Publications

Revised pob-TZVP-rev2 and pob-DZVP-rev2 basis sets for elements H through Br are derived by incorporating a BSSE correction scheme based on counterpoise energies of hydride dimers into the optimization procedure. The revised basis sets show significantly reduced and more consistent BSSE across the periodic table, with improved portability and SCF stability compared to the original pob basis sets.
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The ab initio cyclic cluster model is presented. The similarity between this Γ-point and molecular approaches allows in principle the application of sophisticated post Hartree–Fock methods to solid-state problems. The cover background shows the treatment of four-center integrals of a periodic hydrogen chain within the Wigner–Seitz supercells of the atoms. The results obtained by the conventional supercell model are fully reproduced, as shown by the crystalline orbitals of the H₈ cluster. Featured on the cover of J. Comput. Chem., Vol. 35, Issues 11–12, 2014.
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The structure, electronic properties, and relative stability of seven thermodynamically stable, metastable, and high-pressure alumina polymorphs as well as four aluminum hydroxides are investigated using periodic hybrid DFT (PW1PW). This is the first comprehensive quantum-chemical study covering all known Al₂O₃ modifications. The energetic order obtained is: gibbsite < bayerite < boehmite < akdalaite < α-Al₂O₃ < κ-Al₂O₃ < θ-Al₂O₃ < δ-Al₂O₃ < γ-Al₂O₃ < η-Al₂O₃ < ι-Al₂O₃.
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High-level multireference quantum-chemical calculations (CASSCF/SC-NEVPT2) are used to elucidate the bonding in charged stacks of thianthrene, selenanthrene, dithiin, and diselenin radical cations. Multicenter bonds form between singly occupied orbitals of adjacent radicals. The singlet state is the ground state in all cases, and only the thianthrene trimers are stable in the gas phase, consistent with experimental observations.
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The geometrical counterpoise correction (gCP) is extended to periodic DFT calculations for the first time. Combined with the DFT-D3 dispersion correction, the approach achieves near-complete-basis-set accuracy for sublimation energies of molecular crystals (X23 benchmark set) at a fraction of the computational cost. gCP parameters are also derived for the pob-TZVP solid-state basis set.
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The pob-TZVP basis sets are presented: consistent, all-electron Gaussian basis sets of triple-zeta valence with polarization quality for periodic solid-state calculations with the CRYSTAL code. Derived from the molecular def2-TZVP standard, the exponents and contraction coefficients are reoptimized for robust SCF convergence across a wide range of ionic, semiconducting, and metallic systems.
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Reactions of thianthrene and selenanthrene with AlCl₃ are studied in melt and in liquid SO₂. Crystal structures of four products are reported, including the novel triple-decker cation (Thianthrene)₃²⁺. Quantum-chemical calculations elucidate bonding and electronic structure of the radical ion dimers and trimers.
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The cover image shows the crystal structure of V₂O₅ and illustrates the implementation of Grimme’s DFT-D3 empirical dispersion correction into a plane wave code, enabling correct description of weak noncovalent interactions in solids. Featured on the cover of J. Comput. Chem., Vol. 33, Issues 25–26, 2012.
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