Weiming Lü

Highly Active Epitaxial La(1-x)Sr(x)MnO3 Surfaces for the Oxygen Reduction Reaction: Role of Charge Transfer.

Most studies of oxide catalysts for the oxygen reduction reaction (ORR) use oxide powder, where the heterogeneity of exposed surfaces and the composite nature of electrodes limit fundamental understanding of the reaction mechanism. We present the ORR activity of epitaxially oriented La(1-x)Sr(x)MnO3 surfaces and investigate, by varying Sr substitution, the relationship between the role of charge transfer and catalytic activity in an alkaline environment. The activity is greatest for La(1-x)Sr(x)MnO3 with 33% Sr, containing mixed Mn(3+/4+), and the (110) and (111) orientations display comparable activities to that of the (001). Electrochemical measurements using the facile redox couple [Fe(CN)6](3-/4-) illustrate that increasing ORR activity trends with faster charge-transfer kinetics, indicating the importance of facile charge transfer at the oxide/water interface and mixed Mn valence in promoting ORR kinetics.

Ultrathin BaTiO3-Based Ferroelectric Tunnel Junctions through Interface Engineering

The ability to change states using voltage in ferroelectric tunnel junctions (FTJs) offers a route for lowering the switching energy of memories. Enhanced tunneling electroresistance in FTJ can be achieved by asymmetric electrodes or introducing metal-insulator transition interlayers. However, a fundamental understanding of the role of each interface in a FTJ is lacking and compatibility with integrated circuits has not been explored adequately. Here, we report an incisive study of FTJ performance with varying asymmetry of the electrode/ferroelectric interfaces. Surprisingly high TER (∼400%) can be achieved at BaTiO3 layer thicknesses down to two unit cells (∼0.8 nm). Further our results prove that band offsets at each interface in the FTJs control the TER ratio. It is found that the off state resistance (R(Off)) increases much more rapidly with the number of interfaces compared to the on state resistance (ROn). These results are promising for future low energy memories.

Liquid-Gated High Mobility and Quantum Oscillation of the Two-Dimensional Electron Gas at an Oxide Interface

Electric field effect in electronic double layer transistor (EDLT) configuration with ionic liquids as the dielectric materials is a powerful means of exploring various properties in different materials. Here, we demonstrate the modulation of electrical transport properties and extremely high mobility of two-dimensional electron gas at LaAlO3/SrTiO3 (LAO/STO) interface through ionic liquid-assisted electric field effect. With a change of the gate voltages, the depletion of charge carrier and the resultant enhancement of electron mobility up to 19 380 cm(2)/(V s) are realized, leading to quantum oscillations of the conductivity at the LAO/STO interface. The present results suggest that high-mobility oxide interfaces, which exhibit quantum phenomena, could be obtained by ionic liquid-assisted field effect.

The Effect of Polar Fluctuation and Lattice Mismatch on Carrier Mobility at Oxide Interfaces

Since the discovery of two-dimensional electron gas (2DEG) at the oxide interface of LaAlO3/SrTiO3 (LAO/STO), improving carrier mobility has become an important issue for device applications. In this paper, by using an alternate polar perovskite insulator (La0.3Sr0.7) (Al0.65Ta0.35)O3 (LSAT) for reducing lattice mismatch from 3.0% to 1.0%, the low-temperature carrier mobility has been increased 30 fold to 35,000 cm(2) V(-1) s(-1). Moreover, two critical thicknesses for the LSAT/STO (001) interface are found, one at 5 unit cells for appearance of the 2DEG and the other at 12 unit cells for a peak in the carrier mobility. By contrast, the conducting (110) and (111) LSAT/STO interfaces only show a single critical thickness of 8 unit cells. This can be explained in terms of polar fluctuation arising from LSAT chemical composition. In addition to lattice mismatch and crystal symmetry at the interface, polar fluctuation arising from composition has been identified as an important variable to be tailored at the oxide interfaces to optimize the 2DEG transport.

Multi‐Nonvolatile State Resistive Switching Arising from Ferroelectricity and Oxygen Vacancy Migration

Resistive switching phenomena form the basis of competing memory technologies. Among them, resistive switching, originating from oxygen vacancy migration (OVM), and ferroelectric switching offer two promising approaches. OVM in oxide films/heterostructures can exhibit high/low resistive state via conducting filament forming/deforming, while the resistive switching of ferroelectric tunnel junctions (FTJs) arises from barrier height or width variation while ferroelectric polarization reverses between asymmetric electrodes. Here the authors demonstrate a coexistence of OVM and ferroelectric induced resistive switching in a BaTiO3 FTJ by comparing BaTiO3 with SrTiO3 based tunnel junctions. This coexistence results in two distinguishable loops with multi-nonvolatile resistive states. The primary loop originates from the ferroelectric switching. The second loop emerges at a voltage close to the SrTiO3 switching voltage, showing OVM being its origin. BaTiO3 based devices with controlled oxygen vacancies enable us to combine the benefits of both OVM and ferroelectric tunneling to produce multistate nonvolatile memory devices.

Tailoring the Two Dimensional Electron Gas at Polar ABO3/SrTiO3 Interfaces for Oxide Electronics.

The 2D electron gas at the polar/non-polar oxide interface has become an important platform for several novel oxide electronic devices. In this paper, the transport properties of a wide range of polar perovskite oxide ABO3/SrTiO3 (STO) interfaces, where ABO3 includes LaAlO3, PrAlO3, NdAlO3, NdGaO3 and LaGaO3 in both crystalline and amorphous forms, were investigated. A robust 4 unit cell (uc) critical thickness for metal insulator transition was observed for crystalline polar layer/STO interface while the critical thickness for amorphous ones was strongly dependent on the B site atom and its oxygen affinity. For the crystalline interfaces, a sharp transition to the metallic state (i.e. polarization catastrophe induced 2D electron gas only) occurs at a growth temperature of 515 °C which corresponds to a critical relative crystallinity of ~70 ± 10% of the LaAlO3 overlayer. This temperature is generally lower than the metal silicide formation temperature and thus offers a route to integrate oxide heterojunction based devices on silicon.

Tetragonal (K, Na)NbO3 based lead-free single crystal: Growth, full tensor properties, and their orientation dependence

A Li and Ta modified (K, Na)NbO3 lead-free single crystal with a large size (13 × 10 × 20 mm3) has been grown by using the top-seeded solution growth method. The large size allows us to carry out an extensive study on this tetragonal crystal. We have measured a complete set of elastic, dielectric, and piezoelectric constants for the [001]C poled crystal with the single domain state. The crystal exhibits high shear piezoelectricity with d15 = 518 pC/N and k15 = 0.733, showing excellent potential in shear electro-sonic energy transformation devices. It is found that the high shear piezoelectricity originates from the vicinity of orthorhombic-tetragonal phase transition, which favors polarization rotation greatly. The orientation dependence of longitudinal dielectric, piezoelectric, and elastic constants and electromechanical coupling factor in the 3-dimentional space were calculated based on the single domain dataset. We believe that this work is of great importance for both fundamental studies and device d...

Dynamic scaling of internal bias field in Mn-doped 0.24Pb(In 1/2 Nb 1/2 )O 3 –0.42Pb(Mg 1/3 Nb 2/3 )O 3 –0.34PbTiO 3 ferroelectric ceramic

The influences of temperature, electric field, and frequency on the internal bias field Ei have been investigated in poled and aged Mn-doped 0.24Pb(In1/2Nb1/2)O3–0.42Pb(Mg1/3Nb2/3)O3–0.34PbTiO3 ferroelectric ceramic. It was found that Ei decreases with temperature T and electric field amplitude E0, but increases with frequency f. The relaxation behavior of the internal bias field is related to the redistribution of preferentially oriented defect dipoles. Based on our results, scaling relations of Ei on temperature, electric field, and frequency were established in both rhombohedral and tetragonal phases, which provide the foundation for making “harder” piezoelectric materials through point defect engineering in order to meet the demand of high-power piezoelectric device applications.

Temperature dependent piezoelectric anisotropy in tetragonal 0.63Pb(Mg1/3Nb2/3)-0.37PbTiO3 single crystal

In this work, we studied the temperature-dependent effective piezoelectric coefficient d 33 * along the arbitrary direction of a tetragonal 0.63Pb(Mg1/3Nb2/3)-0.37PbTiO3 single crystal. Results show that the crystal changes from a rotator ferroelectrics with the maximum d 33 * occurring along the nonpolar direction to a extender type with maximum piezoelectricity along [001]C. Two polymorphic phase transitions, orthorhombic-tetragonal and tetragonal-cubic, greatly influence the PS dynamics, leading to the change of d 33 * anisotropy with temperature. The [011]C oriented crystals possess both improved piezoelectricity and high thermal stability, hence are the best choice for practical applications.In this work, we studied the temperature-dependent effective piezoelectric coefficient d 33 * along the arbitrary direction of a tetragonal 0.63Pb(Mg1/3Nb2/3)-0.37PbTiO3 single crystal. Results show that the crystal changes from a rotator ferroelectrics with the maximum d 33 * occurring along the nonpolar direction to a extender type with maximum piezoelectricity along [001]C. Two polymorphic phase transitions, orthorhombic-tetragonal and tetragonal-cubic, greatly influence the PS dynamics, leading to the change of d 33 * anisotropy with temperature. The [011]C oriented crystals possess both improved piezoelectricity and high thermal stability, hence are the best choice for practical applications.

Origin and Quenching of Novel ultraviolet and blue emission in NdGaO3: Concept of Super-Hydrogenic Dopants

In this study we report the existence of novel ultraviolet (UV) and blue emission in rare-earth based perovskite NdGaO3 (NGO) and the systematic quench of the NGO photoluminescence (PL) by Ce doping. Study of room temperature PL was performed in both single-crystal and polycrystalline NGO (substrates and pellets) respectively. Several NGO pellets were prepared with varying Ce concentration and their room temperature PL was studied using 325 nm laser. It was found that the PL intensity shows a systematic quench with increasing Ce concentration. XPS measurements indicated that nearly 50% of Ce atoms are in the 4+ state. The PL quench was attributed to the novel concept of super hydrogenic dopant (SHD)”, where each Ce4+ ion contributes an electron which forms a super hydrogenic atom with an enhanced Bohr radius, due to the large dielectric constant of the host. Based on the critical Ce concentration for complete quenching this SHD radius was estimated to be within a range of 0.85 nm and 1.15 nm whereas the predicted theoretical value of SHD radius for NdGaO3 is ~1.01 nm.