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In this work, the high entropy oxide A2CuO4 Ruddlesden-Popper (La0.2Pr0.2Nd0.2Sm0.2Eu0.2)2CuO4 is explored by charge doping with Ce+4 and Sr+2 at concentrations known to induce superconductivity in the simple parent compounds, Nd2CuO4 and La2CuO4. Electron doped (La0.185Pr0.185Nd0.185Sm0.185Eu0.185Ce0.075)2CuO4 and hole doped (La0.18Pr0.18Nd0.18Sm0.18Eu0.18Sr0.1)2CuO4 are synthesized and shown to be single crystal, epitaxially strained, and highly uniform. Transport measurements demonstrate that all as-grown films are insulating regardless of doping. Annealing studies show that resistivity can be tuned by modifying oxygen stoichiometry and inducing metallicity but without superconductivity. These results in turn are connected to extended x-ray absorption fine structure (EXAFS) results indicating that the lack of superconductivity in the high entropy cuprates likely originates from a large distortion within the Cu-O plane ({\sigma}2>0.015 {\AA}2) due to A-site cation size variance, which drives localization of charge carriers. These findings describe new opportunities for controlling charge- and orbital-mediated functional responses in Ruddlesden-Popper crystal structures, driven by balancing of cation size and charge variances that may be exploited for functionally important behaviors such as superconductivity, antiferromagnetism, and metal-insulator transitions, while opening less understood phase spaces hosting doped Mott insulators, strange metals, quantum criticality, pseudogaps, and ordered charge density waves.

The influence of hole doping on magnetic properties is mapped for the compositionally complex high-entropy oxide ${AB\mathrm{O}}_{3}$ perovskite ${\mathrm{La}}_{1\text{\ensuremath{-}}x}{\mathrm{Sr}}_{x}({\mathrm{Cr}}_{0.2}{\mathrm{Mn}}_{0.2}{\mathrm{Fe}}_{0.2}{\mathrm{Co}}_{0.2}{\mathrm{Ni}}_{0.2}){\mathrm{O}}_{3}$ $(0\ensuremath{\le}x\ensuremath{\le}0.5)$. It is found that aliovalent A-site substitution is a viable means to manipulate the magnetically active B-site sublattice. A series of single-crystal films are synthesized and show a general trend toward stronger ferromagnetic response and a shift in magnetic anisotropy as the Sr concentration increases. Magnetometry demonstrates complex and nonuniform responses similar to rigid and uncoupled composites at intermediate dopings. This behavior points to the presence of locally inhomogeneous magnetic phase competition, where ferromagnetic and antiferromagnetic magnetic contributions create a frustrated matrix containing uncompensated spins at the boundaries between these regions. The observations are discussed in the context of known responses to hole doping in the less complex ternary $\mathrm{La}{T}_{M}{\mathrm{O}}_{3}$ $({T}_{M}=\mathrm{Cr},\mathrm{Mn},\mathrm{Fe},\mathrm{Co},\mathrm{Ni})$ oxides, and they are found to be different from a simple sum of the doped parents. The results are summarized in a preliminary magnetic phase diagram.

In classical morphotropic piezoelectric materials, rhombohedral and tetragonal phase variants can energetically compete to form a mixed phase regime with improved functional properties. While the discovery of morphotropic-like phases in multiferroic BiFeO3 films has broadened this definition, accessing these phase spaces is still typically accomplished through isovalent substitution or heteroepitaxial strain which do not allow for continuous modification of phase composition postsynthesis. Here, we show that it is possible to use low-energy helium implantation to tailor morphotropic phases of epitaxial BiFeO3 films postsynthesis in a continuous and iterative manner. Applying this strain doping approach to morphotropic films creates a new phase space based on internal and external lattice stress that can be seen as an analogue to temperature–composition phase diagrams of classical morphotropic ferroelectric systems.

Disorder can have a dominating influence on correlated and quantum materials leading to novel behaviors which have no clean limit counterparts. In magnetic systems, spin and exchange disorder can provide access to quantum criticality, frustration, and spin dynamics, but broad tunability of these responses and a deeper understanding of strong limit disorder is lacking. In this work, we demonstrate that high entropy oxides present an unexplored route to designing quantum materials in which the presence of strong local compositional disorder hosted on a positionally ordered lattice can be used to generate highly tunable emergent magnetic behavior--from macroscopically ordered states to frustration-driven dynamic spin interactions. Single crystal La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 films are used as a structurally uniform model system hosting a magnetic sublattice with massive microstate disorder in the form of site-to-site spin and exchange type inhomogeneity. A classical Heisenberg model is found to be sufficient to describe how compositionally disordered systems can paradoxically host long-range magnetic uniformity and demonstrates that balancing the populating elements based on their discrete quantum parameters can be used to give continuous control over ordering types and critical temperatures. Theory-guided experiments show that composite exchange values derived from the complex mix of microstate interactions can be used to design the required compositional parameters for a desired response. These predicted materials are synthesized and found to possess an incipient quantum critical point when magnetic ordering types are designed to be in direct competition; this leads to highly controllable exchange bias sensitivity in the monolithic single crystal films previously accessible only in intentionally designed bilayer heterojunctions.

Magnetic insulators are important materials for a range of next-generation memory and spintronic applications. Structural constraints in this class of devices generally require a clean heterointerface that allows effective magnetic coupling between the insulating layer and the conducting layer. However, there are relatively few examples of magnetic insulators that can be synthesized with surface qualities that would allow these smooth interfaces and precisely tuned interfacial magnetic exchange coupling, which might be applicable at room temperature. In this work, we demonstrate an example of how the configurational complexity in the magnetic insulator layer can be used to realize these properties. The entropy-assisted synthesis is used to create single-crystal (Mg

Controlling electronic band structure is an important step toward harnessing quantum materials for practical uses. This is exemplified in the spin-polarized bands near the Fermi level of a ferromagnet where small variation to the Berry curvature can be used to control the intrinsic anomalous Hall effect (AHE). Since these pathways are highly sensitive to crystal structure, iterative post-synthesis manipulation of the underlying lattice can act as a fundamental probe and provide new opportunities for functionalization. In this work, depth-dependent magnetic inhomogeneity in a $4d$ itinerant ferromagnet ${\mathrm{SrRuO}}_{3}$ film is controlled by applying low energy He ion irradiation. Combined magnetometry, polarized neutron reflectometry, and magnetotransport experiments demonstrate that the Berry phase and associated AHE can be continuously and iteratively modified post-synthesis. The findings of this work should be widely applicable to other quantum materials where crystal distortions and symmetry are tightly bound to band structure and resulting Berry phase effects.

The surfaces of rutile transition-metal oxides $({\mathrm{TMO}}_{2})$ are widely investigated for catalysis, photoelectrochemical solar cells, memristors, and supercapacitors, but their structures have remained controversial. Here we employ density functional theory to predict that a universal behavior of metallic ${\mathrm{TMO}}_{2}$ surfaces, i.e., the stoichiometric ${\mathrm{TMO}}_{2}$ surfaces, exhibit a contrast reversal in simulated scanning tunneling microscopy (STM) images at different scanning biases. The predictions are verified by experimental STM imaging of ${\mathrm{RuO}}_{2}(110)$ surfaces and this feature is shown to enable accurate determinations of the ${\mathrm{TMO}}_{2}(110)$ surface structures under various conditions. This work provides different insights into the electronic properties of ${\mathrm{TMO}}_{2}(110)$ surfaces and offers an effective method to directly map the surface structure and point defects using bias-dependent STM.

The 2D layered Ruddlesden-Popper crystal structure can host a broad range of functionally important behaviors. Here we establish extraordinary configurational disorder in a two dimensional layered Ruddlesden-Popper (RP) structure using entropy stabilization assisted synthesis. A protype A2CuO4 RP cuprate oxide with five components (La, Pr, Nd, Sm, Eu) on the A-site sublattice is designed and fabricated into epitaxial single crystal films using pulsed laser deposition. By comparing (La0.2Pr0.2Nd0.2Sm0.2Eu0.2)2CuO4 crystals grown under identical conditions but different substrates, it is found that heteroepitaxial strain plays an important role in crystal phase formation. When grown on a near lattice matched substrate, the high entropy oxide film features a T'-type RP structure with uniform A-site cation mixing and square-planar CuO4 units, however, growing under strong compressive strain results in a single crystal non-RP cubic phase consistent with a CuX2O4 spinel structure. These observations are made with a range of combined characterizations using X-ray diffraction, atomic-resolution scanning transmission electron microscopy, energy-dispersive X-ray spectroscopy, and X-ray absorption spectroscopy measurements. Designing configurational complexity and moving between 2D layered RP and 3D cubic crystal structures in this class of cuprate materials opens many opportunities for new design strategies related to magnetoresistance, unconventional superconductivity, ferroelectricity, catalysis, and ion transport.

Micrometer-tall vertically aligned single-crystalline CoFe2O4 nanobrush architectures with extraordinarily large aspect ratio have been achieved by the precise control of a kinetic and thermodynamic non-equilibrium pulsed laser epitaxy process. Direct observations by scanning transmission electron microscopy reveal that the nanobrush crystal is mostly defect-free by nature, and epitaxially connected to the substrate through a continuous 2D interface layer. In contrast, periodic dislocations and lattice defects such as anti-phase boundaries and twin boundaries are frequently observed in the 2D interface layer, suggesting that interface misfit strain relaxation under a non-equilibrium growth condition plays a critical role in the self-assembly of such artificial architectures. Magnetic property measurements have found that the nanobrushes exhibit a saturation magnetization value of 6.16 B/f.u., which is much higher than the bulk value. The discovery not only enables insights into an effective route for fabricating unconventional high-quality nanostructures, but also demonstrates a novel magnetic architecture with potential applications in nanomagnetic devices.

Configurational disorder can have a dominating role in the formation of macroscopic functional responses in strongly correlated materials. Here, we use entropy-stabilization synthesis to create single-crystal epitaxial $\mathrm{AB}{\mathrm{O}}_{3}$ perovskite thin films with equal atomic concentration of 3d transition-metal cations on the B-site sublattice. X-ray diffraction, atomic force microscopy, and scanning transmission electron microscopy of $\mathrm{La}(\mathrm{C}{\mathrm{r}}_{0.2}\mathrm{M}{\mathrm{n}}_{0.2}\mathrm{F}{\mathrm{e}}_{0.2}\mathrm{C}{\mathrm{o}}_{0.2}\mathrm{N}{\mathrm{i}}_{0.2}){\mathrm{O}}_{3}$ (L5BO) films demonstrate excellent crystallinity, smooth film surfaces, and uniform mixing of the 3d transition-metal cations throughout the B-site sublattice. The magnetic properties are strongly dependent on substrate-induced lattice anisotropy and suggest the presence of long-range magnetic order in these exceptionally disordered materials. The ability to populate multiple elements onto a single sublattice in complex crystal structures opens new possibilities to design functionality in correlated systems and enable novel fundamental studies seeking to understand how diverse local bonding environments can work to generate macroscopic responses, such as those driven by electron-phonon channels and complex exchange interaction pathways.

In electric double-layer transistors (EDLTs), it is well known that the EDL formed by ionic liquids (ILs) can induce an ultrahigh carrier density at the semiconductor surface, compared to solid dielectric. However, the mechanism of device performance is still not fully understood, especially at a molecular level. Here, we evaluate the gating performance of amorphous indium gallium zinc oxide (a-IGZO) transistor coupled with a series of imidazolium-based ILs, using an approach combining of molecular dynamics simulation and finite element modeling. Results reveal that the EDL with different ion structures could produce inhomogeneous electric fields at the solid-electrolyte interface, and the heterogeneity of electric field-induced charge distributions at semiconductor surface could reduce the electrical conductance of a-IGZO during gating process. Meanwhile, a resistance network analysis was adopted to bridge the nanoscopic data with the macroscopic transfer characteristics of IL-gated transistor, and showed that our theoretical results could well estimate the gating performance of practical devices. Thereby, our findings could provide both new concepts and modeling techniques for IL-gated transistors.

The formation of an electric double layer in ionic liquid (IL) can electrostatically induce charge carriers and/or intercalate ions in and out of the lattice which can trigger a large change of the electronic, optical, and magnetic properties of materials and even modify the crystal structure. We present a systematic study of ionic liquid gating of exfoliated 2D molybdenum trioxide (MoO3) devices and correlate the resultant electrical properties to the electrochemical doping via ion migration during the IL biasing process. A nearly 9 orders of magnitude modulation of the MoO3 conductivity is obtained for the two types of ionic liquids that are investigated. In addition, notably rapid on/off switching was realized through a lithium-containing ionic liquid whereas much slower modulation was induced via oxygen extraction/intercalation. Time of flight–secondary ion mass spectrometry confirms the Li intercalation. Density functional theory (DFT) calculations have been carried out to examine the underlying meta...

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.

In this study, high-performance multilayer WSe2 field-effect transistor (FET) devices with carrier type control are demonstrated via thickness modulation and a remote oxygen plasma surface treatment. Carrier type control in multilayer WSe2 FET devices with Cr/Au contacts is initially demonstrated by modulating the WSe2 thickness. The carrier type evolves with increasing WSe2 channel thickness, being p-type, ambipolar, and n-type at thicknesses 5 nm, respectively. The thickness-dependent carrier type is attributed to changes in the bandgap of WSe2 as a function of the thickness and the carrier band offsets relative to the metal contacts. Furthermore, we present a strong hole carrier doping effect via remote oxygen plasma treatment. It non-degenerately converts n-type characteristics into p-type and enhances field-effect hole mobility by three orders of magnitude. This work demonstrates progress towards the realization of high-performance multilayer WSe2 FETs with carrier type control, potentially extendable to other transition metal dichalcogenides, for future electronic and optoelectronic applications.

Discovering high-performance energy storage materials is indispensable for renewable energy, electric vehicle performance, and mobile computing. Owing to the open atomic framework and good room temperature conductivity, bronze-phase vanadium dioxide [VO2(B)] has been regarded as a highly promising electrode material for Li ion batteries. However, previous attempts were unsuccessful to show the desired cycling performance and capacity without chemical modification. Here, we show with epitaxial VO2(B) films that one can accomplish the theoretical limit for capacity with persistent charging–discharging cyclability owing to the high structural stability and unique open pathways for Li ion conduction. Atomic-scale characterization by scanning transmission electron microscopy and density functional theory calculations also reveal that the unique open pathways in VO2(B) provide the most stable sites for Li adsorption and diffusion. Thus, this work ultimately demonstrates that VO2(B) is a highly promising energy ...

The impact of single-axis lattice expansion on the optical response of $\mathrm{BiFe}{\mathrm{O}}_{3}$ films is examined. Low-energy He implantation is used to tailor morphotropic phases of $\mathrm{BiFe}{\mathrm{O}}_{3}$ films and study changes in their optical spectra with continuously increasing lattice expansion. He ion implantation of epitaxial rhombohedral (R)- and tetragonal (T)-like $\mathrm{BiFe}{\mathrm{O}}_{3}$ films induces uniaxial out-of-plane strain that, on R-like films, eventually leads to a complete R-T phase transition. This approach allows us to provide insights into the optical response of $\mathrm{BiFe}{\mathrm{O}}_{3}$ films. Strain doping of T-like films leads to a significant redshift of the optical absorption spectra that is theoretically explained by a lowering of Fe $3d\phantom{\rule{0.28em}{0ex}}{t}_{2g}$ states. R-like films, on the other hand, show a less-pronounced sensitivity to uniaxial strain and a blueshift of about 250 meV at the strain-induced R-T transition. The results demonstrate that strain doping allows a deeper examination of the optical properties of epitaxial phases that are otherwise impossible to access by standard epitaxy.

Due to the limit in computing power arising from the Von Neumann bottleneck, computational devices are being developed that mimic neuro-biological processing in the brain by correlating the device characteristics with the synaptic weight of neurons. This platform combines ionic liquid gating and electrowetting for programmable placement/connectivity of the ionic liquid. In this platform, both short-term potentiation (STP) and long-term potentiation (LTP) are realized via electrostatic and electrochemical doping of the amorphous indium gallium zinc oxide (aIGZO), respectively, and pulsed bias measurements are demonstrated for lower power considerations. While compatible with resistive elements, we demonstrate a platform based on transitive amorphous indium gallium zinc oxide (aIGZO) pixel elements. Using a lithium based ionic liquid, we demonstrate both potentiation (decrease in device resistance) and depression (increase in device resistance), and propose a 2D platform array that would enable a much higher pixel count via Active Matrix electrowetting.

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 SrTiO(3) (STO), which is so subtle that it is still unresolved. Here, we demonstrate an approach to resolve this issue by epitaxially grown rhombohedral La(0.7)Sr(0.3)MnO(3) (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 ∼139 K, the untwinned, atomically flat domains start to grow rapidly into micrometer scale and finally become dominant at ∼108 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 (∼105 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.

In classical morphotropic piezoelectric materials, rhombohedral and tetragonal phase variants can energetically compete to form a mixed phase regime with improved functional properties. While the discovery of morphotropic-like phases in multiferroic BiFeO

Thickness dependent strain relaxation effects are utilized to study the impact of crystal anisotropy on the optical band gap of epitaxial SnO2 films grown by pulsed laser deposition on (0001)-oriented sapphire substrates. An X-ray diffraction analysis reveals that all films are under tensile biaxial in-plane strain and that strain relaxation occurs with increasing thickness. Variable angle spectroscopic ellipsometry shows that the optical band gap of the SnO2 films continuously increases with increasing film thickness. This increase in the band gap is linearly related to the strain state of the films, which indicates that the main origin of the band gap change is strain relaxation. The experimental observation is in excellent agreement with results from density functional theory for biaxial in-plane strain. This work demonstrates that strain is an effective way to tune the band gap of SnO2 films and suggests that strain engineering is an appealing route to tailor the optical properties of oxide semiconductors.

Self-poling of ferroelectric films, i.e., a preferred, uniform direction of the ferroelectric polarization in as-grown samples is often observed yet poorly understood despite its importance for device applications. The multiferroic perovskite BiFeO3, which crystallizes in two distinct structural polymorphs depending on applied epitaxial strain, is well known to exhibit self-poling. This study investigates the effect of self-poling on the monoclinic domain configuration and the switching properties of the two polymorphs of BiFeO3 (R′ and T′) in thin films grown on LaAlO3 substrates with slightly different La0.3Sr0.7MnO3 buffer layers. This study shows that the polarization state formed during the growth acts as “imprint” on the polarization and that switching the polarization away from this self-poled direction can only be done at the expense of the sample's monoclinic domain configuration. The observed reduction of the monoclinic domain size is largely reversible; hence, the domain size is restored when the polarization is switched back to its original orientation. This is a direct consequence of the growth taking place in the polar phase (below Tc). Switching the polarization away from the preferred configuration, in which defects and domain patterns synergistically minimize the system's energy, leads to a domain state with smaller (and more highly strained and distorted) monoclinic domains.

Amorphous metal-oxide semiconductors offer the high carrier mobilities and excellent large-area uniformity required for high performance, transparent, flexible electronic devices; however, a critical bottleneck to their widespread implementation is the need to activate these materials at high temperatures which are not compatible with flexible polymer substrates. The highly controllable activation of amorphous indium gallium zinc oxide semiconductor channels using ionic liquid gating at room temperature is reported. Activation is controlled by electric field-induced oxygen migration across the ionic liquid-semiconductor interface. In addition to activation of unannealed devices, it is shown that threshold voltages of a transistor can be linearly tuned between the enhancement and depletion modes. Finally, the first ever example of transparent flexible thin film metal oxide transistor on a polyamide substrate created using this simple technique is demonstrated. This study demonstrates the potential of field-induced activation as a promising alternative to traditional postdeposition thermal annealing which opens the door to wide scale implementation into flexible electronic applications.

The optical band gap of the prototypical semiconducting oxide SnO2 is shown to be continuously controlled through single axis lattice expansion of nanometric films induced by low-energy helium implantation. While traditional epitaxy-induced strain results in Poisson driven multidirectional lattice changes shown to only allow discrete increases in bandgap, we find that a downward shift in the band gap can be linearly dictated as a function of out-of-plane lattice expansion. Our experimental observations closely match density functional theory that demonstrates that uniaxial strain provides a fundamentally different effect on the band structure than traditional epitaxy-induced multiaxes strain effects. Charge density calculations further support these findings and provide evidence that uniaxial strain can be used to drive orbital hybridization inaccessible with traditional strain engineering techniques.

Finite range ferromagnetism and antiferromagnetism in two-dimensional (2D) systems within an isotropic Heisenberg model at non-zero temperature were originally proposed to be impossible. However, recent theoretical studies using an Ising model have shown that 2D magnetic crystals can exhibit magnetism. Experimental verification of existing 2D magnetic crystals in this system has remained exploratory. In this work we exfoliated CrSiTe3, a bulk ferromagnetic semiconductor, to mono- and few-layer 2D crystals onto a Si/SiO2 substrate. Raman spectra indicate good stability and high quality of the exfoliated flakes, consistent with the computed phonon spectra of 2D CrSiTe3, giving strong evidence for the existence of 2D CrSiTe3 crystals. When the thickness of the CrSiTe3 crystals is reduced to a few layers, we observed a clear change in resistivity at 80–120 K, consistent with theoretical calculations of the Curie temperature (Tc) of ∼80 K for the magnetic ordering of 2D CrSiTe3 crystals. The ferromagnetic mono- and few-layer 2D CrSiTe3 indicated here should enable numerous applications in nano-spintronics.

A new class of ceramics, called entropy stabilized oxides, High Entropy Oxides (HEOs), multicomponent oxides, compositionally complex oxides, or polycation oxides, has generated considerable research interest since the first report in 2015. This multicomponent approach has created new opportunities for materials design and discovery. This Perspective will highlight some current research developments and possible applications while also providing an overview of the many successfully synthesized HEO systems to date. The polycation approach to composition development will be discussed along with a few case studies, challenges, and future possibilities afforded by this novel class of materials.

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., Electric-field-induced cracks are generally detrimental to functionality of ferroelectric ceramics. Liu et al. use an intermetallic alloy and ferroelectric oxide junction to mediate the reversible formation of cracks at nanoscales, resulting in colossal electroresistance modulation for memory applications.

High-quality epitaxial growth of inter-metallic MnPt films on oxides is achieved, with potential for multiferroic heterostructure applications. Antisite-stabilized spin-flipping induces ferromagnetism in MnPt films, although it is robustly antiferromagnetic in bulk. Moreover, highly ordered antiferromagnetic MnPt films exhibit superiorly large exchange coupling with a ferromagnetic layer.

Ionic liquid gating of transition metal oxides has enabled new states (magnetic, electronic, metal-insulator), providing fundamental insights into the physics of strongly correlated oxides. However, despite much research activity, little is known about the correlation of the structure of the liquids in contact with the transition metal oxide surface, its evolution with the applied electric potential, and its correlation with the measured electronic properties of the oxide. Here, we investigate the structure of an ionic liquid at a semiconducting oxide interface during the operation of a thin film transistor where the electrical double layer gates the device using experiment and theory. We show that the transition between the ON and OFF states of the amorphous indium gallium zinc oxide transistor is accompanied by a densification and preferential spatial orientation of counterions at the oxide channel surface. This process occurs in three distinct steps, corresponding to ion orientations, and consequently, regimes of different electrical conductivity. The reason for this can be found in the surface charge densities on the oxide surface when different ion arrangements are present. Overall, the field-effect gating process is elucidated in terms of the interfacial ionic liquid structure, and this provides unprecedented insight into the working of a liquid gated transistor linking the nanoscopic structure to the functional properties. This knowledge will enable both new ionic liquid design as well as advanced device concepts.

Finding a route to synthesize nanostructures with a high‐surface area is critical for developing high‐performance energy materials. In article number 1700045, Lisha Fan, Ho Nyung Lee, and co‐workers demonstrate that precise control of nonequilibrium growth conditions during pulsed laser deposition can produce single‐crystalline anatase TiO2 nanobrush architectures with large surface areas terminated with high energy {001} facets.

In this paper, high performance top-gated WSe

Atomic resolution imaging and spectroscopy suffers from inherently low signal to noise ratios often prohibiting the interpretation of single pixels or spectra. We introduce local low rank (LLR) denoising as tool for efficient noise removal in scanning transmission electron microscopy (STEM) images and electron energy-loss (EEL) spectrum images. LLR denoising utilizes tensor decomposition techniques, in particular the multilinear singular value decomposition (MLSVD), to achieve a denoising in a general setting largely independent of the signal features and data dimension, by assuming that the signal of interest is of low rank in segments of appropriately chosen size. When applied to STEM images of graphene, LLR denoising suppresses statistical noise while retaining fine image features such as scan row-wise distortions, possibly related to rippling of the graphene sheet and consequent motion of atoms. When applied to EEL spectra, LLR denoising reveals fine structures distinguishing different lattice sites in the spinel system CoFe

Discovering high-performance energy storage materials is indispensable for renewable energy, electric vehicle performance, and mobile computing. Owing to the open atomic framework and good room temperature conductivity, bronze-phase vanadium dioxide [VO

We report a giant, ~22%, 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/BaTiO3 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., 6 pages, 3 figures

This study demonstrates that precise control of nonequilibrium growth conditions during pulsed laser deposition (PLD) can be exploited to produce single‐crystalline anatase TiO2 nanobrush architectures with large surface areas terminated with high energy {001} facets. The data indicate that the key to nanobrush formation is controlling the atomic surface transport processes to balance defect aggregation and surface‐smoothing processes. High‐resolution scanning transmission electron microscopy data reveal that defect‐mediated aggregation is the key to TiO2 nanobrush formation. The large concentration of defects present at the intersection of domain boundaries promotes aggregation of PLD growth species, resulting in the growth of the single‐crystalline nanobrush architecture. This study proposes a model for the relationship between defect creation and growth mode in nonequilibrium environments, which enables application of this growth method to novel nanostructure design in a broad range of materials.