A Doubly Nudged Elastic Band Method for Finding Transition States

TL;DR

This paper introduces a modified nudged elastic band method, called DNEB, that significantly improves the efficiency of finding transition states in molecular rearrangements, especially when combined with L-BFGS optimization.

Contribution

The paper presents the doubly nudged elastic band (DNEB) method, enhancing stability and speed in transition state searches using L-BFGS and SQVV minimizers, with applications to Lennard-Jones clusters.

Findings

DNEB/L-BFGS is up to 100 times faster than previous methods.

DNEB effectively finds transition pathways in complex molecular systems.

An updated algorithm for multi-step pathway construction is proposed.

Abstract

A modification of the nudged elastic band (NEB) method is presented that enables stable optimisations to be run using both the limited-memory quasi-Newton (L-BFGS) and slow-response quenched velocity Verlet (SQVV) minimisers. The performance of this new `doubly nudged' DNEB method is analysed in conjunction with both minimisers and compared with previous NEB formulations. We find that the fastest DNEB approach (DNEB/L-BFGS) can be quicker by up to two orders of magnitude. Applications to permutational rearrangements of the seven-atom Lennard-Jones cluster (LJ7) and highly cooperative rearrangements of LJ38 and LJ75 are presented. We also outline an updated algorithm for constructing complicated multi-step pathways using successive DNEB runs.