Entwicklung linear-skalierender Methoden zur Berechnung von Energiegradienten und NMR-Verschiebungen im Rahmen der Møller-Plesset-Störungstheorie zweiter Ordnung

• Antragsteller: Professor Dr. Christian Ochsenfeld
• Fachliche Zuordnung: Theoretische Chemie: Elektronenstruktur, Dynamik, Simulation
• Förderung: Förderung von 2013 bis 2017
• Projektkennung: Deutsche Forschungsgemeinschaft (DFG) - Projektnummer 244944579

• Erstellungsjahr: 2018

Zusammenfassung der Projektergebnisse

Overall the present project funded by the DFG has lead to a pletora of new approaches useful for calculating first- and second-order properties at the MP2 and also at the double-hybrid DFT level. We were able to acquire a solid basis for further developments regarding molecular properties: Our new RI-CDD MP2 energy gradients allow for further studies, especially in regard of EPR spectroscopic parameters. With investigations of second-order properties both at DFT as well as the newly parametrized SCS-/SOS-MP2 methods for calculating NMR chemical shifts new applications for extending the links between theory and experiment open up. Despite the success, many challenges remain for the efficient calculation of MP2 NMR shieldings for large systems and we are continuing our work in this direction, while the accuracies of MP2 shieldings are most promising.

Projektbezogene Publikationen (Auswahl)

• (2018) Gauge-origin dependence in electronic g-tensor calculations. The Journal of chemical physics 148 (21) 214101
  Glasbrenner, Michael; Vogler, Sigurd; Ochsenfeld, Christian
  (Siehe online unter https://doi.org/10.1063/1.5028454)
• (2018) Selected-Nuclei Method for the Computation of Hyperfine Coupling Constants within Second-Order Møller-Plesset Perturbation Theory. Journal of chemical theory and computation 14 (6) 3014–3024
  Vogler, Sigurd; Savasci, Gökcen; Ludwig, Martin; Ochsenfeld, Christian
  (Siehe online unter https://dx.doi.org/10.1021/acs.jctc.8b00116)
• A linear- and sublinear-scaling method for calculating NMR shieldings in atomic orbital-based second-order Møller-Plesset perturbation theory, J. Chem. Phys. 2013, 138, 174104
  M. Maurer, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1063/1.4801084)
• Benchmarking Hydrogen and Carbon NMR Chemical Shifts at HF, DFT, and MP2 Levels, J. Chem. Theory Comput. 2014, 10, 572–578
  D. Flaig, M. Maurer, M. Hanni, K. Braunger, L. Kick, M. Thubauville, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1021/ct400780f)
• Cholesky-decomposed density MP2 with density fitting: accurate MP2 and double-hybrid DFT energies for large systems, J. Chem. Phys. 2014, 140, 224112
  S. A. Maurer, L. Clin, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1063/1.4881144)
• Communication: A reduced scaling J-engine based refomulation of SOS-MP2 using graphics processing units, J. Chem. Phys. 2014, 141, 051106
  S. Maurer, J. Kussmann, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1063/1.4891797)
• A reduced-scaling density matrixbased method for the computation of vibrational Hessian matrix at the selfconsistent field level, J. Chem. Phys. 2015, 142, 094101
  J. Kussmann, A. Luenser, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1063/1.4908131)
• Preselective Screening for Linear-Scaling Exact Exchange-Gradient Calculations for Graphics Processing Units and General Strong-Scaling Massively Parallel Calculations, J. Chem. Theory Comput. 2015, 11, 918–922
  J. Kussmann, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1021/ct501189u)
• Spin Component-Scaled Second-Order Møller- Plesset Perturbation Theory for Calculating NMR Shieldings, J. Chem. Theory Comput. 2015, 11, 37–44
  M. Maurer, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1021/ct5007295)
• Computation of indirect nuclear spin–spin couplings with reduced complexity in pure and hybrid density functional approximations, J. Chem. Phys. 2016, 145, 124103
  A. Luenser, J. Kussmann, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1063/1.4962260)
• Intermolecular 119 Sn,31 P Through-Space Spin-Spin Coupling in a Solid Bivalent Tin Phosphido Complex, Inorg. Chem. 2016, 55, 4669–4675
  J. Arras, K. Eichele, B. Maryasin, H. Schubert, C. Ochsenfeld, K. Wesemann
  (Siehe online unter https://doi.org/10.1021/acs.inorgchem.6b00573)
• Communication: Almost errorfree resolution-of-the-identity correlation methods by null space removal of the particle-hole interactions, J. Chem. Phys. 2017, 146, 211106
  H. F. Schurkus, A. Luenser, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1063/1.4985085)
• Distance-including rigorous upper bounds and tight estimates for two-electron integrals over long- and short-range operators, J. Chem. Phys. 2017, 147, 144101
  T. H. Thompson, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1063/1.4994190)
• Low-scaling first-order properties within second-order Møller-Plesset perturbation theory using Cholesky decomposed density matrices, J. Chem. Phys. 2017, 147, 024101
  S. Vogler, M. Ludwig, M. Maurer, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1063/1.4990413)
• Nuclear Magnetic Shieldings of Stacked Aromatic and Antiaromatic Molecules, J. Chem. Theory Comput. 2017, 13, 1952–1962
  D. Sundholm, M. Rauhalahti, N. Özcan, R. Mera-Adasme, J. Kussmann, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1021/acs.jctc.6b01250)
• Vanishing-Overhead Linear- Scaling Random Phase Approximation by Cholesky Decomposition and an Attenuated Coulomb-Metric, J. Chem. Theory Comput. 2017, 13, 1647–1655
  A. Luenser, H. F. Schurkus, C. Ochsenfeld
  (Siehe online unter https://doi.org/10.1021/acs.jctc.6b01235)