Subnanometer Scale Mapping of Hydrogen Doping in Vanadium Dioxide

Hydrogen donor doping of correlated electron systems such as vanadium dioxide (VO₂) profoundly modifies the ground state properties. The electrical behavior of HVO₂ is strongly dependent on the hydrogen concentration; hence, atomic scale control of the doping process is necessary. It is however a nontrivial problem to quantitatively probe the hydrogen distribution in a solid matrix. As hydrogen transfers its sole electron to the material, the ionization mechanism is suppressed. In this study, a methodology mapping the doping distribution at subnanometer length scale is demonstrated across a HVO₂ thin film focusing on the oxygen-hydrogen bonds using electron energy loss spectroscopy (EELS) coupled with first-principles EELS calculations. The hydrogen distribution was revealed to be nonuniform along the growth direction and between different VO₂ grains, calling for intricate hydrogenation mechanisms. Our study points to a powerful approach to quantitatively map dopant distribution in quantum materials relevant to energy and information sciences.