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Deepening the understanding of interface-type resistive switching (RS) in metal/oxide heterojunctions is a key step for the development of high-performance memristors and Schottky rectifiers. In this study, we address the role of metallization technique by fabricating prototypical metal/Nb-doped SrTiO3 (M/NSTO) Schottky contacts via pulsed laser deposition (PLD). Ultrathin Pt and Au electrodes are deposited by PLD onto single-crystal (001)-terminated NSTO substrates and interfacial transport is characterized by conventional macroscale methods and nanoscale Ballistic Electron Emission Microscopy. We show that PLD metallization gives Schottky contacts with highly reversible current-voltage characteristics under cyclic polarization. Room-temperature (RT) transport is governed by thermionic emission with Schottky barrier height ϕ B ( Pt / NSTO ) ∼ 0.71 − 0.75 eV , ϕ B ( Au / NSTO ) ∼ 0.70 − 0.83 eV and ideality factors as small as n ( Pt / NSTO ) ∼ 1.1 and n ( Au / NSTO ) ∼ 1.6 . RS remains almost completely suppressed upon imposing broad variations of the Nb doping and of the external stimuli (polarization bias, working temperature, ambient air exposure). At the nanoscale, we find that both systems display high spatial homogeneity of ϕ B ( ⩽ 50 meV ), which is only partially affected by the NSTO mixed termination ( | ϕ B ( M / SrO ) − ϕ B ( M / Ti O 2 ) | < 35 meV ). Experimental evidences and theoretical arguments—based on a metal-insulator-semiconductor description of the M/NSTO—indicate that the PLD metallization mitigates interfacial layer effects responsible for RS. This occurs thanks to the reduction of the interfacial layer thickness and to the creation of an effective barrier against the permeation of ambient gas species affecting charge trapping and redox reactions. This description allows to rationalize interfacial aging effects, observed upon several-months-exposure to ambient air, in terms of a slow interfacial re-oxidation. Our work contributes to the fundamental understanding of interface-type RS and demonstrates that RT PLD offers a viable platform for the realization of robust, RS-free NSTO-based Schottky contacts.
Deepening the understanding of interface-type resistive switching (RS) in metal/oxide heterojunctions is a key step for the development of high-performance memristors and Schottky rectifiers. In this study, we address the role of metallization technique by fabricating prototypical metal/Nb-doped SrTiO3 (M/NSTO) Schottky contacts via pulsed laser deposition (PLD). Ultrathin Pt and Au electrodes are deposited by PLD onto single-crystal (001)-terminated NSTO substrates and interfacial transport is characterized by conventional macroscale methods and nanoscale Ballistic Electron Emission Microscopy. We show that PLD metallization gives Schottky contacts with highly reversible current-voltage characteristics under cyclic polarization. Room-temperature (RT) transport is governed by thermionic emission with Schottky barrier height ϕ B ( Pt / NSTO ) ∼ 0.71 − 0.75 eV , ϕ B ( Au / NSTO ) ∼ 0.70 − 0.83 eV and ideality factors as small as n ( Pt / NSTO ) ∼ 1.1 and n ( Au / NSTO ) ∼ 1.6 . RS remains almost completely suppressed upon imposing broad variations of the Nb doping and of the external stimuli (polarization bias, working temperature, ambient air exposure). At the nanoscale, we find that both systems display high spatial homogeneity of ϕ B ( ⩽ 50 meV ), which is only partially affected by the NSTO mixed termination ( | ϕ B ( M / SrO ) − ϕ B ( M / Ti O 2 ) | < 35 meV ). Experimental evidences and theoretical arguments—based on a metal-insulator-semiconductor description of the M/NSTO—indicate that the PLD metallization mitigates interfacial layer effects responsible for RS. This occurs thanks to the reduction of the interfacial layer thickness and to the creation of an effective barrier against the permeation of ambient gas species affecting charge trapping and redox reactions. This description allows to rationalize interfacial aging effects, observed upon several-months-exposure to ambient air, in terms of a slow interfacial re-oxidation. Our work contributes to the fundamental understanding of interface-type RS and demonstrates that RT PLD offers a viable platform for the realization of robust, RS-free NSTO-based Schottky contacts.
Ag/Nb:SrTiO3(NSTO)/Ag and Au/NSTO/Ag structures were prepared and their current–voltage curves were studied in detail. The Ag/NSTO/Ag structure can demonstrate a pronounced resistive switching effect and the characteristics of its resistance change sequence as demonstrated in the I–V curves are significantly different from those of the Au/NSTO/Ag structure. Under a unipolar current, the Ag/NSTO/Ag structure translates first from a low-resistance state (LRS) to a high-resistance state (HRS) and then from the HRS to the LRS. However, the Au/NSTO/Ag structure only shows a transition from the HRS to the LRS. The phenomenon is analyzed taking into account the migration of oxygen ions and the electrochemical reaction of the Ag electrode, which lead to the formation of the Ag2O insulation layer as well as Ag conductive filaments in the Ag/NSTO/Ag structure and a change in the barrier height of the Au/NSTO interface.
A barrier-type resistive switching (RS) unit, composed of a metal and Nb:SrTiO3 (NSTO), holds significant potential for data storage applications due to its high storage density, low operating voltage, and excellent stability. While extensive research has been conducted on conductive oxides (COs), there has been relatively less focus on the RS properties of heterogeneous structures combing CO electrodes and NSTO. Epitaxial growth of CO on NSTO is expected to yield devices with enhanced stability and repeatability. This study explores the RS characteristics of La0.8Ca0.2MnO3 (LCMO)/NSTO heterostructures through epitaxy of both conventional and anoxic LCMO films on (00 l)-oriented NSTO single crystal substrates. The results reveal that the conventional LCMO/NSTO structure exhibits a conventional counterclockwise bipolar RS (BRS) effect, while the anoxic LCMO/NSTO heterostructure demonstrates a unique clockwise (CW) BRS effect (exhibiting different RS characteristics under different applied voltages). The study concludes that the CW-BRS effect mechanism is attributed to a high concentration of oxygen vacancies (Vo) in LCMO. Under different external electric fields, Vo in LCMO and NSTO migrate to the LCMO/NSTO interface, respectively, leading to multiple changes in the interface barrier. These findings offer valuable experimental insights for utilizing CO in the field of RS applications.
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