Automated reaction kinetics and network exploration (Arkane): A statistical mechanics, thermodynamics, transition state theory, and master equation software

Abstract

The open-source statistical mechanics software described here, Arkane-Automated Reaction Kinetics and Network Exploration-facilitates computations of thermodynamic properties of chemical species, high-pressure limit reaction rate coefficients, and pressure-dependent rate coefficient over multi-well molecular potential energy surfaces (PES) including the effects of collisional energy transfer on phenomenological kinetics. Arkane can use estimates to fill in information for molecules or reactions where quantum chemistry information is missing. The software solves the internal energy master equation for complex unimolecular reaction systems. Inputs to the software include converged electronic structure computations performed by the user using a variety of supported software packages (Gaussian, Molpro, Orca, TeraChem, Q-Chem, Psi4). The software outputs high-pressure limit rate coefficients and pressure-dependentThis is an open access article under the terms of the Creative Commons Attribution-NonCommercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.

Detailed Multiphase Chemical Kinetic Model for Polymer Fouling in a Distillation Column

“…Moreover, whenever errors and failures are raised in a calculation, ARC automatically troubleshoots it and relaunches a new job with updated arguments. Once finishing the necessary quantum calculations, ARC collects the results and feeds them to Arkane, , a statistical mechanics and rate theory calculation package, to yield thermochemical properties or reaction rate coefficients. A graphical depiction of the calculation workflow can be found in our previous work …”

“…Atom energy corrections and Petersson-type bond additivity corrections , to CBS-QB3 are applied for the enthalpy of formation of non-TS molecules. Partition functions of molecules are calculated, and the thermochemical parameters are fitted to NASA polynomials using Arkane. , Furthermore, rate coefficients are obtained using the TS theory (TST) with the Eckart tunneling correction with Arkane. , The SI provides detailed information on the quantum chemical calculations, including the calculation environment, the calculation scheme for different job types, the comparison between estimated and calculated thermochemical parameters, the TS geometries, and how to access the calculation output files.…”

Computing Kinetic Solvent Effects and Liquid Phase Rate Constants Using Quantum Chemistry and COSMO-RS Methods

“…For other QM levels of theory listed in Table , because most of the optimized geometries of the TSs are found to be very similar to those from the ωB97XD/def2-TZVP level, IRC calculations are not performed unless the optimized TS geometries are found to be very different. Instead, the TSs obtained from other QM levels are verified by ensuring that only one imaginary frequency exists and by visually inspecting that the vibrational motion of the imaginary frequency corresponds to the direction along the expected reaction coordinate. High-pressure-limit gas phase rate constants ( k ∞,gas ) are computed using the Arkane software package based on the energies, frequencies, and torsional potentials obtained from Step 1. The rate constants are calculated using the transition state theory with the 1D hindered rotor approximation and the Wigner quantum tunneling correction .…”

“…High-pressure-limit gas phase rate constants ( k ∞,gas ) are computed using the Arkane software package based on the energies, frequencies, and torsional potentials obtained from Step 1. The rate constants are calculated using the transition state theory with the 1D hindered rotor approximation and the Wigner quantum tunneling correction .…”

Pynta─An Automated Workflow for Calculation of Surface and Gas–Surface Kinetics

“…Similar challenges posed in the exploration of gas-phase systems have led to the development of many workflow tools that automate quantum chemistry calculations. Software for computing thermochemistry and rate coefficients for gas-phase kinetic systems include ARC, , Automech, , and KinBot. − The Automat , package can automate the calculation of the energies of adsorbed species. However, we are not aware of any widely distributed software that can automate kinetics calculations for surface reactions.…”