Accurate Energetics for Open-Shell Systems

Among the greatest challenges in quantum chemistry is to compute accurate energies for the different electronic or spin states of systems that can adopt different valence electronic configurations, or for processes that involve a change in the total number of electrons. The difficulty is further magnified when the effects of the environment, such as solvation, need to be properly accounted for. Both for transition metals and for “simple” organic molecules, our group has been exploring, benchmarking, and applying computational methods from across quantum chemistry with emphasis on modern implementations of correlated wave function methods to achieve reliable and accurate predictions of spin-state energetics, ionization energies, electron affinities, and redox potentials.

Representative publications:

S. E. Neale, D. A. Pantazis, S. A. Macgregor (2020) Accurate computed spin-state energetics for Co(III) complexes: implications for modelling homogeneous catalysis, Dalton Trans., 49, 6478-6487.
https://doi.org/10.1039/d0dt00993h

M. Roemelt, D. A. Pantazis (2019) Multireference Approaches to Spin-State Energetics of Transition Metal Complexes Utilizing the Density Matrix Renormalization Group, Adv. Theory Simul., 1800201.
https://dx.doi.org/10.1002/adts.201800201

R. G. Shirazi, F. Neese, D. A. Pantazis and G. Bistoni (2019) Physical Nature of Differential Spin-State Stabilization of Carbenes by Hydrogen and Halogen Bonding: A Domain-Based Pair Natural Orbital Coupled Cluster Study, J. Phys. Chem. A, 123, 5081-5090. (Cover article)
https://dx.doi.org/10.1021/acs.jpca.9b01051

C. E. Schulz, A. K. Dutta, R. Izsák and D. A. Pantazis (2018) Systematic high-accuracy prediction of electron affinities for biological quinones, J. Comput. Chem., 39, 2439-2451.
https://dx.doi.org/10.1002/jcc.25570

R. G. Shirazi, F. Neese and D. A. Pantazis (2018) Accurate spin-state energetics for aryl carbenes, J. Chem. Theory Comput., 14, 4733-4746.
https://dx.doi.org/10.1021/acs.jctc.8b00587

M. Isegawa, F. Neese, and D. A. Pantazis (2016) Ionization energies and aqueous redox potentials of organic molecules: comparison of DFT, correlated ab initio theory and pair natural orbital approaches, J. Chem. Theory Comput., 12, 2272-2284.
https://dx.doi.org/10.1021/acs.jctc.6b00252

V. Krewald and D. A. Pantazis (2016) Understanding and tuning the properties of redox-accumulating manganese helicates, Dalton Trans., 45, 18900-18908.
https://dx.doi.org/10.1039/C6DT02800D