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Bibliographic Details
Main Authors: Simm, Gregor N. C., Hélie, Jean, Schulz, Hannes, Chen, Yicheng, Simeon, Guillem, Kuzina, Anna, Martinez-Baez, Ernesto, Gasparotto, Piero, Tocci, Gabriele, Chen, Chi, Li, Yatao, Cheng, Lixue, Wang, Zun, Nguyen, Bichlien H., Smith, Jake A., Sun, Lixin
Format: Preprint
Published: 2025
Subjects:
Online Access:https://arxiv.org/abs/2510.13696
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Table of Contents:
  • Polymers are a versatile class of materials with widespread industrial applications. Advanced computational tools could revolutionize their design, but their complex, multi-scale nature poses significant modeling challenges. Conventional force fields often lack the accuracy and transferability required to capture the intricate interactions governing polymer behavior. Conversely, quantum-chemical methods are computationally prohibitive for the large systems and long timescales required to simulate relevant polymer phenomena. Here, we overcome these limitations with a machine learning force field (MLFF) approach. We demonstrate that macroscopic properties for a broad range of polymers can be predicted ab initio, without fitting to experimental data. Specifically, we develop a fast and scalable MLFF to accurately predict polymer densities, outperforming established classical force fields. Our MLFF also captures second-order phase transitions, enabling the prediction of glass transition temperatures. To accelerate progress in this domain, we introduce a benchmark of experimental bulk properties for 130 polymers and an accompanying quantum-chemical dataset. This work lays the foundation for a fully in silico design pipeline for next-generation polymeric materials.