The OpenMolcas Web: A Community-Driven Approach to Advancing Computational Chemistry

The developments of the open-source OpenMolcas chemistry software environment since spring 2020 are described, with a focus on novel functionalities accessible in the stable branch of the package or via interfaces with other packages. These developments span a wide range of topics in computational chemistry and are presented in thematic sections: electronic structure theory, electronic spectroscopy simulations, analytic gradients and molecular structure optimizations, ab initio molecular dynamics, and other new features. This report offers an overview of the chemical phenomena and processes OpenMolcas can address, while showing that OpenMolcas is an attractive platform for state-of-the-art atomistic computer simulations

The OpenMolcas Web: A Community-Driven Approach to Advancing Computational Chemistry

The developments of the open-source OpenMolcas chemistry software environment since spring 2020 are described, with a focus on novel functionalities accessible in the stable branch of the package or via interfaces with other packages. These developments span a wide range of topics in computational chemistry and are presented in thematic sections: electronic structure theory, electronic spectroscopy simulations, analytic gradients and molecular structure optimizations, ab initio molecular dynamics, and other new features. This report offers an overview of the chemical phenomena and processes OpenMolcas can address, while showing that OpenMolcas is an attractive platform for state-of-the-art atomistic computer simulations

Nonadiabatic Transition State Theory: Application to Intersystem Crossings in the Active Sites of Metal-Sulfur Proteins

Текст статьи не публикуется в открытом доступе в соответствии с политикой журнала.Nonadiabatic transition state theory (NA-TST) is a powerful tool to investigate the nonradiative transitions between electronic states with different spin multiplicities. The statistical nature of NA-TST provides an elegant and computationally inexpensive way to calculate the rate constants for intersystem crossings, spin-forbidden reactions, and spin-crossovers in large complex systems. The relations between the microcanonical and canoni- cal versions of NA-TST and the traditional transition state theory are shown, followed by a review of the basic steps in a typical NA-TST rate constant calculation. These steps include evalua- tions of the transition probability and coupling between electronic states with different spin multiplicities, a search for the minimum energy crossing point (MECP), and computing the densities of states and partition functions for the reactant and MECP structures. The shortcomings of the spin-diabatic version of NA-TST related to ill-defined state coupling and state count- ing are highlighted. In three examples, we demonstrate the application of NA-TST to intersystem crossings in the active sites of metal-sulfur proteins focusing on [NiFe]-hydrogenase, rubre- doxin, and Fe2S2-ferredoxin. 2016 Wiley Periodicals, Inc

Nonadiabatic Transition State Theory: Application to Intersystem Crossings in the Active Sites of Metal-Sulfur Proteins

Текст статьи не публикуется в открытом доступе в соответствии с политикой журнала.Nonadiabatic transition state theory (NA-TST) is a powerful tool to investigate the nonradiative transitions between electronic states with different spin multiplicities. The statistical nature of NA-TST provides an elegant and computationally inexpensive way to calculate the rate constants for intersystem crossings, spin-forbidden reactions, and spin-crossovers in large complex systems. The relations between the microcanonical and canoni- cal versions of NA-TST and the traditional transition state theory are shown, followed by a review of the basic steps in a typical NA-TST rate constant calculation. These steps include evalua- tions of the transition probability and coupling between electronic states with different spin multiplicities, a search for the minimum energy crossing point (MECP), and computing the densities of states and partition functions for the reactant and MECP structures. The shortcomings of the spin-diabatic version of NA-TST related to ill-defined state coupling and state count- ing are highlighted. In three examples, we demonstrate the application of NA-TST to intersystem crossings in the active sites of metal-sulfur proteins focusing on [NiFe]-hydrogenase, rubre- doxin, and Fe2S2-ferredoxin. 2016 Wiley Periodicals, Inc