Geodesic interpolation for reaction pathways
Abstract
The development of high throughput reaction discovery methods such as the ab initio nanoreactor demands massive numbers of reaction rate calculations through the optimization of minimum energy reaction paths. These are often generated from interpolations between the reactant and product endpoint geometries. Unfortunately, straightforward interpolation in Cartesian coordinates often leads to poor approximations that lead to slow convergence. In this work, we reformulate the problem of interpolation between endpoint geometries as a search for the geodesic curve on a Riemannian manifold. We show that the perceived performance difference of interpolation methods in different coordinates is the result of an implicit metric change. Accounting for the metric explicitly allows us to obtain good results in Cartesian coordinates, bypassing the difficulties caused by redundant coordinates. Using only geometric information, we are able to generate paths from reactants to products which are remarkably close to the true minimum energy path. We show that these geodesic paths are excellent starting guesses for minimum energy path algorithms.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Apr 22, 2019
- Source ID
- 10.1063/1.5090303
Entities
People
- Keiran C Thompson
- Todd Martinez
- Xiaolei Zhu
Organizations
- Office of Naval Research
- Stanford University
- Toyota Motor North America