title: Double-Ended Surface Walking Method for Pathway Building and Transition State Location of Complex Reactions.
abstract: Toward the activity prediction with large-scale computations, here a double-ended surface walking (DESW) method is developed for connecting two minima on a potential energy surface (PES) and locating the associated transition state (TS) using only the first derivatives. The method operates two images starting from the initial and the final states, respectively, to walk in a stepwise manner toward each other. The surface walking involves repeated bias potential addition and local relaxation with the constrained Broyden dimer method to correct the walking direction. We apply the method to a model PES, a large set of gas phase Baker reactions, and complex surface catalytic reactions, which demonstrates that the DESW method can establish a low energy pathway linking two minima even without iterative optimization of the pathway, from which the TS can be located readily. By comparing the efficiency of the new method with the existing methods, we show that the DESW method is much less computationally demanding and is applicable for reactions with complex PESs. We hope that the DESW method may be integrated with the PES sampling methods for automated reaction prediction.
authors.affiliation: Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Key Laboratory of Computational Physical Science (Ministry of Education), Department of Chemistry, Fudan University , Shanghai 200433, China.
authors.forename: Xiao-Jie
authors.initials: XJ
authors.lastname: Zhang
authors.affiliation: Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Key Laboratory of Computational Physical Science (Ministry of Education), Department of Chemistry, Fudan University , Shanghai 200433, China.
authors.forename: Cheng
authors.initials: C
authors.lastname: Shang
authors.affiliation: Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Key Laboratory of Computational Physical Science (Ministry of Education), Department of Chemistry, Fudan University , Shanghai 200433, China.
authors.forename: Zhi-Pan
authors.initials: ZP
authors.lastname: Liu