A Q-learning method based on coarse-to-fine potential energy surface for locating transition state and reaction pathway.

Transition state (TS) on the potential energy surface (PES) plays a key role in determining the kinetics and thermodynamics of chemical reactions. Inspired by the fact that the dynamics of complex systems are always driven by rare but significant transition events, we herein propose a TS search method in accordance with the Q-learning algorithm. Appropriate reward functions are set for a given PES to optimize the reaction pathway through continuous trial and error, and then the TS can be obtained from the optimized reaction pathway. The validity of this Q-learning method with reasonable settings of Q-value table including actions, states, learning rate, greedy rate, discount rate, and so on, is exemplified in 2 two-dimensional potential functions. In the applications of the Q-learning method to two chemical reactions, it is demonstrated that the Q-learning method can predict consistent TS and reaction pathway with those by ab initio calculations. Notably, the PES must be well prepared before using the Q-learning method, and a coarse-to-fine PES scanning scheme is thus introduced to save the computational time while maintaining the accuracy of the Q-learning prediction. This work offers a simple and reliable Q-learning method to search for all possible TS and reaction pathway of a chemical reaction, which may be a new option for effectively exploring the PES in an extensive search manner.

Machine Learning Prediction of the Exfoliation Energies of Two-Dimension Materials via Data-Driven Approach.

Exfoliation energy is one of the fundamental parameters in the science and engineering of two-dimensional (2D) materials. Traditionally, it was obtained via indirect experimental measurement or first-principles calculations, which are very time- and resource-consuming. Herein, we provide an efficient machine learning (ML) method to accurately predict the exfoliation energies for 2D materials. Toward this end, a series of simple descriptors with explicit physical meanings are defined. Regression trees (RT), support vector machines (SVM), multiple linear regression (MLR), and ensemble trees (ET) are compared to develop the most suitable model for the prediction of exfoliation energies. It is shown that the ET model can efficiently predict the exfoliation energies through extensive validations and stability analysis. The influence of the defined features on the exfoliation energies is analyzed by sensitivity analysis to provide novel physical insight into the affecting factors of the exfoliation energies.

Accelerating the optimization of enzyme-catalyzed synthesis conditions via machine learning and reactivity descriptors.

Enzyme-catalyzed synthesis reactions are of crucial importance for a wide range of applications. An accurate and rapid selection of optimal synthesis conditions is crucial and challenging for both human knowledge and computer predictions. In this work, a new scenario, which combines a data-driven machine learning (ML) model with reactivity descriptors, is developed to predict the optimal enzyme-catalyzed synthesis conditions and the reaction yield. Fourteen reactivity descriptors in total are constructed to describe 125 reactions (classified into five categories) included in different reaction mechanisms. Nineteen ML models are developed to train the dataset and the Quadratic support vector machine (SVM) model is found to exhibit the best performance. The Quadratic SVM model is then used to predict the optimal reaction conditions, which are subsequently used to obtain the highest yield among 109 200 reaction conditions with different molar ratios of substrates, solvents, water contents, enzyme concentrations and temperatures for each reaction. The proposed protocol should be generally applicable to a diverse range of chemical reactions and provides a black-box evaluation for optimizing the reaction conditions of organic synthesis reactions.

Data-driven machine learning model for the prediction of oxygen vacancy formation energy of metal oxide materials.

Metal oxides are widely used in the fields of chemistry, physics and materials science. Oxygen vacancy formation energy is a key parameter to describe the chemical, mechanical, and thermodynamic properties of metal oxides. How to acquire quickly and accurately oxygen vacancy formation energy remains a challenge for both experimental and theoretical researchers. Herein, we propose a machine learning model for the prediction of oxygen vacancy formation energy via data-driven analysis and the definition of simple descriptors. Starting with the database containing oxygen vacancy formation energies for 1750 metal oxides with enough structural diversity, new descriptors that effectively avoid the defects of molecular fingerprints, molecular graphic descriptors and site descriptors are defined. The descriptors have obvious physical meanings and wide practicability. Multiple linear regression analysis is then used to screen important features for machine learning model development, and two strongly associated features are obtained. The selected descriptors are used as input for the training of 21 machine learning models to select and develop the most accurate machine learning model. Finally, it is shown that the least squares support vector regression method exhibits the best performance for accurate prediction of the targeted oxygen vacancy formation energy through systematic error analysis, and the prediction accuracy is also verified by the external dataset. Our work establishes a novel and simple computational approach for accurate prediction of the oxygen vacancy formation energy of metal oxides and highlights the availability of data-driven analysis for metal oxide material research.