WeChat Mini Program
Old Version Features

Capturing Dichotomic Solvent Behavior in Solute--Solvent Reactions with Neural Network Potentials

JOURNAL OF CHEMICAL THEORY AND COMPUTATION(2024)

Ecole Polytechnique Fédérale de Lausanne

Cited 0|Views5
Abstract
Simulations of chemical reactivity in condensed phase systems represent an ongoing challenge in computational chemistry, where traditional quantum chemical approaches typically struggle with both the size of the system and the potential complexity of the reaction. Here, we introduce a workflow aimed at efficiently training neural network potentials (NNPs) to explore energy barriers in solution at the hybrid density functional theory level. The computational burden associated with training at the PBE0-D3(BJ) level is bypassed through the use of active and transfer learning techniques, whereas extensive sampling of the transition state region is accelerated by well-tempered metadynamics simulations using multiple time step integration. These NNPs serve to explore a puzzling solute-solvent reactivity route involving the ring opening of N-enoxyphthalimide experimentally observed in methanol but not in 2,2,2-trifluoroethanol (TFE). This reaction represents a challenging example characterized by intricate hydrogen bonding networks and structurally ambiguous solvent-sensitive transition states. The methodology successfully delivers detailed free energy surfaces and relative energy barriers in agreement with experiment. These barriers are associated with an ensemble of transition states involving the direct participation of up to five solvent molecules. While this picture contrasts with the single transition state structure assumed by current static models, no drastic qualitative difference is observed between the formed hydrogen bonding networks and the number of participating solvent molecules in methanol or TFE. The dichotomy between the two solvents thus essentially arises from an electronic effect (i.e., distinct nucleophilicity) and from the larger conformational entropy contributions in methanol. This example underscores the critical role that dynamic simulations at the ab initio levels play in capturing the full complexity of solute-solvent interactions.
More
Translated text
求助PDF
上传PDF
Bibtex
AI Read Science
AI Summary
AI Summary is the key point extracted automatically understanding the full text of the paper, including the background, methods, results, conclusions, icons and other key content, so that you can get the outline of the paper at a glance.
Example
Background
Key content
Introduction
Methods
Results
Related work
Fund
Key content
  • Pretraining has recently greatly promoted the development of natural language processing (NLP)
  • We show that M6 outperforms the baselines in multimodal downstream tasks, and the large M6 with 10 parameters can reach a better performance
  • We propose a method called M6 that is able to process information of multiple modalities and perform both single-modal and cross-modal understanding and generation
  • The model is scaled to large model with 10 billion parameters with sophisticated deployment, and the 10 -parameter M6-large is the largest pretrained model in Chinese
  • Experimental results show that our proposed M6 outperforms the baseline in a number of downstream tasks concerning both single modality and multiple modalities We will continue the pretraining of extremely large models by increasing data to explore the limit of its performance
Upload PDF to Generate Summary
Must-Reading Tree
Example
Generate MRT to find the research sequence of this paper
Data Disclaimer
The page data are from open Internet sources, cooperative publishers and automatic analysis results through AI technology. We do not make any commitments and guarantees for the validity, accuracy, correctness, reliability, completeness and timeliness of the page data. If you have any questions, please contact us by email: report@aminer.cn
Chat Paper
Summary is being generated by the instructions you defined