Hamiltonian Learning of Triplon Excitations in an Artificial Nanoscale Molecular Quantum Magnet

Extracting the Hamiltonian parameters of nanoscale quantum magnets from experimental measurements is a significant challenge in quantum matter. Here we establish a machine learning strategy to extract the parameters of a spin Hamiltonian from inelastic spectroscopy with scanning tunneling microscopy, and we demonstrate this methodology experimentally with an artificial nanoscale molecular magnet based on cobalt phthalocyanine (CoPC) molecules on NbSe₂. We show that this technique allows us to extract the Hamiltonian parameters of a quantum magnet from the differential conductance, including the substrate-induced spatial variation of the exchange couplings. Our methodology leverages a machine learning algorithm trained on exact quantum many-body simulations with tensor networks of finite quantum magnets, leading to a methodology that predicts the Hamiltonian parameters of CoPC quantum magnets of arbitrary size. Our results demonstrate how quantum many-body methods and machine learning enable us to learn a microscopic description of nanoscale quantum many-body systems with scanning tunneling spectroscopy.