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Crystalline GeSb 2 Te 4  (GST) is a remarkable material, as it allows to continuously tune the electrical resistance by orders of magnitude without involving a structural phase transition or stoichiometric changes. While well‐ordered specimen are metallic, increasing amounts of disorder eventually lead to an insulating state with vanishing conductivity in the 0 K limit, but a similar number of charge carriers. Hence, GST provides ideal grounds to explore the impact of disorder on transport properties. Here, a sputter‐deposition process is employed that enables growing biaxially textured GST films with large grain sizes on mica substrates. The resulting films exhibit a systematic variation between metallic and truly insulating specimen upon varying deposition temperature. Transport measurements reveal that their electron mean free path can be altered by a factor of 20, while always remaining more than an order of magnitude smaller than the lateral grain size. This proves unequivocally that grain boundaries play a negligible role for electron scattering, while intra‐grain scattering, presumably by disordered vacancies, dominates. These findings underline that the insulating state and the system's evolution toward metallic conductivity are intrinsic properties of the material.

Disorder Control in Crystalline GeSb 2 Te 4 and its Impact on Characteristic Length Scales