Nagy pontosságú számítások az elméleti kémiában: módszerfejlesztés és alkalmazás
Title in English
High-accuracy calculations in theoretical chemistry: method development and application
Panel
Chemistry 1
Department or equivalent
Department of Physical Chemistry and Materials Science (Budapest University of Technology and Economics)
Starting date
2004-01-01
Closing date
2008-03-31
Funding (in million HUF)
18.203
FTE (full time equivalent)
0.00
state
closed project
Final report
Results in Hungarian
Kutatásaink legfontosabb eredménye olyan nagy pontosságú elméleti módszerek kifejlesztése, amelyek alacsonyabb számításigénnyel rendelkeznek, mint a korábban használt módszerek, de pontosságuk nem marad el az utóbbiak mögött. Kutatásaink nyomán lehetségessé vált kvantumkémiai számítások végzése 10-15 atomos molekulákra és gyökökre 1 kJ/mol-nál nagyobb pontossággal. A pályázat keretében számos olyan molekuláris tulajdonság (pl. polarizálhatóságok, mágneses tulajdonságok) nagy pontosságú számítását is lehetővé tettük, amelyek korábban nem voltak elérhetők. Emellett a kifejlesztett és más kvantumkémiai módszereket kiterjedten alkalmaztuk kémiai problémák megoldására különösen a spektroszkópia és a szerves kémia területén.
Results in English
High-accuracy theoretical methods have been developed, which can provide better computational efficiency than the existing approaches without sacrificing accuracy. Employing these models, high-accuracy calculations (e.g., accuracy of better than 1 kJ/mol for thermochemical properties) can now be performed for molecules and radicals of 10 to 15 atoms. The high-accuracy calculations of molecular properties (e.g., polarizabilities, magnetic properties) that were previously not available have been enabled. Furthermore, the developed and other methods have been applied to chemical problems, especially in the field of spectroscopy and organic chemistry.
Bomble YJ; Saeh JC; Stanton JF; Szalay PG; Kállay M; Gauss J: Equation-of-motion coupled-cluster methods for ionized states with an approximate treatment of triple excitations, J Chem Phys 122:154107, 2005
Kállay M; Gauss J: Approximate treatment of higher
excitations in coupled-cluster theory, J Chem Phys 123:214105, 2005
Willitsch S; Merkt F; Kállay M; Gauss J: Thermochemical properties of small open-shell systems:
Experimental and high-level ab initio results for NH2 and
NH2+, Mol Phys 104:1457, 2006
Poór B; Michniewicz N; Kállay M; Buma WJ; Kubinyi M; Szemik-Hojniak A; Deperasinska I; Puszko A; Zhang H: Femtosecond Studies of Charge-Transfer Mediated Proton Transfer in 2-Butylamino-6-Methyl-4-Nitropyridine N-Oxide, J Phys Chem A 110:7086, 2006
Noga J; Kállay M; Valiron P: On the role of high excitations in the intermolecular
potential of H2-CO, Mol Phys 104:2337, 2006
Heckert M; Kállay M; Tew DP; Klopper W; Gauss J: Basis-Set Extrapolation Techniques for the Accurate Calculation
of Molecular Equilibrium Geometries using Coupled-Cluster Theory, J Chem Phys 125:044108, 2006
Tasi G; Izsák R; Matisz G; Császár AG;Kállay M; Ruscic B; Stanton JF: The Origin of Systematic Error in the Standard Enthalpies of Formation of Hydrocarbons Computed via Atomization Schemes, ChemPhysChem 7:1664, 2006
Bomble YJ; Vazquéz J; Kállay M; Michauk C; Szalay PG; Császár AG; Gauss J; Stanton JF: HEAT: High Accuracy Extrapolated Ab initio Thermochemistry. II. Minor
Improvements to the Protocol and a Vital Simplification, J Chem Phys 125:064108, 2006
Gauss J; Tajti A; Kállay M; Stanton JF; Szalay PG: Analytic Calculation of the Diagonal Born-Oppenheimer Correction within
Configuration-Interaction and Coupled-Cluster Theory, J Chem Phys 125:144111, 2006
Kállay M; Gauss J: Calculation of Frequency-Dependent Polarizabilities using General Coupled-Cluster Models, J Mol Struct (Theochem) 768:71 (invited paper), 2006
Pál K; Kállay M; Kubinyi M; Bakó P; Makó A: Circular dichroism spectra of trans-chalcone epoxides, Tetrahedron Asym. 18:1521, 2007
Gauss J; Ruud K; Kállay M: Gauge-origin independent calculation of magnetizabilities and rotational g tensors at the coupled-cluster level, J Chem Phys 127:074101, 2007
O'Neill D P; Gauss J; Kállay M: Analytic evaluation of Raman intensities in coupled-cluster theory, Mol Phys 105:2447, 2007
O'Neill D P; Gauss J; Kállay M: Calculation of frequency-dependent hyperpolarizabilities using general coupled-cluster models, J Chem Phys 127:134109, 2007
Werner H-J; Kállay M; Gauss J: The barrier height of the F + H2 reaction revisited: Coupled-cluster and multireference configuration-interaction benchmark calculations, J Chem Phys 128:034305, 2008
Costero A M; Colera M; Gavina P; Gil S; Kubinyi M; Pal K; Kállay M: Chiral cyclohexane based fluorescent chemosensors for enantiomeric discrimination of aspartate, Tetrahedron 64:3217, 2008
Shepard R; Kedziora G S; Lischka H; Shavitt I; Müller T; Szalay P G; Kállay M; Seth M: The Accuracy of Molecular Bond Lengths Computed by Multireference Electronic Structure Methods, Chem Phys 349:37, 2008
Pál K; Kállay M; Köhler G; Zhang H; Bitter I; Kubinyi M; Vidóczy T; Grabner G: Efficient singlet state deactivation of cyano-substituted indolines in protic solvents via CN-HO hydrogen bonds, ChemPhysChem 8:2627, 2007
