Here, the atop and bridged bondings of the CO molecule on the Pt/C system are studied. Vibrational frequencies, Mulliken populations, charge transfer, charge density differences and density of states are examined to determine the influence of the carbon support on electronic properties and catalytic activity of the Pt adatom and dimer. Comparing orbital populations and the amount of electron transfer to/from the CO molecule show that the net amount of electron transfer to the anti-bonding 2π * orbitals of the CO molecule is higher for the supported Pt dimer than for the substrate-free Pt dimer which leads to a lower vibrational frequency and a larger C−O bond distance. The hybridization between the π orbitals of the polycyclic aromatic hydrocarbons surface and the d orbitals of the Pt adatoms is responsible for enhancing the back donation of electrons to the 2π * orbitals of the CO molecule which results in a larger peak below the Fermi level for the 2π * states of the CO molecule in the corresponding density of state analysis. Therefore, it can be concluded that the carbon support significantly enhances the catalytic activity of the Pt atoms in contact with the surface for activating the CO molecule. The calculated C−O vibrational stretching frequencies provide valuable guidance for experiments considering the use of atom-type catalyst as building blocks for designing new catalysts.

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“…The small size of these bases ensures they are competitive with PP sets in terms of computational efficiency, even though they require a relativistic Hamiltonian such as DKH or zeroth-order regular approximation (ZORA). [139][140][141] The SARC primitives are extrapolated based on CASSCF results, before contraction based on scalar relativistic CASSCF calculations. This procedure was carried out for the 5d transition metal elements, [142] the lanthanides, [143] and the actinides, [144] with a relativistic recontraction of the def2 basis sets performed for the elements of the first three rows of the periodic table to ensure consistency with the SARC bases.…”

Section: Polarization Consistent Basis Setsmentioning

confidence: 99%

Gaussian basis sets for molecular applications

Hill¹

2012

Int J of Quantum Chemistry

188

155

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The choice of basis set in quantum chemical calculations can have a huge impact on the quality of the results, especially for correlated ab initio methods. This article provides an overview of the development of Gaussian basis sets for molecular calculations, with a focus on four popular families of modern atom-centered, energy-optimized bases: atomic natural orbital, correlation consistent, polarization consistent, and def2. The terminology used for describing basis sets is briefly covered, along with an overview of the auxiliary basis sets used in a number of integral approximation techniques and an outlook on possible future directions of basis set design.

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The zero-order regular approximation for relativistic effects: The effect of spin–orbit coupling in closed shell molecules

Cited by 1,604 publications

References 47 publications

Remarkably High Stability of Late Actinide Dioxide Cations: Extending Chemistry to Pentavalent Berkelium and Californium

Remarkably High Stability of Late Actinide Dioxide Cations: Extending Chemistry to Pentavalent Berkelium and Californium

Influence of Carbon Support on Electronic Structure and Catalytic Activity of Pt Catalysts: Binding to the CO Molecule

Gaussian basis sets for molecular applications

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