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A design concept of phase-separated amorphous nanocomposite thin films is presented which realizes interfacial resistive switching (RS) in hafnium-oxide-based devices. The films are formed by incorporating an average of 7% Ba into hafnium oxide during pulsed laser deposition at temperatures ≤400 °C. The added Ba prevents the films from crystallizing and leads to ∼20-nm-thin films consisting of an amorphous HfOx host matrix interspersed with ∼2-nmwide, ∼5-to-10-nm-pitch Ba-rich amorphous nanocolumns penetrating ∼2/3 through the films. This restricts the RS to an interfacial Schottky-like energy barrier whose magnitude is tuned by ionic migration under an applied electric field. Resulting devices achieve stable cycle-to-cycle, device-to-device, and sample-to-sample reproducibility with a measured switching endurance of ≥10⁴ cycles for a memory window ≥10 at switching voltages of ±2 V. Each device can be set to multiple intermediate resistance states, which enables synaptic spike-timing-dependent plasticity. The presented concept unlocks additional design variables for RS devices.

Micro-solid oxide fuel cells based on thin films have strong potential for use in portable power devices. However, devices based on silicon substrates typically involve thin-film metallic electrodes which are unstable at high temperatures. Devices based on bulk metal substrates overcome these limitations, though performance is hindered by the challenge of growing state-of-the-art epitaxial materials on metals. Here, we demonstrate for the first time the growth of epitaxial cathode materials on metal substrates (stainless steel) commercially supplied with epitaxial electrolyte layers (1.5 {um (Y2O3)0.15(ZrO2)0.85 (YSZ) + 50 nm CeO2). We create epitaxial mesoporous cathodes of (La0.60Sr0.40)0.95Co0.20Fe0.80O3 (LSCF) on the substrate by growing LSCF/MgO vertically aligned nanocomposite films by pulsed laser deposition, followed by selectively etching out the MgO. To enable valid comparison with the literature, the cathodes are also grown on single-crystal substrates, confirming state-of-the-art performance with an area specific resistance of 100ohmegacm2 at 500dC and activation energy down to 0.97 eV. The work marks an important step toward the commercialization of high-performance micro-solid oxide fuel cells for portable power applications.

Negative pressure has emerged as a powerful tool to tailor the physical properties of functional materials. However, a negative pressure control of spin-phonon coupling for engineering magnetism and multiferroicity has not been explored to date. Here, using uniform three-dimensional strain-induced negative pressure in nanocomposite films of (EuTiO3)0.5:(MgO)0.5, we demonstrate an emergent multiferroicity with magnetodielectric coupling in EuTiO3, matching exactly with density functional theory calculations. Density functional theory calculations are further used to explore the underlying physics of antiferromagnetic-paraelectric to ferromagnetic-ferroelectric phase transitions, the spin-phonon coupling, and its correlation with negative pressures. The observation of magnetodielectric coupling in the EuTiO3 reveals that an enhanced spin-phonon coupling originates from a negative pressure induced by uniform three-dimensional strain. Our work provides a route to creating multiferroicity and magnetoelectric coupling in single-phase oxides using a negative pressure approach.

Orthorhombic RMnO3 (R = rare-earth cation) compounds are type-II multiferroics induced by inversion-symmetry-breaking of spin order. They hold promise for magneto-electric devices. However, no spontaneous room-temperature ferroic property has been observed to date in orthorhombic RMnO3. Here, using 3D straining in nanocomposite films of (SmMnO3)0.5((Bi,Sm)2O3)0.5, we demonstrate room temperature ferroelectricity and ferromagnetism with TC,FM ~ 90 K, matching exactly with theoretical predictions for the induced strain levels. Large in-plane compressive and out-of-plane tensile strains (−3.6% and +4.9%, respectively) were induced by the stiff (Bi,Sm)2O3 nanopillars embedded. The room temperature electric polarization is comparable to other spin-driven ferroelectric RMnO3 films. Also, while bulk SmMnO3 is antiferromagnetic, ferromagnetism was induced in the composite films. The Mn-O bond angles and lengths determined from density functional theory explain the origin of the ferroelectricity, i.e. modification of the exchange coupling. Our structural tuning method gives a route to designing multiferroics.

High-performance p-type oxide thin film transistors (TFTs) have great potential for many semiconductor applications. However, these devices typically suffer from low hole mobility and high off-state currents. We fabricated p-type TFTs with a phase-pure polycrystalline Cu2O semiconductor channel grown by atomic layer deposition (ALD). The TFT switching characteristics were improved by applying a thin ALD Al2O3 passivation layer on the Cu2O channel, followed by vacuum annealing at 300 C. Detailed characterisation by TEM-EDX and XPS shows that the surface of Cu2O is reduced following Al2O3 deposition and indicates the formation of 1-2 nm thick CuAlO2 interfacial layer. This, together with field-effect passivation caused by the high negative fixed charge of the ALD Al2O3, leads to an improvement in the TFT performance by reducing the density of deep trap states as well as by reducing the accumulation of electrons in the semiconducting layer in the device off-state., Comment: 25 pages, 6 figures, full paper

Orthorhombic RMnO3 (R = rare-earth cation) compounds are type-II multiferroics induced by inversion-symmetry-breaking of spin order. They hold promise for magneto-electric devices. However, no spontaneous room-temperature ferroic property has been observed to date in orthorhombic RMnO3. Here, using 3D straining in nanocomposite films of (SmMnO3)0.5((Bi,Sm)2O3)0.5, we demonstrate room temperature ferroelectricity and ferromagnetism with TC,FM ~ 90 K, matching exactly with theoretical predictions for the induced strain levels. Large in-plane compressive and out-of-plane tensile strains (−3.6% and +4.9%, respectively) were induced by the stiff (Bi,Sm)2O3 nanopillars embedded. The room temperature electric polarization is comparable to other spin-driven ferroelectric RMnO3 films. Also, while bulk SmMnO3 is antiferromagnetic, ferromagnetism was induced in the composite films. The Mn-O bond angles and lengths determined from density functional theory explain the origin of the ferroelectricity, i.e. modification of the exchange coupling. Our structural tuning method gives a route to designing multiferroics., Multiferroic materials exhibiting ferromagnetism (FM) and ferroeletricity (FE) at room temperature (RT) are promising for applications. Here, the authors demonstrate by inducing strain in SmMnO3 via introducing vertically aligned nanocomposites that exchange coupling can be modified tuning the system from anti-FM to FM and simultaneously inducing FE at RT.

We demonstrate a new way to increase the superconducting TC of cuprates using 3-D strain control in nanocomposite thin films., A long-term goal for superconductors is to increase the superconducting transition temperature, TC. In cuprates, TC depends strongly on the out-of-plane Cu-apical oxygen distance and the in-plane Cu-O distance, but there has been little attention paid to tuning them independently. Here, in simply grown, self-assembled, vertically aligned nanocomposite thin films of La2CuO4+δ + LaCuO3, by strongly increasing out-of-plane distances without reducing in-plane distances (three-dimensional strain engineering), we achieve superconductivity up to 50 K in the vertical interface regions, spaced ~50 nm apart. No additional process to supply excess oxygen, e.g., by ozone or high-pressure oxygen annealing, was required, as is normally the case for plain La2CuO4+δ films. Our proof-of-concept work represents an entirely new approach to increasing TC in cuprates or other superconductors.

In all-oxide-based spintronic devices, large exchange bias effect with robustness against temperature fluctuation and compatibility with perpendicular magnetic recording is highly desired. In this work, rock-salt antiferromagnetic NiO with a Néel temperature ( TN) of ∼525 K and spinel ferrimagnetic NiFe2O4 with a high Curie temperature, TC, ≈ 790 K and TC > TN were chosen as compatible materials to form a well-phase-separated, vertically aligned nanocomposite thin film. In this nanoengineered thin film, an exchange bias effect with a blocking temperature far above room temperature has been achieved. A large perpendicular exchange bias field of up to 0.91 kOe with an interfacial exchange energy density of 0.11-0.34 erg/cm2 was obtained at room temperature. It was also demonstrated that the exchange bias effect can be easily tuned by changing the alignment of the magnetic moments in the NiO phase using substrates of different crystalline orientations and by changing the microstructure of the film with substrates of different lattice parameters. The results demonstrate that proper choice of the phases (including use of nonperovskite compositions) and careful strain engineering and nanostructure engineering makes oxide nanocomposites strong potential candidate systems for next generation spintronic devices.

Resistive switches are non-volatile memory cells based on nano-ionic redox processes that offer energy efficient device architectures and open pathways to neuromorphics and cognitive computing. However, channel formation typically requires an irreversible, not well controlled electroforming process, giving difficulty to independently control ionic and electronic properties. The device performance is also limited by the incomplete understanding of the underlying mechanisms. Here, we report a novel memristive model material system based on self-assembled Sm-doped CeO2 and SrTiO3 films that allow the separate tailoring of nanoscale ionic and electronic channels at high density (∼1012 inch−2). We systematically show that these devices allow precise engineering of the resistance states, thus enabling large on–off ratios and high reproducibility. The tunable structure presents an ideal platform to explore ionic and electronic mechanisms and we expect a wide potential impact also on other nascent technologies, ranging from ionic gating to micro-solid oxide fuel cells and neuromorphics., Metal oxide resistive switches rely on the migration of oxygen vacancies and electrons under applied voltage. Here, Cho et al. use nanocomposites to control the electronic and ionic conductivities in spatially distinct channels, and fabricate memristors with high on/off ratios and reproducibility.