Characterization of the onset of a phase transition is often challenging due to the fluctuations of the correlation length scales of the order parameters. This is especially true for second-order structural-phase transition due to minute changes involved in the relevant lattice constants. A classic example is the cubic-to-tetragonal second-order phase transition in SrTiO3 (STO), which is so subtle that it is still unresolved. Here, we demonstrate an approach to resolve this issue by epitaxially grown rhombohedral La0.7Sr0.3MnO3 (LSMO) thin films on the cubic STO (100) substrate. The shear strain induced nanotwinning waves in the LSMO film are extremely sensitive to the cubic-to-tetragonal structural-phase transitions of the STO substrate. Upon cooling from room temperature, the development of the nanotwinning waves is spatially inhomogeneous. Untwinned, atomically flat domains, ranging in size from 100 to 300 nm, start to appear randomly in the twinned phase between 265 and 175 K. At â¼139 K, the untwinned, atomically flat domains start to grow rapidly into micrometer scale and finally become dominant at â¼108 K. These results indicate that the low-temperature tetragonal precursor phase of STO has already nucleated at 265 K, significantly higher than the critical temperature of STO (â¼105 K). Our work paves a pathway to visualize the onset stages of structural-phase transitions that are too subtle to be observed using direct-imaging methods.
Cracks in solid-state materials are typically irreversible. Here we report electrically reversible opening and closing of nanoscale cracks in an intermetallic thin film grown on a ferroelectric substrate driven by a small electric field (~0.83 kV/cm). Accordingly, a nonvolatile colossal electroresistance on-off ratio of more than 108 is measured across the cracks in the intermetallic film at room temperature. Cracks are easily formed with low-frequency voltage cycling and remain stable when the device is operated at high frequency, which offers intriguing potential for next-generation high-frequency memory applications. Moreover, endurance testing demonstrates that the opening and closing of such cracks can reach over 107 cycles under 10-µs pulses, without catastrophic failure of the film.
We report the synthesis of single-crystal iron germanium nanowires via chemical vapor deposition without the assistance of any catalysts. The assembly of single-crystal FeGe2 nanowires with tetragonal C16 crystal structure shows anisotropic magnetic behavior along the radial direction or the growth axial direction, with both antiferromagnetic and ferromagnetic orders. Single FeGe2 nanowire devices were fabricated using e-beam lithography. Electronic transport measurement in these devices show two resistivity anomalies near 250 K and 200 K which are likely signatures of the two spin density wave states in FeGe2.
The perovskite unit cell is the fundamental building block of many functional materials. The manipulation of this crystal structure is known to be of central importance to controlling many technologically promising phenomena related to superconductivity, multiferroicity, mangetoresistivity, and photovoltaics. The broad range of properties that this structure can exhibit is in part due to the centrally coordinated octahedra bond flexibility, which allows for a multitude of distortions from the ideal highly symmetric structure. However, continuous and fine manipulation of these distortions has never been possible. Here, we show that controlled insertion of He atoms into an epitaxial perovskite film can be used to finely tune the lattice symmetry by modifying the local distortions, i.e., octahedral bonding angle and length. Orthorhombic SrRuO3 films coherently grown on SrTiO3 substrates are used as a model system. Implanted He atoms are confirmed to induce out-of-plane strain, which provides the ability to controllably shift the bulk-like orthorhombically distorted phase to a tetragonal structure by shifting the oxygen octahedra rotation pattern. These results demonstrate that He implantation offers an entirely new pathway to strain engineering of perovskite-based complex oxide thin films, useful for creating new functionalities or properties in perovskite materials.
We report a giant, â¼22%, electroresistance modulation for a metallic alloy above room temperature. It is achieved by a small electric field of 2 kV/cm via piezoelectric strain-mediated magnetoelectric coupling and the resulting magnetic phase transition in epitaxial FeRh/BaTiO_{3} heterostructures. This work presents detailed experimental evidence for an isothermal magnetic phase transition driven by tetragonality modulation in FeRh thin films, which is in contrast to the large volume expansion in the conventional temperature-driven magnetic phase transition in FeRh. Moreover, all the experimental results in this work illustrate FeRh as a mixed-phase model system well similar to phase-separated colossal magnetoresistance systems with phase instability therein.
The realization of a controllable metamagnetic transition from AFM to FM ordering would open the door to a plethora of new spintronics based devices that, rather than reorienting spins in a ferromagnet, harness direct control of a materials intrinsic magnetic ordering. In this study FeRh films with drastically reduced transition temperatures and a large magneto-thermal hysteresis were produced for magnetocaloric and spintronics applications. Remarkably, giant controllable magnetization changes (measured to be as high has ~25%) are realized by manipulating the strain transfer from the external lattice when subjected to two structural phase transitions of BaTiO3 (001) single crystal substrate. These magnetization changes are the largest seen to date to be controllably induced in the FeRh system. Using polarized neutron reflectometry we reveal how just a slight in plane surface strain change at ~290C results in a massive magnetic transformation in the bottom half of the film clearly demonstrating a strong lattice-spin coupling in FeRh. By means of these substrate induced strain changes we show a way to reproducibly explore the effects of temperature and strain on the relative stabilities of the FM and AFM phases in multi-domain metamagnetic systems. This study also demonstrates for the first time the depth dependent nature of a controllable magnetic order using strain in an artificial multiferroic heterostructure.
A metastable phase α-FeSi_{2} was epitaxially stabilized on a silicon substrate using pulsed laser deposition. Nonmetallic and ferromagnetic behaviors are tailored on α-FeSi_{2} (111) thin films, while the bulk material of α-FeSi_{2} is metallic and nonmagnetic. The transport property of the films renders two different conducting states with a strong crossover at 50 K, which is accompanied by the onset of a ferromagnetic transition as well as a substantial magnetoresistance. These experimental results are discussed in terms of the unusual electronic structure of α-FeSi_{2} obtained within density functional calculations and Boltzmann transport calculations with and without strain. Our finding sheds light on achieving ferromagnetic semiconductors through both their structure and doping tailoring, and provides an example of a tailored material with rich functionalities for both basic research and practical applications.
Physical and electrochemical phenomena at the surfaces of transition metal oxides and their coupling to local functionality remains one of the enigmas of condensed matter physics. Understanding the emergent physical phenomena at surfaces requires the capability to probe the local composition, map order parameter fields and establish their coupling to electronic properties. Here we demonstrate that measuring the sub-30-pm displacements of atoms from high-symmetry positions in the atomically resolved scanning tunnelling microscopy allows the physical order parameter fields to be visualized in real space on the single-atom level. Here, this local crystallographic analysis is applied to the in-situ-grown manganite surfaces. In particular, using direct bond-angle mapping we report direct observation of structural domains on manganite surfaces, and trace their origin to surface-chemistry-induced stabilization of ordered Jahn-Teller displacements. Density functional calculations provide insight into the intriguing interplay between the various degrees of freedom now resolved on the atomic level.
Organic spintronic devices have been appealing because of the long spin lifetime of the charge carriers in the organic materials and their low cost, flexibility and chemical diversity. In previous studies, the control of resistance of organic spin valves is generally achieved by the alignment of the magnetization directions of the two ferromagnetic electrodes, generating magnetoresistance. Here we employ a new knob to tune the resistance of organic spin valves by adding a thin ferroelectric interfacial layer between the ferromagnetic electrode and the organic spacer: the magnetoresistance of the spin valve depends strongly on the history of the bias voltage, which is correlated with the polarization of the ferroelectric layer; the magnetoresistance even changes sign when the electric polarization of the ferroelectric layer is reversed. These findings enable active control of resistance using both electric and magnetic fields, opening up possibility for multi-state organic spin valves.
Highly strained BiFeO3 films transition into a true tetragonal state at 430 °C but remain polar to much higher temperatures (â¼800 °C). Piezoelectric switching is only possible up to 300 °C, i.e., at temperatures for which strain stabilizes the stripe-like coexistence of multiple polymorphs.
In strongly correlated electronic systems, the global transport behavior depends sensitively on spin ordering. We show that spin ordering in manganites can be controlled by depositing isolated ferromagnetic nanodots at the surface. The exchange field at the interface is tunable with nanodot density and makes it possible to overcome dimensionality and strain effects in frustrated systems to greatly increasing the metal-insulator transition and magnetoresistance. These findings indicate that electronic phase separation can be controlled by the presence of magnetic nanodots.
Interfacial diffusion between magnetic electrodes and organic spacer layers is a serious problem in the organic spintronics which complicates attempts to understand the spin-dependent transport mechanism and hurts the achievement of a desirably high magnetoresistance (MR). We deposit nanodots instead of atoms onto the organic layer using buffer layer assist growth. Spin valves using this method exhibit a sharper interface and a giant MR of up to â¼300%. Analysis of the current-voltage characteristics indicates that the spin-dependent carrier injection correlates with the observed MR.
We studied the surface structure of La_{5/8}Ca_{3/8}MnO_{3}(001) thin films using in situ scanning tunneling microscopy (STM). Atomically resolved STM images reveal that a (sqrt[2]xsqrt[2])R45;{ degrees } reconstructed surface and a (1x1) surface can be converted back and forth through adsorption and desorption of oxygen at the surface. The electrical properties of the surfaces are investigated by scanning tunneling spectroscopy. I-V curves clearly show that the presence of an oxygen overlayer renders the surface insulating while the (1x1) surface without the oxygen overlayer is metallic.
The dynamics of first-order electronic phase transitions in complex transition metal oxides are not well understood but are crucial in understanding the emergent phenomena of electronic phase separation. We show that a manganite system reduced to the scale of its inherent electronic charge-ordered insulating and ferromagnetic metal phase domains allows for the direct observation of single electronic phase domain fluctuations within a critical regime of temperature and magnetic field at the metal-insulator transition.
The metal-insulator transition is characterized as a single peak in the temperature-dependent resistivity measurements; exceptions to this have never been seen in any single crystal material system. We show that by reducing a single crystal manganite thin film to a wire with a width comparable to the mesoscopic phase-separated domains inherent in the material, a second and robust metal-insulator transition peak appears in the resistivity versus temperature measurement. This new observation suggests that spatial confinement is a promising route for the discovery of emergent physical phenomena in complex oxides.
Optical lithography is used to fabricate LPCMO wires starting from a single (La(5/8-0.3)Pr(0.3))Ca3/8MnO3 (LPCMO) film epitaxially grown on a LaAlO3(100) substrate. As the width of the wires is decreased, the resistivity of the LPCMO wires exhibits giant and ultrasharp steps upon varying temperature and magnetic field in the vicinity of the metal-insulator transition. The origin of the ultrasharp transitions is attributed to the effect of spatial confinement on the percolative transport in manganites.
