Tracking the complex non-adiabatic transitions in far-ultraviolet photodissociation demands highly accurate diabatic potential energy matrices (PEMs) across numerous excited states. To address this, we introduce a fully automated diabatization method that leverages artificial neural networks to fit PEMs. Our approach divides the PEM into a physically grounded zeroth-order diagonal term, which is then corrected by a neural network matrix to capture electronic couplings. By enforcing symmetry constraints on off-diagonal elements and sharing degenerate diabatic states between the A′ and A′′ irreducible representations, the { diabatization} process becomes completely automatic. We validate this method using time-dependent wavepacket calculations to simulate the photodissociation of CH2+, incorporating relevant states up to ≈13.6~eV. Finally, we compute partial cross-sections for all fragmentation channels -- including total and partial fragmentation yielding \ce{CH+}, \ce{CH}, \ce{H2}, and \ce{H2+} diatoms -- revealing a notably high cross-section for the formation of the \ce{CH} radical.
@article{arxiv.2605.04756,
title = {Multistate Coupled Diabatic Neural Network potential for the quantum non-adiabatic Photofragmentation of CH$_2^+$},
author = {Pablo del Mazo-Sevillano and Susana Gomez-Carrasco and Alfredo Aguado and Octavio Roncero},
journal= {arXiv preprint arXiv:2605.04756},
year = {2026}
}