The Journal of Chemical Physics · 2013 · 334 citations · 64 references
Natural SciencesChemistryPhysicsComputational ChemistryQuantum ChemistryTheoretical ChemistryAb Initio MethodsComputational Quantum ChemistryComputational Quantum MechanicsMolecular SymmetryPotential Energy SurfacesQuantum Machine LearningGlobal Potential Energy Surface FittingMachine Learning Potential Energy SurfacesMolecular Potential Energy SurfacesMolecular Symmetry In Quantum ChemistryMultidimensional Potential Energy SurfacesPermutationally Invariant Potential Energy SurfacesQuantum Chemical ModelingReactive Potential Energy Surfaces
A rigorous, general, and simple method to fit global and permutation invariant potential energy surfaces (PESs) using neural networks (NNs) is discussed. This so-called permutation invariant polynomial neural network (PIP-NN) method imposes permutation symmetry by using in its input a set of symmetry functions based on PIPs. For systems with more than three atoms, it is shown that the number of symmetry functions in the input vector needs to be larger than the number of internal coordinates in order to include both the primary and secondary invariant polynomials. This PIP-NN method is successfully demonstrated in three atom-triatomic reactive systems, resulting in full-dimensional global PESs with average errors on the order of meV. These PESs are used in full-dimensional quantum dynamical calculations.
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