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While phase-change materials (PCMs) composed of chalcogenide have differentcrystallization mechanisms (CM), such as nucleation-dominated Ge2Sb2Te5 (GST)and growth-dominated GeTe (GT), revealing the essential reason of CM as well asthe tuned properties is still a long-standing issue. Here, we remarkably findthe distinct stability of Te-terminated (111) boundaries (TTB) in differentsystems, which provides a path to understand the difference in CM. It stemsfrom the quantum effect of molecular orbital theory: the optimal local chemicalcomposition results in the formation of TTB without dangling bonds (DB) in GSTbut with DB in GT, where DB destabilizes boundary due to its distorted localenvironment mismatching Oh symmetry of p orbitals. Moreover, the inner vacancyconcentration in GST is alterable and controlled by TTB, manifested by theabsence of cubic-to-hexagonal transition in carbon-doped GST of small grainsand minimized inner vacancy. Finally, the charge transport property (CTP) iscontrolled by boundary via changing the density of charge or hole nearby aswell as vacancy. These findings open the door to tune CTP by CM, which isnecessary for achieving low-power and ultrafast devices.

Crystallization Mechanism Tuned Phase-Change Materials: Quantum Effect on Te-Terminated Boundary