Electronic structure calculations and irradiation measurements are used to obtain insight into oxide trapped charge mechanisms in varying hydrogen ambients. Quantitative agreement between measured and simulated oxide and interface-trap charge densities is obtained over a wide range of H <formula formulatype="inline" xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"><tex Notation="TeX">$_{2}$</tex></formula> concentrations by implementing first-principles calculations of the energetics, and dynamics of charge transport and trapping, into TCAD simulations of irradiated MOS structures. Hole trapping dominates for typical H <formula formulatype="inline" xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex Notation="TeX">$_{2}$</tex></formula> densities, but protons can dominate at high H <formula formulatype="inline" xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"><tex Notation="TeX">$_{2}$</tex></formula> densities. The rate of the interface trap reaction, in which protons that are liberated from charged oxygen vacancies by molecular hydrogen form dangling bonds on the interface, is found to play a key role in determining the relative concentrations of oxide and interface-trap charge densities.