A new strategy is presented for computing anharmonic partition functions for the motion of adsorbates relative to a catalytic surface. Importance sampling is compared with conventional Monte Carlo. The importance sampling is significantly more …
A method for computing anharmonic thermophysical properties for adsorbates on metal surfaces has been extended to include libration, or frustrated rotation. Classical phase space integration is used with Monte Carlo sampling of the configuration …
Many important industrial processes rely on heterogeneous catalytic systems. However, given all possible catalysts and conditions of interest, it is impractical to optimize most systems experimentally. Automatically generated microkinetic models can …
We present a new algorithm for the optimization of molecular structures to saddle points on the potential energy surface using a redundant internal coordinate system. This algorithm automates the procedure of defining the internal coordinate system, …
A new method for computing anharmonic thermophysical properties for adsorbates on metal surfaces is presented. Classical Monte Carlo phase space integration is performed to calculate the partition function for the motion of a hydrogen atom on …
We present a new geodesic-based method for geometry optimization in a basis set of redundant internal coordinates. Our method updates the molecular geometry by following the geodesic generated by a displacement vector on the internal coordinate …
Identification and refinement of first order saddle point (FOSP) structures on the potential energy surface (PES) of chemical systems is a computational bottleneck in the characterization of reaction pathways. Leading FOSP refinement strategies for …
We propose a method that exploits sparse representation of potential energy surfaces (PES) on a polynomial basis set selected by compressed sensing. The method is useful for studies involving large numbers of PES evaluations, such as the search for …