“…Therefore, the observed relative Raman shift of the TO band (Δ ω TO,i ) at an individual point i in the Raman map is the sum of the Raman shift of the TO band due to volume densification (magnitude Δ ω TO,vol,i ) and the opposing shift due to increase in the structural disorder (magnitude Δ ω TO,dis,i ): Hence, the wavenumber change of the TO band for point i can be calculated as: The shift due to structural disorder was estimated in the following way. Based on various datasets published in previous studies, 16,19,23,54 the wavenumbers of the TO band were plotted as a function of the bond angle distribution (a measure of the structural disorder) for samples exhibiting different degrees of disorder (FIG 3). The data sets were then fit with linear equations.…”