Yin XWang YTZU-HSUAN CHANGZhang PLi JXue PLong YShohet J.LVoyles P.MMa ZWang X.2023-06-092023-06-0920209359648https://www.scopus.com/inward/record.uri?eid=2-s2.0-85083738818&doi=10.1002%2fadma.202000801&partnerID=40&md5=6afde5ee79008b988f2759386d8ba3c8https://scholars.lib.ntu.edu.tw/handle/123456789/632300The emergence of memristive behavior in amorphous–crystalline 2D oxide heterostructures, which are synthesized by atomic layer deposition (ALD) of a few-nanometer amorphous Al2O3 layers onto atomically thin single-crystalline ZnO nanosheets, is demonstrated. The conduction mechanism is identified based on classic oxygen vacancy conductive channels. ZnO nanosheets provide a 2D host for oxygen vacancies, while the amorphous Al2O3 facilitates the generation and stabilization of the oxygen vacancies. The conduction mechanism in the high-resistance state follows Poole–Frenkel emission, and in the the low-resistance state is fitted by the Mott–Gurney law. From the slope of the fitting curve, the mobility in the low-resistance state is estimated to be ≈2400 cm2 V−1 s−1, which is the highest value reported in semiconductor oxides. When annealed at high temperature to eliminate oxygen vacancies, Al is doped into the ZnO nanosheet, and the memristive behavior disappears, further confirming the oxygen vacancies as being responsible for the memristive behavior. The 2D heterointerface offers opportunities for new design of high-performance memristor devices. © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim2D heterostructures; atomic layer deposition; memristors; oxygen vacancies; zinc oxideAlumina; Aluminum oxide; Atomic layer deposition; Curve fitting; Heterojunctions; II-VI semiconductors; Nanosheets; Wide band gap semiconductors; Zinc oxide; Conduction Mechanism; Conductive channels; High-resistance state; Low-resistance state; Memristive behavior; Oxide heterostructures; Semiconductor oxides; Single-crystalline; Oxygen vacanciesjournal article10.1002/adma.202000801323191532-s2.0-85083738818