Superconducting performance is tunable not only via chemical modification or defect engineering, but also through external parameters such as pressure, though this method remains less readily accessible. In this work, we study how compression influences vortex dynamics and critical currents in an iron-based superconductor. Specifically, we perform magnetization measurements using an off-the-shelf pressure cell to investigate the effects of hydrostatic pressures up to 1.08 GPa on the magnetic properties of BaFe 2(As 0.62P 0.38) 2 crystals across a range of temperatures T and magnetic fields H. Although these pressures minimally affect the superconducting critical temperature, they produce a clear increase in the critical current density Jc(T,H), a pronounced reduction in the rate of thermally activated vortex motion S(T,H), and can change the dominant vortex pinning mechanism. Furthermore, the effects of pressure are irreversible: after pressurization and subsequent release at room temperature, high-density microcracks are observed and the crystals retain their enhanced critical current densities. The second magnetization peak vanishes above 18 K after the pressure cycle, which we attribute to a transition from predominantly delta kappa pinning to a mixed mechanism of delta Tc and surface pinning. Lastly, a threefold increase in Jc, a more than 40% reduction in S at 8 K and 0.5 T, and an expanded elastic-creep region were achieved after 1-2 pressure cycles. These findings demonstrate the potential utility of pressure cycling for improving Jc, which may offer a simpler alternative compared to approaches such as chemical doping or the introduction of artificial pinning centers.
Superconducting performance is tunable not only via chemical modification or defect engineering, but also through external parameters such as pressure, though this method remains less readily accessible. In this work, we study how compression influences vortex dynamics and critical currents in an iron-based superconductor. Specifically, we perform magnetization measurements using an off-the-shelf pressure cell to investigate the effects of hydrostatic pressures up to 1.08 GPa on the magnetic properties of BaFe_2(As_0.62P_0.38)_2 crystals across a range of temperatures T and magnetic fields H. Although these pressures minimally affect the superconducting critical temperature, they produce a clear increase in the critical current density J_c(T,H), a pronounced reduction in the rate of thermally activated vortex motion S(T,H), and can change the dominant vortex pinning mechanism. Furthermore, the effects of pressure are irreversible: after pressurization and subsequent release at room temperature, high-density microcracks are observed and the crystals retain their enhanced critical current densities. The second magnetization peak vanishes above 18 K after the pressure cycle, which we attribute to a transition from predominantly δκ pinning to a mixed mechanism of δT_c and surface pinning. Lastly, a threefold increase in J_c, a more than 40% reduction in S at 8 K and 0.5 T, and an expanded elastic-creep region were achieved after 1-2 pressure cycles. These findings demonstrate the potential utility of pressure cycling for improving J_c, which may offer a simpler alternative compared to approaches such as chemical doping or the introduction of artificial pinning centers.
The electromagnetic properties of type-II superconductors depend on vortices—magnetic flux lines whose motion introduces dissipation that can be mitigated by pinning from material defects. The material disorder landscape is tuned by the choice of materials growth technique and incorporation of impurities that serve as vortex pinning centers. For example, metal organic deposition (MOD) and pulsed laser deposition (PLD) produce high-quality superconducting films with uncorrelated versus correlated disorder, respectively. Here, we study vortex dynamics in PLD-grown EuBa2Cu3Oy films containing varying concentrations of BaHfO3 inclusions and compare our results with those of MOD-grown (Y,Gd)Ba2Cu3Oy films. Despite both systems exhibiting behavior consistent with strong pinning theory, which predicts the critical current density Jc based on vortex trapping by randomly distributed spherical inclusions, we find striking differences in the vortex dynamics owing to the correlated versus uncorrelated disorder. Specifically, we find that the EuBa2Cu3Oy films grown without inclusions exhibit surprisingly slow vortex creep, comparable to the slowest creep rates achieved in (Y,Gd)Ba2Cu3Oy films containing high concentrations of BaHfO3. Whereas adding inclusions to (Y,Gd)Ba2Cu3Oy is effective in slowing creep, BaHfO3 increases creep in EuBa2Cu3Oy even while concomitantly improving Jc. Lastly, we find evidence of variable range hopping and that Jc is maximized at the BaHfO3 concentration that hosts creep of large vortex bundles or a Bose glass state. This study investigates vortex dynamics in pulsed laser deposition-grown EuBa2Cu3Oy films containing varying concentrations of BaHfO3 inclusions, with the results compared to metal organic deposition-grown (Y,Gd)Ba2Cu3Oy films.
Magnetic skyrmions are topologically protected spin textures that are promising candidates for low-power spintronic memory and logic devices. Realizing skyrmion-based devices requires an understanding of how structural disorder affects their stability and transport properties. This study uses Ne$^{+}$ ion irradiation at fluences from $10^{11}$ to $10^{14}$ ions-cm$^{-2}$ to systematically vary defect densities in 80 nm epitaxial FeGe films and quantify the resulting modifications to magnetic phase boundaries and electronic scattering. Temperature- and field-dependent Hall measurements reveal that increasing disorder progressively extends the topological Hall signal from a narrow window near 200K in pristine films down to 4K at the highest fluence, with peak amplitude more than doubling. Simultaneously, the anomalous Hall effect transitions from quadratic Berry curvature scaling to linear skew scattering behavior, with the skew coefficient increasing threefold. These results establish quantitative correlations between defect concentration, skyrmion phase space, and transport mechanisms in a chiral magnet. It demonstrates that ion-beam modification provides systematic control over both topological texture stability and electrical detectability.
Tantalum (Ta) has emerged as a promising low-loss material, enabling record coherence times in superconducting qubits. This enhanced performance is largely attributed to its stable native oxide, which may host fewer two-level system (TLS) defects, which are the key contributors to decoherence in superconducting circuits. Nevertheless, aluminum oxide remains the predominant choice for Josephson junction (JJ) barriers in most qubit architectures. Here, we investigate techniques for forming high-quality oxide layers on α-phase tantalum films to develop tantalum-oxide JJ barriers. We explore thermal oxidation in a tube furnace, rapid thermal annealing, and plasma oxidation of both room-temperature and heated Ta films, characterize the resulting structures using X-ray techniques and electron microscopy, and propose a mechanistic picture of the oxidation pathways. We find that plasma oxidation provides the smoothest Ta_2O_5 layers, is compatible with in situ Ta deposition, and offers thickness control through the annealing temperature, advantageous for JJ fabrication. Lastly, we evaluate methods for growing Ta/TaO_x/Ta trilayers. All trilayers showed c-axis-oriented columnar growth of the bottom Ta layer, with sapphire substrates producing larger, better-aligned grains yet higher dislocation densities than silicon. Nucleation of c-axis-oriented α-Ta on tantalum-oxide required an Nb seed layer, as direct Ta deposition yielded amorphous Ta. These results demonstrate the feasibility of α-Ta/Nb/TaO_x/α-Ta stacks for JJs with clean interfaces.
Disordered iron germanium (FeGe) has recently garnered interest as a testbed for a variety of magnetic phenomena as well as for use in magnetic memory and logic applications. This is partially owing to its ability to host skyrmions and antiskyrmions—nanoscale whirlpools of magnetic moments that could serve as information carriers in spintronic devices. In particular, a tunable skyrmion–antiskyrmion system may be created through precise control of the defect landscape in B20-phase FeGe, motivating the development of methods to systematically tune disorder in this material and understand the ensuing structural properties. To this end, we investigate a route for modifying magnetic properties in FeGe. In particular, we irradiate epitaxial B20-phase FeGe films with 2.8 MeV Au4+ ions, which creates a dispersion of amorphized regions that may preferentially host antiskyrmions at densities controlled by the irradiation fluence. To further tune the disorder landscape, we conduct a systematic electron diffraction study with in situ annealing, demonstrating the ability to recrystallize controllable fractions of the material at temperatures ranging from ∼150 to 250 °C. Finally, we describe the crystallization kinetics using the Johnson–Mehl–Avrami–Kolmogorov model, finding that the growth of crystalline grains is consistent with diffusion-controlled one-to-two dimensional growth with a decreasing nucleation rate.
The sense of touch is fundamental to how we interact with the physical and digital world. Conventional interactive surfaces and tactile interfaces use electronic sensors embedded into objects, however this approach poses serious challenges both for environmental sustainability and a future of truly ubiquitous interaction systems where information is encoded into everyday objects. In this work, we present Biodegradable Interactive Materials: backyard-compostable interactive interfaces that leverage information encoded in material properties. Inspired by natural systems, we propose an architecture that programmatically encodes multidimensional information into materials themselves and combines them with wearable devices that extend human senses to perceive the embedded data. We combine unrefined biological matter from plants and algae like chlorella with natural minerals like graphite and magnetite to produce materials with varying electrical, magnetic, and surface properties. We perform in-depth analysis using physics models, computational simulations, and real-world experiments to characterize their information density and develop decoding methods. Our passive, chip-less materials can robustly encode 12 bits of information, equivalent to 4096 unique classes. We further develop wearable device prototypes that can decode this information during touch interactions using off-the-shelf sensors. We demonstrate sample applications such as customized buttons, tactile maps, and interactive surfaces. We further demonstrate the natural degradation of these interactive materials in degrade outdoors within 21 days and perform a comparative environmental analysis of the benefits of this approach.
Skyrmions and antiskyrmions are nanoscale swirling textures of magnetic moments formed by chiral interactions between atomic spins in magnetic non-centrosymmetric materials and multilayer films with broken inversion symmetry. These quasiparticles are of interest for use as information carriers in next-generation, low-energy spintronic applications. To develop skyrmion-based memory and logic, we must understand skyrmion-defect interactions with two main goals -- determining how skyrmions navigate intrinsic material defects and determining how to engineer disorder for optimal device operation. Here, we introduce a tunable means of creating a skyrmion-antiskyrmion system by engineering the disorder landscape in FeGe using ion irradiation. Specifically, we irradiate epitaxial B20-phase FeGe films with 2.8 MeV Au$^{4+}$ ions at varying fluences, inducing amorphous regions within the crystalline matrix. Using low-temperature electrical transport and magnetization measurements, we observe a strong topological Hall effect with a double-peak feature that serves as a signature of skyrmions and antiskyrmions. These results are a step towards the development of information storage devices that use skyrmions and anitskyrmions as storage bits and our system may serve as a testbed for theoretically predicted phenomena in skyrmion-antiskyrmion crystals.
Reactive inks are an attractive method to selectively pattern metallic features with minimal post-processing. While significant progress has been made developing silver and copper reactive inks for printed electronics, less progress has been made in developing metal reactive inks with properties suitable for structural or magnetic applications. To address this gap, this work introduces particle-free iron and cobalt metal reactive inks to print magnetic iron and cobalt metals. Interestingly, structure analysis of the printed reactive inks showed that the iron reactive ink produced fully amorphous iron and the cobalt reactive ink produced nanocrystals dispersed in an amorphous matrix. This work also demonstrates two combinatorial methods of printing these inks: by mixing the two inks together to produce amorphous iron-cobalt alloys and by spatially patterning the iron and cobalt monometallic inks to achieve control over both the local composition and the correlated atomic structure. Triiron dodecacarbonyl and dicobalt octacarbonyl are used as the iron and cobalt metal precursors, respectively, because these zerovalent metal complexes directly decompose to metal and carbon monoxide gas. The printed metals' elemental and chemical compositions were evaluated using energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, and Mossbauer effect spectroscopy showing that the amorphous phases are likely stabilized by either remnant carbonyl bonds from incomplete decomposition of the metal carbonyl or residual octylamine solvent interacting with the metal atoms. Additional characterization includes resistivity measurements to verify metallic conductivity, nanoindentation to quantify hardness, and magnetometry studies to quantify the magnetic performance. As a demonstration, the Fe and Co reactive inks were sequentially printed in a combinatorial layer-by-layer manner to produce a vertically graded iron and cobalt line, as well as a matrix of nanocrystalline cobalt dots on an amorphous iron film. Overall, this work introduces a method to directly print continuous, amorphous, magnetic, and structural alloys at moderate temperatures from a particle-free reactive ink.
Iron-based 1111-type superconductors display high critical temperatures and relatively high critical current densities Jc. The typical approach to increasing Jc is to introduce defects to control dissipative vortex motion. However, when optimized, this approach is theoretically predicted to be limited to achieving a maximum Jc of only ∼30% of the depairing current density Jd, which depends on the coherence length and the penetration depth. Here we dramatically boost Jc in SmFeAsO1-xHx films using a thermodynamic approach aimed at increasing Jd and incorporating vortex pinning centres. Specifically, we reduce the penetration depth, coherence length and critical field anisotropy by increasing the carrier density through high electron doping using H substitution. Remarkably, the quadrupled Jd reaches 415 MA cm-2, a value comparable to cuprates. Finally, by introducing defects using proton irradiation, we obtain high Jc values in fields up to 25 T. We apply this method to other iron-based superconductors and achieve a similar enhancement of current densities.
In type-II superconductors exposed to magnetic fields between upper and lower critical values, $H_{c1}$ and $H_{c2}$, penetrating magnetic flux forms a lattice of vortices whose motion can induce dissipation. Consequently, the magnetization $M$ of superconductors is typically progressively weakened with increasing magnetic field $B \propto n_v$ (for vortex density $n_v$). However, some materials exhibit a non-monotonic $M(B)$, presenting a maximum in $M$ at what is known as the second magnetization peak. This phenomenon appears in most classes of superconductors, including low $T_c$ materials, iron-based, and cuprates, complicating pinpointing its origin and garnering intense interest. Here, we report on vortex dynamics in optimally doped and overdoped HgBa$_2$CuO$_{4+x}$ crystals, with a focus on a regime in which plastic deformations of the vortex lattice govern magnetic properties. Specifically, we find that both crystals exhibit conspicuous second magnetization peaks and, from measurements of the field- and temperature- dependent vortex creep rates, identify and characterize phase boundaries between elastic and plastic vortex dynamics, as well as multiple previously unreported transitions within the plastic flow regime. We find that the second magnetization peak coincides with the elastic-to-plastic crossover for a very small range of high fields, and a sharp crossover within the plastic flow regime for a wider range of lower fields. We find evidence that this transition in the plastic flow regime is due to a dimensional crossover, specifically a transition from 3D to 2D plastic dynamics.
Nitride perovskites are an emerging class of materials that have been predicted to display a range of interesting physics and functional properties, but they are under-explored due to the difficulty of synthesizing oxygen-free nitrides. LaWN3, recently reported as the first oxygen-free nitride perovskite, exhibited polar symmetry and a large piezoelectric coefficient. However, the predicted ferroelectric switching was hindered by large leakage current, which motivates better understanding of its electronic structure and optical properties. Here, we study the structure and optoelectronic properties of thin film LaWN3 in greater detail, employing combinatorial techniques to correlate these properties with cation stoichiometry. We report a two-step synthesis that utilizes a more common RF substrate bias instead of a nitrogen plasma source, yielding nanocrystalline films that are crystallized by ex-situ annealing. We investigate the structure and composition of these films, finding polycrystalline La-rich and highly textured W-rich films. The optical absorption onset and temperature- and magnetic field-dependent resistivity are consistent with semiconducting behavior and are highly sensitive to cation stoichiometry, which may be related to amorphous impurities: metallic W or WNx in W-rich samples and insulating La2O3 in La-rich samples. The fractional magnetoresistance is linear and small, consistent with defect scattering, and a W-rich sample has n-type carriers with high densities and low mobilities. We demonstrate a photoresponse in LaWN3: the resistivity of a La-rich sample is enhanced by 28% at low temperature, likely due to a defect trapping mechanism. The physical properties of LaWN3 are highly sensitive to cation stoichiometry, like many oxide perovskites, which therefore calls for precise composition control to utilize the interesting properties observed in this nitride perovskite.
Large spin-orbit torques (SOTs) generated by topological materials and heavy metals interfaced with ferromagnets are promising for next-generation magnetic memory and logic devices. SOTs generated from y spin originating from spin Hall and Edelstein effects can realize field-free magnetization switching only when the magnetization and spin are collinear. Here we circumvent the above limitation by utilizing unconventional spins generated in a MnPd3 thin film grown on an oxidized silicon substrate. We observe conventional SOT due to y spin, and out-of-plane and in-plane anti-damping-like torques originated from z spin and x spin, respectively, in MnPd3/CoFeB heterostructures. Notably, we have demonstrated complete field-free switching of perpendicular cobalt via out-of-plane anti-damping-like SOT. Density functional theory calculations show that the observed unconventional torques are due to the low symmetry of the (114)-oriented MnPd3 films. Altogether our results provide a path toward realization of a practical spin channel in ultrafast magnetic memory and logic devices.
The minority carrier lifetime in B-doped Czochralski (Cz) Si declines upon carrier injection due to light-induced degradation (LID), which is attributed to the formation of a recombination-active boron-oxygen complex. Ga-doped Cz Si does not undergo LID. Previously, we showed that B-doped Cz Si undergoes a transition from paramagnetic to diamagnetic due to LID. Herein, we show that Ga-doped Cz Si remains paramagnetic upon carrier injection. This suggests that either the shallow hole traps that are formed in B-doped Cz Si are absent in Ga-doped Cz Si, or the negative-U centers in Ga-doped Cz Si do not transform into a recombination-active configuration, because the shallow acceptor trap state is shallower than the Ga acceptor level in the forbidden gap. In contrast to B-doped Cz Si, the defect signatures in Ga-doped Cz Si do not change upon light exposure, as detected by both electron paramagnetic resonance and deep-level transient spectroscopy.
Nitride perovskites have only been experimentally realized in very few cases despite the widespread existence and commercial importance of perovskite materials. From oxide perovskites used in ultrasonics to halide perovskites that have revolutionized the photovoltaics industry, the discovery of new perovskite materials has historically impacted a wide number of fields. Here, we add two new perovskites, CeWN3 and CeMoN3, to the list of experimentally realized perovskite nitrides using high-throughput computational screening and subsequent high-throughput thin film growth techniques. Candidate compositions are first down-selected using a tolerance factor and then thermochemical stability. A novel competing fluorite-family phase is identified for both material systems, which we hypothesize is a transient intermediate phase that crystallizes during the evolution from an amorphous material to a stable perovskite. Different processing routes to overcome the competing fluorite phase and obtain phase-pure nitride perovskites are demonstrated for the CeMoN3-x and CeWN3-x material systems, which provide a starting point for the development of future nitride perovskites. Additionally, we find that these new perovskite phases have interesting low-temperature magnetic behavior: CeMoN3-x orders antiferromagnetically below TN ≈ 8 K with indications of strong magnetic frustration, while CeWN3-x exhibits no long-range order down to T = 2 K but has strong antiferromagnetic correlations. This work demonstrates the importance and effectiveness of using high-throughput techniques, both computational and experimental: they are integral to optimize the process of realizing two entirely novel nitride perovskites.
We examine the DC and radio frequency (RF) response of superconducting transmission line resonators comprised of very thin NbTiN films, <12 nm in thickness, in the high-temperature limit, where the photon energy is less than the thermal energy. The resonant frequencies of these superconducting resonators show a significant nonlinear response as a function of RF input power, which can approach a frequency shift of Δf=−0.15% in a −20 dB span in the thinnest film. The strong nonlinear response allows these very thin film resonators to serve as high kinetic inductance parametric amplifiers.
Using electron paramagnetic resonance, we show that under light exposure, nearly all the 1016 boron doping sites in Si degrade to form shallow traps. Of these 1016 traps, only 1012–1013 cm−3 are spin-active and responsible for light-induced degradation.
In superconductors, the motion of vortices introduces unwanted dissipation that is disruptive to applications. Fortunately, material defects can immobilize vortices, acting as vortex pinning centers, which engenders dramatic improvements in superconductor material properties and device operation. This has motivated decades of research into developing methods of tailoring the disorder landscape in superconductors to increase the strength of vortex pinning. Yet, efficacious materials engineering still eludes us. The electromagnetic properties of real (disordered) superconducting materials cannot yet be reliably predicted, such that designing superconductors for applications remains a largely inefficient process of trial and error. This is ultimately due to large gaps in our knowledge of vortex dynamics: the field is challenged by the extremely complex interplay between vortex elasticity, vortex–vortex interactions, and material disorder. In this Perspective, we review obstacles and recent successes in understanding and controlling vortex dynamics in superconducting materials and devices. We further identify major open questions and discuss opportunities for transformative research in the field. This includes improving our understanding of vortex creep, determining and reaching the ceiling for the critical current, advanced microscopy to garner accurate structure–property relationships, frontiers in predictive simulations and the benefits of artificial intelligence, as well as controlling and exploiting vortices in quantum information applications.
YBa2Cu3O7-based coated conductors (CCs) achieve the highest critical current densities (J(c)) of any known superconductor and are a key technology for applications such as rotatory machines, high-field magnets and power transmission. Incorporation of nano-sized non-superconducting second phases as additional vortex pinning centers has been considered the most amenable route to further enhance J(c) at an industrial scale, and has been successfully used in commercial CCs. The resulting pinning landscape is quite complex, with both synergistic and competing interactions among the various types of defects. Particle irradiation, on the other hand, allows for a controlled post-processing incorporation of a well-defined defect morphology. We have previously shown that irradiation with protons and other light ions can further enhance the in-field J(c) in commercial state-of-the-art CCs. Here we develop a combined irradiation process that increases J(c) above values previously achieved by irradiating with only one species. Our new approach involves sequentially irradiating with 250 MeV Au ions and 4 MeV protons. For example, at T similar to 27 K (liquid neon) and mu H-0 similar to 4 T, a region of interest for rotatory machines applications, we obtain J(c) similar to 5 MA cm(-2), which is about 40% higher than the values produced by the individual irradiations. Finally, we conclude that this is due to the synergistic pinning effects of the introduced splayed, non-uniform columnar defects and small clusters.