No abstract

Controlling crystalline phases in polymorphic materials is critical not only for the fundamental understanding of the physics of phase formation but also for the technological application of forbidden, but potentially useful physical properties of the nominally unstable phases. Here, using tin oxide (SnO 2 ) as a model system, we demonstrate a new way to enhance the mechanical hardness of an oxide by stabilizing a highpressure dense phase through nitrogen integration in the oxide. Pristine SnO 2 has a tetragonal structure at the ambient pressure, and undergoes phase transitions to orthorhombic and cubic phases with increasing pressure. Leveraging the enhanced reactivity of nitrogen in plasma, we are able to synthesize tin oxynitride (SnON) thin films with a cubic phase same as the high-pressure phase of SnO 2 . Such nitrogen-stabilized cubic SnON films exhibit a mechanical hardness of ∼23 ± 4 GPa, significantly higher than even the nitride counterpart (Sn 3 N 4 ) as the result of the shortened atomic distance of the denser, high-pressure cubic phase. Moreover, SnON has a heavily doped, n-type semiconducting property with a controllable optical bandgap. Our work will provide new opportunities to search for and to utilize beneficial, but hidden physical properties that exist in a particular phase stable only at extreme conditions.

Manipulation of electrons in a solid through transmitting, storing, and switching is the fundamental basis for the microelectronic devices. Recently, the electroresistance effect in the ferroelectric capacitors has provided a novel way to modulate the electron transport by polarization reversal. Here, we demonstrate a giant electroresistive ferroelectric diode integrating a ferroelectric capacitor into two-dimensional electron gas (2DEG) at oxide interface. As a model system, we fabricate an epitaxial Au/Pb(Zr0.2Ti0.8)O3/LaAlO3/SrTiO3 heterostructure, where 2DEG is formed at LaAlO3/SrTiO3 interface. This device functions as a two-terminal, non-volatile memory of 1 diode-1 resistor with a large I+/I− ratio (>108 at ±6 V) and Ion/Ioff ratio (>107). This is attributed to not only Schottky barrier modulation at metal/ferroelectric interface by polarization reversal but also the field-effect metal-insulator transition of 2DEG. Moreover, using this heterostructure, we can demonstrate a memristive behavior for an artificial synapse memory, where the resistance can be continuously tuned by partial polarization switching, and the electrons are only unidirectionally transmitted. Beyond non-volatile memory and logic devices, our results will provide new opportunities to emerging electronic devices such as multifunctional nanoelectronics and neuromorphic electronics.

Two-dimensional electron gas (2DEG) at the complex oxide interfaces have brought about considerable interest for the application of the next-generation multifunctional oxide electronics due to the exotic properties that do not exist in the bulk. In this study, we report the integration of 2DEG into the nonvolatile resistance switching cell as a bottom electrode, where the metal-insulator transition of 2DEG by an external field serves to significantly reduce the OFF-state leakage current while enhancing the on/off ratio. Using the Pt/Ta2O5-y/Ta2O5-x/SrTiO3 heterostructure as a model system, we demonstrate the nonvolatile resistance switching memory cell with a large on/off ratio (>10(6)) and a low leakage current at the OFF state (∼10(-13) A). Beyond exploring nonvolatile memory, our work also provides an excellent framework for exploring the fundamental understanding of novel physics in which electronic and ionic processes are coupled in the complex heterostructures.