Chemoton 2.0: Autonomous Exploration of Chemical Reaction Networks

Abstract

Fueled by advances in hardware and algorithm design, large-scale automated explorations of chemical reaction space have become possible. Here, we present our approach to an open-source, extensible framework for explorations of chemical reaction mechanisms based on the first principles of quantum mechanics. It is intended to facilitate reaction network explorations for diverse chemical problems with a wide range of goals such as mechanism elucidation, reaction path optimization, retrosynthetic path validation, reagent design, and microkinetic modeling. The stringent first-principles basis of all algorithms in our framework is key for the general applicability that avoids any restrictions to specific chemical systems. Such an agile framework requires multiple specialized software components of which we present three modules in this work. The key module, Chemoton,drives the exploration of reaction networks. For the exploration itself, we introduce two new algorithms for elementary-step searches that are based on Newton trajectories. The performance of these algorithms is assessed for a variety of reactions characterized by a broad chemical diversity in terms of bonding patterns and chemical elements. We reproduce and significantly extend what is known about these reactions and provide the resulting data to be used as a starting point for further explorations and for future reference.

44 pages, 14 figures, 3 tables

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• Context-Driven Exploration of Complex Chemical Reaction Networks
• Interactive Chemical Reactivity Exploration
• Real-time Quantum Chemistry
• Steering Orbital Optimization out of Local Minima and Saddle Points Toward Lower Energy
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Cited by in corpus (4)

• Universal QM/MM Approaches for General Nanoscale Applications
• Pathfinder -- Navigating and Analyzing Chemical Reaction Networks with an Efficient Graph-based Approach
• High-throughput ab initio reaction mechanism exploration in the cloud with automated multi-reference validation
• Characterizing Reaction Route Map of Realistic Molecular Reactions based on Weight Rank Clique Filtration of Persistent Homology