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Christopher Bell

Publications and source records attributed to Christopher Bell.

At least 19 recordsLinked to original sources

A Topotactic Phase Transition in the Uranium Oxide System

A topotactic phase transition involves the transformation of one crystalline solid to another, which may include the loss or gain of material, where the orientation of the parent crystal determines the orientation of the daughter. We set out an experimental approach, based on polyepitaxial thin film deposition, where the precise transformation mechanism in important physico-chemical processes can be revealed in brilliant detail. Here, we find a reversible topotactic transition from (001) cubic UO2 to a (130) orthorhombic U3O8 structure; a >35% expansion/contraction. This remarkable result solves a puzzle that has eluded researchers for decades, and presents a method for determining the mechanism of crystallographic transformation in many other compounds.

cond-mat.mtrl-sci

Magnetism and 3D Electron Diffraction Solution of Hydrated Rubidium-Ruthenium Oxide Rb$_2$Ru$_2$O$_7$.H$_2$O

The crystal structure of Rb$_2$Ru$_2$O$_7$.H$_2$O was determined by three-dimensional electron diffraction from the individual crystallites of a solid-state powder product. Rb$_2$Ru$_2$O$_7$.H$_2$O crystallizes in space group \textit{C}2/\textit{c} ($a=7.841(3)$ \AA, $b=12.500(3)$ \AA, $c=8.392(2)$ \AA, $\beta=93.57(4)^\circ$, Z=4). The structure contains infinite chains that run normal to the (101) plane and consist of alternating RuO$_6$ octahedra and square-pyramidal RuO$_5$ units connected via shared O-O edges. Magnetic properties were measured on the bulk powder, showing a diamagnetic baseline from 300 to 60 K with a small Curie tail below 55 K. The magnetic moment, calculated from the 1.8 K isotherm, saturates at $M=4.4\times10^{-3}\,\mu_\mathrm{B}\,\mathrm{Ru}^{-1}$, much less than would be expected for $S=1$ ruthenium. Bond-valence-sum analysis indicates high-valent Ru, and the near-diamagnetic response is consistent with the edge-sharing Ru-Ru motif, where weak direct Ru-Ru overlap yields a local singlet.

cond-mat.mtrl-sci

Resistivity anomalies and intrinsic spin-orbit coupling in superconducting thin film solid solutions of Nb$_{1-x}$U$_x$ for $0.15 < x < 0.40$

Polycrystalline thin films of $\mathrm{Nb}_{1-x}\mathrm{U}_{x}$ solid solutions with $0.15\leq x \leq 0.40$ were prepared via d.c. magnetron sputtering at ambient conditions. X-ray characterisation of the samples revealed a systematic shift of the (110) Nb Bragg reflection with U concentration, consistent with substitutional replacement of the Nb by U. Superconductivity was observed in all samples below $2$ K. Analysis of the superconducting critical fields revealed a direct scaling of the spin-orbit scattering and transport scattering times, indicating Elliott-Yafet-type spin relaxation in the system. Magnetoresistivity measurements showed a feature in the range $4$ K $\leq T \leq30$ K suggesting a possible a complex interplay between electron-electron interaction and localisation physics.

cond-mat.supr-con

Epitaxial thin film growth in the U-Ge binary system

We explore the U-Ge phase diagram using thin film growth by co-deposition of U and Ge via d.c. magnetron sputtering. Using three different single crystal substrates - MgO, CaF$_2$ and SrTiO$_3$ - we have stabilised mixed phase films of mostly UGe$_3$ and UGe, with evidence of UGe$_2$ as well. At higher temperatures UO$_2$ forms as a consequence of gettering of oxygen from several types of substrate. Several UGe$_3$ dominated samples grown on MgO substrates have also been characterised electrically, showing residual resistivity ratios up to six.

cond-mat.mtrl-sci

Absence of Induced Ferromagnetism in Epitaxial Uranium Dioxide Thin Films

Recently, Sharma et al. [Adv. Sci. 9, 2203473 (2022)] claimed that thin films (around 20 nm) of UO2 deposited on perovskite substrates exhibit strongly enhanced paramagnetism (called induced ferromagnetism by the authors). Moments of up to 3 Bohr magneton/U atom were claimed in magnetic fields of 6 T. We have reproduced such films and, after characterisation, have examined them with X-ray circular magnetic dichroism (XMCD) at the uranium M edges, a technique that is element specific. We do not confirm the published results. We find a small increase, as compared to the bulk, in the magnetic susceptibility of UO2 in such films, but the magnetisation versus field curves, measured by XMCD, are linear with field and there is no indication of any ferromagnetism. The absence of any anomaly around 30 K (the antiferromagnetic ordering temperature of bulk UO2) in the XMCD signal suggests the films do not order magnetically.

cond-mat.mtrl-sci

Universal bound to the amplitude of the vortex Nernst signal in superconductors

A liquid of superconducting vortices generates a transverse thermoelectric response. This Nernst signal has a tail deep in the normal state due to superconducting fluctuations. Here, we present a study of the Nernst effect in two-dimensional hetero-structures of Nb-doped strontium titanate (STO) and in amorphous MoGe. The Nernst signal generated by ephemeral Cooper pairs above the critical temperature has the magnitude expected by theory in STO. On the other hand, the peak amplitude of the vortex Nernst signal below $T_c$ is comparable in both and in numerous other superconductors despite the large distribution of the critical temperature and the critical magnetic fields. In four superconductors belonging to different families, the maximum Nernst signal corresponds to an entropy per vortex per layer of $\approx$ k$_Bln2$.

cond-mat.supr-con

Dual-Gate Modulation of Carrier Density and Disorder in an Oxide Two-Dimensional Electron System

Carrier density and disorder are two crucial parameters that control the properties of correlated two-dimensional electron systems. In order to disentangle their individual contributions to quantum phenomena, independent tuning of these two parameters is required. Here, by utilizing a hybrid liquid/solid electric dual-gate geometry acting on the conducting LaAlO3/SrTiO3 heterointerface, we obtain an additional degree of freedom to strongly modify the electron confinement profile and thus the strength of interfacial scattering, independent from the carrier density. A dual-gate controlled nonlinear Hall effect is a direct manifestation of this profile, which can be quantitatively understood by a Poisson-Schrodinger subband model. In particular, the large nonlinear dielectric response of SrTiO3 enables a very wide range of tunable density and disorder, far beyond that for conventional semiconductors. Our study provides a broad framework for understanding various reported phenomena at the LaAlO3/SrTiO3 interface.

cond-mat.str-el

Observation of the signatures of sub-resolution defects in two-dimensional superconductors with scanning SQUID

The diamagnetic susceptibility of a superconductor is directly related to its superfluid density. Mutual inductance is a highly sensitive method for characterizing thin films; however, in traditional mutual inductance measurements, the measured response is a non-trivial average over the area of the mutual inductance coils, which are typically of millimeter size. Here we image localized, isolated features in the diamagnetic susceptibility of {\delta}-doped SrTiO3, the 2-DES at the interface between LaAlO3 and SrTiO3, and Nb superconducting thin film systems using scanning superconducting quantum interference device susceptometry, with spatial resolution as fine as 0.7 {\mu}m. We show that these features can be modeled as locally suppressed superfluid density, with a single parameter that characterizes the strength of each feature. This method provides a systematic means of finding and quantifying submicron defects in two-dimensional superconductors.

cond-mat.supr-con

Imaging and tuning polarity at SrTiO3 domain walls

Electrostatic fields tune the ground state of interfaces between complex oxide materials. Electronic properties, such as conductivity and superconductivity, can be tuned and then used to create and control circuit elements and gate-defined devices. Here we show that naturally occurring twin boundaries, with properties that are different from their surrounding bulk, can tune the LaAlO3/SrTiO3 interface 2DEG at the nanoscale. In particular, SrTiO3 domain boundaries have the unusual distinction of remaining highly mobile down to low temperatures, and were recently suggested to be polar. Here we apply localized pressure to an individual SrTiO3 twin boundary and detect a change in LaAlO3/SrTiO3 interface current distribution. Our data directly confirm the existence of polarity at the twin boundaries, and demonstrate that they can serve as effective tunable gates. As the location of SrTiO3 domain walls can be controlled using external field stimuli, our findings suggest a novel approach to manipulate SrTiO3-based devices on the nanoscale.

cond-mat.mes-hall

Enhanced Superconducting Transition Temperature due to Tetragonal Domains in Two-Dimensionally Doped SrTiO$_3$

Strontium titanate is a low-temperature, non-Bardeen-Cooper-Schrieffer superconductor that superconducts to carrier concentrations lower than in any other system and exhibits avoided ferroelectricity at low temperatures. Neither the mechanism of superconductivity in strontium titanate nor the importance of the structure and dielectric properties for the superconductivity are well understood. We studied the effects of twin structure on superconductivity in a 5.5-nm-thick layer of niobium-doped SrTiO$_{3}$ embedded in undoped SrTiO$_{3}$. We used a scanning superconducting quantum interference device susceptometer to image the local diamagnetic response of the sample as a function of temperature. We observed regions that exhibited a superconducting transition temperature $T_{c}$ $\gtrsim$ 10% higher than the temperature at which the sample was fully superconducting. The pattern of these regions varied spatially in a manner characteristic of structural twin domains. Our results emphasize that the anisotropic dielectric properties of SrTiO$_{3}$ are important for its superconductivity, and need to be considered in any theory of the mechanism of the superconductivity.

cond-mat.supr-con

Anisotropic transport at the LaAlO3/SrTiO3 interface explained by microscopic imaging of channel-flow over SrTiO3 domains

Oxide interfaces, including the LaAlO3/SrTiO3 interface, have been a subject of intense interest for over a decade due to their rich physics and potential as low dimensional nanoelectronic systems. The field has reached the stage where efforts are invested in developing devices. It is critical now to understand the functionalities and limitations of such devices. Recent scanning probe measurements of the LaAlO3/SrTiO3 interface have revealed locally enhanced current flow and accumulation of charge along channels related to SrTiO3 structural domains. These observations raised a key question regarding the role these modulations play in the macroscopic properties of devices. Here we show that the microscopic picture, mapped by scanning superconducting quantum interference device, accounts for a substantial part of the macroscopically measured transport anisotropy. We compared local flux data with transport values, measured simultaneously, over various SrTiO3 domain configurations. We show a clear relation between maps of local current density over specific domain configurations and the measured anisotropy for the same device. The domains divert the direction of current flow, resulting in a direction dependent resistance. We also show that the modulation can be significant and that in some cases up to 95% of the current is modulated over the channels. The orientation and distribution of the SrTiO3 structural domains change between different cooldowns of the same device or when electric fields are applied, affecting the device behavior. Our results, highlight the importance of substrate physics, and in particular, the role of structural domains, in controlling electronic properties of LaAlO3/SrTiO3 devices. Further, these results point to new research directions, exploiting the STO domains ability to divert or even carry current.

cond-mat.mtrl-sci

Control of polymorphism in coronene by the application of magnetic fields

Coronene, a polyaromatic hydrocarbon, has been crystallized for the first time in a different polymorph using a crystal growth method that utilizes magnetic fields to access a unit cell configuration that was hitherto unknown. Crystals grown in magnetic field of 1 T are larger, have a different appearance to those grown in zero field and retain their structure in ambient conditions. We identify the new form, beta-coronene, as the most stable at low temperatures. As a result of the new supramolecular configuration we report significantly altered electronic, optical and mechanical properties.

cond-mat.mtrl-sci

Quantum longitudinal and Hall transport at the LaAlO3/SrTiO3 interface at low electron densities

We examined the magneto-transport behavior of electrons confined at the conducting LaAlO3/SrTiO3 interface in the low sheet carrier density regime. We observed well resolved Shubnikov-de Haas quantum oscillations in the longitudinal resistance, and a plateau-like structure in the Hall conductivity. The Landau indices of the plateaus in the Hall conductivity data show spacing close to 4, in units of the quantum of conductance. These experimental features can be explained by a magnetic breakdown transition, which quantitatively explains the area, structure, and degeneracy of the measured Fermi surface.

cond-mat.mtrl-sci

Locally enhanced conductivity due to the tetragonal domain structure in LaAlO$_{3}$/SrTiO$_{3}$ heterointerfaces

The ability to control materials properties through interface engineering is demonstrated by the appearance of conductivity at the interface of certain insulators, most famously the {001} interface of the band insulators LaAlO$_{3}$ and TiO$_{2}$-terminated SrTiO$_{3}$ (STO). Transport and other measurements in this system show a plethora of diverse physical phenomena. To better understand the interface conductivity, we used scanning superconducting quantum interference device microscopy to image the magnetic field locally generated by current in an interface. At low temperature, we found that the current flowed in conductive narrow paths oriented along the crystallographic axes, embedded in a less conductive background. The configuration of these paths changed on thermal cycling above the STO cubic-to-tetragonal structural transition temperature, implying that the local conductivity is strongly modified by the STO tetragonal domain structure. The interplay between substrate domains and the interface provides an additional mechanism for understanding and controlling the behaviour of heterostructures.

cond-mat.mtrl-sci

Tunable Coupling of Two-Dimensional Superconductors in Bilayer SrTiO3 Heterostructures

Interlayer coupling effects between high mobility two-dimensional superconductors are studied in bilayer delta-doped SrTiO3 heterostructures. By tuning the undoped SrTiO3 spacer layer between the dopant planes, clear tunable coupling is demonstrated in the variation of the sheet carrier density, Hall mobility, superconducting transition temperature, and the temperature- and angle-dependences of the superconducting upper critical field. Systematic variation is found between one effective (merged) two-dimensional superconductor to two decoupled two-dimensional superconductors. In the intermediate coupled regime, a crossover is observed due to coupling arising from inter-sub-band interactions.

cond-mat.supr-con

Critical thickness for ferromagnetism in LaAlO3/SrTiO3 heterostructures

In heterostructures of LaAlO3 (LAO) and SrTiO3 (STO), two nonmagnetic insulators, various forms of magnetism have been observed [1-7], which may [8, 9] or may not [10] arise from interface charge carriers that migrate from the LAO to the interface in an electronic reconstruction [11]. We image the magnetic landscape [5] in a series of n-type samples of varying LAO thickness. We find ferromagnetic patches that appear only above a critical thickness, similar to that for conductivity [12]. Consequently we conclude that an interface reconstruction is necessary for the formation of magnetism. We observe no change in ferromagnetism with gate voltage, and detect ferromagnetism in a non-conducting p-type sample, indicating that the carriers at the interface do not need to be itinerant to generate magnetism. The fact that the ferromagnetism appears in isolated patches whose density varies greatly between samples strongly suggests that disorder or local strain induce magnetism in a population of the interface carriers.

cond-mat.str-el

Control of electronic conduction at an oxide heterointerface using surface polar adsorbates

The transfer of electrons between a solid surface and adsorbed atomic or molecular species is fundamental in natural and synthetic processes, being at the heart of most catalytic reactions and many sensors. In special cases, metallic conduction can be induced at the surface of, for example, Si-terminated SiC1, or mixed-terminated ZnO2, in the presence of a hydrogen adlayer. Generally, only the surface atoms are significantly affected by adsorbates. However, remotely changing electronic states far from the adsorbed layer is possible if these states are electrostatically coupled to the surface. Here we show that the surface adsorption of common solvents such as acetone, ethanol, and water can induce a large change (factor of three) in the conductivity at the buried interface between SrTiO3 substrates and LaAlO3 thin films3-8. This phenomenon is observed only for polar solvents. Our result provides experimental evidence that adsorbates at the LaAlO3 surface induce accumulation of electrons at the LaAlO3/SrTiO3 interface, suggesting a general polarization-facilitated electronic transfer mechanism, which can be used for sensor applications.

cond-mat.mtrl-sci

Built-in and induced polarization across LaAlO$_3$/SrTiO$_3$ heterojunctions

Ionic crystals terminated at oppositely charged polar surfaces are inherently unstable and expected to undergo surface reconstructions to maintain electrostatic stability. Essentially, an electric field that arises between oppositely charged atomic planes gives rise to a built-in potential that diverges with thickness. In ultra thin film form however the polar crystals are expected to remain stable without necessitating surface reconstructions, yet the built-in potential has eluded observation. Here we present evidence of a built-in potential across polar \lao ~thin films grown on \sto ~substrates, a system well known for the electron gas that forms at the interface. By performing electron tunneling measurements between the electron gas and a metallic gate on \lao ~we measure a built-in electric field across \lao ~of 93 meV/\AA. Additionally, capacitance measurements reveal the presence of an induced dipole moment near the interface in \sto, illuminating a unique property of \sto ~substrates. We forsee use of the ionic built-in potential as an additional tuning parameter in both existing and novel device architectures, especially as atomic control of oxide interfaces gains widespread momentum.

cond-mat.mtrl-sci