Exciting DeePMD: Learning excited state energies, forces, and non-adiabatic couplings

التفاصيل البيبلوغرافية
العنوان: Exciting DeePMD: Learning excited state energies, forces, and non-adiabatic couplings
المؤلفون: Dupuy, Lucien, Maitra, Neepa T.
سنة النشر: 2024
المجموعة: Physics (Other)
مصطلحات موضوعية: Physics - Chemical Physics
الوصف: We extend the DeePMD neural network architecture to predict electronic structure properties necessary to perform non-adiabatic dynamics simulations. While learning the excited state energies and forces follows a straightforward extension of the DeePMD approach for ground-state energies and forces, how to learn the map between the non-adiabatic coupling vectors (NACV) and the local chemical environment descriptors of DeePMD is less trivial. Most implementations of machine-learning-based non-adiabatic dynamics inherently approximate the NACVs, with an underlying assumption that the energy-difference-scaled NACVs are conservative fields. We overcome this approximation, implementing the method recently introduced by Richardson [J. Chem. Phys. 158 011102 (2023)], which learns the symmetric dyad of the energy-difference-scaled NACV. The efficiency and accuracy of our neural network architecture is demonstrated through the example of the methaniminium cation CH$_2$NH$_2^+$.
نوع الوثيقة: Working Paper
URL الوصول: http://arxiv.org/abs/2407.10881
رقم الأكسشن: edsarx.2407.10881
قاعدة البيانات: arXiv