The germanium distribution in the UTL framework is shown to be the most skewed towards preferential occupation of the D4R units. Note, however, that herein, we adopt a UTL unit cell containing only one D4R unit, deferring the discussion of the asymmetry of D4R occupation to Section 3.3, which focusses on finite size effects. The preference for the occupation of D4R T sites in UTL is sizable already for low germanium content and grows, primarily at the expense of the framework occupation (Figure ), up until Si/Ge of approximately 4 -5, reaching an average of six germaniums per D4R unit, at which it levels off and starts to decrease for very high germanium loading (up to Si/Ge = 2.2). The occupation of the adjacent T-sites is mostly unaffected across the Si/Ge range, hovering just below its statistical class multiplicity. The most stable distributions (Figure ) corresponding to the loading sufficient for half-and complete-filling of the D4R units, reflect these average trends with germanium filling the whole S4R unit (in D4R) and a whole D4R unit, respectively. However as indicated by the average occupation values, besides these global minima, there are multiple distributions very close in energy (e.g., within 10 kJ/mol from GSO -see SI Figures , in which either germanium assumes a different distribution within the D4R or/and some of it spills over to adjacent and framework sites. The spillover germanium atoms tend to cluster, which is most pronounced for the samples with very high germanium content (see SI Figure ), i.e., above the least amount sufficient to fill the D4R unit.