Models.zip contains the input and output files for the nine on-the-fly training simulations described in the main text, as well as the final trained Gaussian process models. Each folder contains files for a different material: Al_Melt: Multi-phase aluminum simulation (Fig. 3) Al_Vacancy: Aluminum with a vacancy (Fig. 4) Al_Adatom: (111) Al slab with an adatom (Fig. 4) AgI: Silver Iodide (Fig. 5) C: Carbon (Fig. 6) Si: Silicon (Fig. 6) Al2O3: Alumin Oxide (Fig. 6) NiTi: Nickel Titanium (Fig. 6) BN: Boron Nitride (Fig. 6) Each folder contains 4 files: .py: Python script used to generate the on-the-fly MD trajectory. .out: FLARE output file containing the coordinates and forces at each timestep. .json: GP model stored in JSON format. The model can be accessed with the "from_dict" method of the FLARE GP class. .gp: GP model stored as a pickled Python object. The model can be accessed with the Python pickle module.