Of the 18 initial conditions considered, the fingerprinting step identifies two initial conditions which produce models with ratios of four-, five-, and six-fold Al coordination environments within error of the experimental data. These are the set of simulations run at 600K and 300K using the cooling scheme at a density of 3.18 g/cm . The results for the 300K model are shown throughout the main text and the 600K results are shown in the Supporting Information with comparable resulting spectra from first principles. The other 16 models, while also within the initial range of possible experimental conditions, therefore likely do not compare to our specific ALD coating of 1000 layers of a-Al2O3, but could possibly be used in future work to model other phases of a-Al2O3 with varying coordination environments.