We report the effects of screening capacity, surface roughness, and interfacial epitaxy of the bottom electrodes on the polarization switching, domain wall (DW) roughness, and ferroelectric Curie temperature (TC) of PbZr0.2Ti0.8O3 (PZT)-based free-standing membranes. Singe crystalline 10−50 nm (001) PZT and PZT/La0.67Sr0.33MnO3 (LSMO) membranes are prepared on Au, correlated oxide LSMO, and two-dimensional (2D) semiconductor MoS2 base layers. Switching the polarization of PZT yields nonvolatile current modulation in the MoS2 channel at room temperature, with an on/off ratio of up to 2 × 105 and no apparent decay for more than 3 days. Piezoresponse force microscopy studies show that the coercive field Ec for the PZT membranes varies from 0.75 to 3.0 MV cm-1 on different base layers and exhibits strong polarization asymmetry. The PZT/LSMO membranes exhibit significantly smaller Ec, with the samples transferred on LSMO showing symmetric Ec of about −0.26/+0.28 MV cm-1, smaller than that of epitaxial PZT films. The DW roughness exponent ζ points to 2D random bond disorder dominated DW roughening (ζ = 0.31) at room temperature. Upon thermal quench at progressively higher temperatures, ζ values for PZT membranes on Au and LSMO approach the theoretical value for 1D random bond disorder (ζ = 2/3), while samples on MoS2 exhibits thermal roughening (ζ = 1/2). The PZT membranes on Au, LSMO, and MoS2 show TC of about 763 ± 12, 725 ± 25, and 588 ± 12 °C, respectively, well exceeding the bulk value. Our study reveals the complex interplay between the electrostatic and mechanical boundary conditions in determining ferroelectricity in free-standing PZT membranes, providing important material parameters for the functional design of PZT-based flexible nanoelectronics.
more »
« less
Ferroelectric Control of Anisotropic Magnetoresistance in Ultrathin Sr 2 IrO 4 Films toward 2D Metallic Limit
Abstract The Ruddlesden‐Popper 5diridate Sr2IrO4is an antiferromagnetic Mott insulator with the electronic, magnetic, and structural properties highly intertwined. Voltage control of its magnetic state is of intense fundmenatal and technological interest but remains to be demonstrated. Here, the tuning of magnetotransport properties in 5.2 nm Sr2IrO4via interfacial ferroelectric PbZr0.2Ti0.8O3is reported. The conductance of the epitaxial PbZr0.2Ti0.8O3/Sr2IrO4heterostructure exhibits ln(T) behavior that is characteristic of 2D correlated metal, in sharp contrast to the thermally activated behavior followed by 3D variable range hopping observed in single‐layer Sr2IrO4films. Switching PbZr0.2Ti0.8O3polarization induces nonvolatile, reversible resistance modulation in Sr2IrO4. At low temperatures, the in‐plane magnetoresisance in the heterostructure transitions from positive to negative at high magnetic fields, opposite to the field dependence in single‐layer Sr2IrO4. In the polarization down state, the out‐of‐plane anisotropic magnetoresistanceRAMRexhibits sinusoidal angular dependence, with a 90° phase shift below 20 K. For the polarization up state, unusual multi‐level resistance pinning appears inRAMRbelow 30 K, pointing to enhanced magnetocrystalline anisotropy. The work sheds new light on the intriguing interplay of interface lattice coupling, charge doping, magnetoelastic effect, and possible incipient ferromagnetism in Sr2IrO4, facilitating the functional design of its electronic and material properties.
more »
« less
- Award ID(s):
- 2044049
- PAR ID:
- 10636333
- Publisher / Repository:
- Advanced Physics Research
- Date Published:
- Journal Name:
- Advanced Physics Research
- Volume:
- 4
- Issue:
- 8
- ISSN:
- 2751-1200
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
The significant role of perovskite defect chemistry through A-site doping of strontium titanate with lanthanum for CO 2 electrolysis properties is demonstrated. Here we present a dual strategy of A-site deficiency and promoting adsorption/activation by making use of redox active dopants such as Mn/Cr linked to oxygen vacancies to facilitate CO 2 reduction at perovskite titanate cathode surfaces. Solid oxide electrolysers based on oxygen-excess La 0.2 Sr 0.8 Ti 0.9 Mn(Cr) 0.1 O 3+δ , A-site deficient (La 0.2 Sr 0.8 ) 0.9 Ti 0.9 Mn(Cr) 0.1 O 3−δ and undoped La 0.2 Sr 0.8 Ti 1.0 O 3+δ cathodes are evaluated. In situ infrared spectroscopy reveals that the adsorbed and activated CO 2 adopts an intermediate chemical state between a carbon dioxide molecule and a carbonate ion. The double strategy leads to optimal performance being observed after 100 h of high-temperature operation and 3 redox cycles, suggesting a promising cathode material for CO 2 electrolysis.more » « less
-
The 5drare Earth iridate is an intriguing material with exhibiting exotic electronic and magnetic phases due to spin‐orbit coupled states. Ternary iridium oxidesLn3IrO7contain an unusual Ir5+(5d4) system, which remain a subject of active research. Fabricating epitaxialLn3IrO7films is challenging due to substrate compatibility, but it offers a valuable platform to explore electronic and magnetic behaviors under reduced dimensionality and substrate interactions, revealing novel phenomena based on Ir5+(5d4). In this regard, this demonstrates that Pr3IrO7with its highly anisotropic orthorhombic structure can be epitaxially grown on a cubic (111)‐oriented yttrium‐stabilized ZrO2(YSZ) substrate. Pr3IrO7film exhibits six epitaxial domains, where the (220) and (202) planes aligning epitaxially to YSZ (111) with the threefold symmetry. This diverse domain configuration in Pr3IrO7film leads to unique magnetic properties, exhibiting spin‐glass‐like behavior. Pr3IrO7thin film offers a platform for exploring unconventional magnetic states, and their successful heteroepitaxy on YSZ substrates opens new avenues for discovering novel physical phenomena.more » « less
-
Abstract The superior size and power scaling potential of ferroelectric-gated Mott transistors makes them promising building blocks for developing energy-efficient memory and logic applications in the post-Moore’s Law era. The close to metallic carrier density in the Mott channel, however, imposes the bottleneck for achieving substantial field effect modulation via a solid-state gate. Previous studies have focused on optimizing the thickness, charge mobility, and carrier density of single-layer correlated channels, which have only led to moderate resistance switching at room temperature. Here, we report a record high nonvolatile resistance switching ratio of 38,440% at 300 K in a prototype Mott transistor consisting of a ferroelectric PbZr0.2Ti0.8O3 gate and an RNiO3(R: rare earth)/La0.67Sr0.33MnO3 composite channel. The ultrathin La0.67Sr0.33MnO3 buffer layer not only tailors the carrier density profile in RNiO3 through interfacial charge transfer, as corroborated by first-principles calculations, but also provides an extended screening layer that reduces the depolarization effect in the ferroelectric gate. Our study points to an effective material strategy for the functional design of complex oxide heterointerfaces that harnesses the competing roles of charge in field effect screening and ferroelectric depolarization effects.more » « less
-
null (Ed.)Sr(Ti 0.3 Fe 0.7 )O 3−δ (STF) and the associated exsolution electrodes Sr 0.95 (Ti 0.3 Fe 0.63 Ru 0.07 )O 3−δ (STFR), or Sr 0.95 (Ti 0.3 Fe 0.63 Ni 0.07 )O 3−δ (STFN) are alternatives to Ni-based cermet fuel electrodes for solid oxide electrochemical cells (SOCs). They can provide improved tolerance to redox cycling and fuel impurities, and may allow direct operation with hydrocarbon fuels. However, such perovskite-oxide-based electrodes present processing challenges for co-sintering with thin electrolytes to make fuel electrode supported SOCs. Thus, they have been mostly limited to electrolyte-supported SOCs. Here, we report the first example of the application of perovskite oxide fuel electrodes in novel oxygen electrode supported SOCs (OESCs) with thin YSZ electrolytes, and demonstrate their excellent performance. The OESCs have La 0.8 Sr 0.2 MnO 3−δ –Zr 0.92 Y 0.16 O 2−δ (LSM–YSZ) oxygen electrode-supports that are enhanced via infiltration of SrTi 0.3 Fe 0.6 Co 0.1 O 3−δ , while the fuel electrodes are either Ni-YSZ, STF, STFN, or STFR. Fuel cell power density as high as 1.12 W cm −2 is obtained at 0.7 V and 800 °C in humidified hydrogen and air with the STFR electrode, 60% higher than the same cell made with a Ni-YSZ electrode. Electrolysis current density as high as −1.72 A cm −2 is obtained at 1.3 V and 800 °C in 50% H 2 O to 50% H 2 mode; the STFR cell yields a value 72% higher than the same cell made with a Ni-YSZ electrode, and competitive with the widely used conventional Ni-YSZ-supported cells. The high performance is due in part to the low resistance of the thin YSZ electrolyte, and also to the low fuel electrode polarization resistance, which decreases with fuel electrode in the order: Ni-YSZ > STF > STFN > STFR. The high performance of the latter two electrodes is due to exsolution of catalytic metal nanoparticles; the results are discussed in terms of the microstructure and properties of each electrode material, and surface oxygen exchange resistance values are obtained over a range of conditions for STF, STFN, and STFN. The STF fuel electrodes also provide good stability during redox cycling.more » « less
An official website of the United States government

