Mesoscopic transport measurements are underexplored as probes of quasiparticles and their properties in correlated metals. The mixed valence compound YbAl3 exhibits a single-ion Kondo temperature of 670 K, while thermodynamic and transport properties (probed with specific heat, magnetic susceptibility, Hall effect, and resistivity) imply the onset of coherence of heavy fermion quasiparticles at T* 37 K. To characterize these quasiparticles, we utilize mesoscopic techniques familiar from weakly correlated conductors. In lithographically defined nanowires etched from epitaxial films, we observe weak antilocalization magnetoresistance and universal conductance fluctuations, consistent with electronic coherence lengths of tens of nanometers. Additionally, analysis of Johnson-Nyquist noise measurements as a function of bias current reveal, within the context of a range of accepted models, a significant electron-phonon energy loss that increases with decreasing temperature, a finding that we contextualize within the broader properties of YbAl3.
We present a detailed x-ray magnetic circular dichroism (XMCD) study of the magnetic properties of Gddoped EuO thin films, synthesized via molecular-beam epitaxy with Gd doping levels up to over 12%. The impact of Gd doping on the electronic and magnetic behavior of EuO is studied using XMCD and magnetometry. Gd doping significantly enhances the Curie temperature (TC) from 69 K in undoped EuO to over 120 K, driven by increased carrier density, while preserving the high quality of the single-crystalline films. At higher doping levels, a plateau in TC is observed, which is attributed to the formation of Eu-Gd nearest-neighbor pairs that limit dopant activation. We also observe a distinctive "double-dome" structure in the temperature-dependent magnetization, which we attribute to both the ferromagnetic ordering of Eu 4 f moments at lower temperatures and the influence of conduction electrons via 4 f-5d exchange interactions at higher temperatures. These findings provide key insights into the mechanisms of carrier-induced magnetic transitions.
We report evidence for superconductivity with onset temperatures up to 11 K in thin films of the infinite-layer nickelate parent compound NdNiO_{2}. A combination of oxide molecular beam epitaxy and atomic hydrogen reduction yields samples with high crystallinity and low residual resistivities, a substantial fraction of which exhibit superconducting transitions. We survey a large series of samples with a variety of techniques, including electrical transport, scanning transmission electron microscopy, x-ray absorption spectroscopy, and resonant inelastic x-ray scattering, to investigate the possible origins of superconductivity. We propose that superconductivity could be intrinsic to the undoped infinite-layer nickelates but suppressed by disorder due to a possibly sign-changing order parameter, a finding which would necessitate a reconsideration of the nickelate phase diagram. Another possible hypothesis is that the parent materials can be hole doped from randomly dispersed apical oxygen atoms, which would suggest an alternative pathway for achieving superconductivity.
We present time-domain THz spectroscopy of thin films of the heavy-fermion superconductor CeCoIn5. Below the approximate to 40 K Kondo coherence temperature, a narrow Drude-like peak forms, as a result of the forbital-conduction-electron hybridization and the formation of the heavy-fermion state. The complex optical conductivity is analyzed through a Drude model and extended Drude model analysis. Via the extended Drude model analysis, we measure the frequency-dependent scattering rate (1/tau) and effective mass (m*/mb). This scattering rate shows a linear dependence on temperature, which matches the dependence of the resistivity as expected. Nevertheless, the width of the low-frequency Drude peak itself that is set by the renormalized quasi-particle scattering rate (1/tau* = mb/m*tau) shows a T2 dependence. This is the scattering rate that characterizes the relaxation time of the renormalized quasiparticles. This gives evidence for a Fermi liquid state, which in conventional transport experiments is hidden by the strong temperature dependent mass.
The discovery of superconductivity in La3Ni2O7 under pressure has motivated the investigation of a parent spin density wave (SDW) state, which could provide the underlying pairing interaction. Here, we employ resonant soft x-ray scattering and polarimetry on thin films of bilayer La3Ni2O7 to determine that the magnetic structure of the SDW forms unidirectional diagonal spin stripes with moments lying within the NiO2 plane and perpendicular to QSDW, but without evidence of the strong charge disproportionation typically associated with other nickelates. These stripes form anisotropic domains with shorter correlation lengths perpendicular versus parallel to QSDW, revealing nanoscale rotational and translational symmetry breaking analogous to the cuprate and Fe-based superconductors, with possible Bloch-like antiferromagnetic domain walls separating orthogonal domains.
Quantum fluctuations in low-dimensional systems and near quantum phase transitions have significant influences on material properties. Yet, it is difficult to experimentally gauge the strength and importance of quantum fluctuations. Here we provide a resonant inelastic x-ray scattering study of magnon excitations in Mott insulating cuprates. From the thin film of SrCuO_2, single- and bi-magnon dispersions are derived. Using an effective Heisenberg Hamiltonian generated from the Hubbard model, we show that the single-magnon dispersion is only described satisfactorily when including significant quantum corrections stemming from magnon-magnon interactions. Comparative results on La_2CuO_4 indicate that quantum fluctuations are much stronger in SrCuO_2 suggesting closer proximity to a magnetic quantum critical point. Monte Carlo calculations reveal that other magnetic orders may compete with the antiferromagnetic Néel order as the ground state. Our results indicate that SrCuO_2 - due to strong quantum fluctuations - is a unique starting point for the exploration of novel magnetic ground states.
A hallmark of many unconventional superconductors is the presence of many-body interactions that give rise to broken-symmetry states intertwined with superconductivity. Recent resonant soft X-ray scattering experiments report commensurate 3 a 0 charge density wave order in infinite-layer nickelates, which has important implications regarding the universal interplay between charge order and superconductivity in both cuprates and nickelates. Here we present X-ray scattering and spectroscopy measurements on a series of NdNiO 2+ x samples, which reveal that the signatures of charge density wave order are absent in fully reduced, single-phase NdNiO 2 . The 3 a 0 superlattice peak instead originates from a partially reduced impurity phase where excess apical oxygens form ordered rows with three-unit-cell periodicity. The absence of any observable charge density wave order in NdNiO 2 highlights a crucial difference between the phase diagrams of cuprate and nickelate superconductors.
We present an integrated procedure for the synthesis of infinite-layer nickelates using molecular-beam epitaxy with gas-phase reduction by atomic hydrogen. We first discuss challenges in the growth and characterization of perovskite NdNiO3/SrTiO3, arising from post growth crack formation in stoichiometric films. We then detail a procedure for fully reducing NdNiO3 films to the infinite-layer phase, NdNiO2, using atomic hydrogen; the resulting films display excellent structural quality, smooth surfaces, and lower residual resistivities than films reduced by other methods. We utilize the in situ nature of this technique to investigate the role that SrTiO3 capping layers play in the reduction process, illustrating their importance in preventing the formation of secondary phases at the exposed nickelate surface. A comparative bulk- and surface-sensitive study indicates that the formation of a polycrystalline crust on the film surface serves to limit the reduction process.
There is significant technological interest in developing ever faster switching between different electronic and magnetic states of matter. Manipulating properties at terahertz rates requires accessing the intrinsic timescales of both electrons and associated phonons, which is possible with short-pulse photoexcitation. However, in many Mott insulators, the electronic transition is accompanied by the nucleation and growth of percolating domains of the changed lattice structure, leading to empirical timescales dominated by slowly coarsening dynamics. Here we use time-resolved X-ray diffraction and reflectivity measurements to show that the photoinduced insulator-to-metal transition in an epitaxially strained Mott insulating thin film occurs without observable domain formation and coarsening effects, allowing the study of the intrinsic electronic and lattice dynamics. Above a fluence threshold, the initial electronic excitation drives a fast lattice rearrangement, which is followed by a slower electronic evolution into a metastable nonequilibrium state. Microscopic model calculations based on time-dependent dynamical mean-field theory and semiclassical lattice dynamics explain the threshold behaviour and elucidate the delayed onset of the electronic phase transition. This work highlights the importance of combined electronic and structural studies in unravelling the physics of dynamic transitions and the timescales of photoinduced processes. During a photoinduced phase transition, electronic rearrangements are usually faster than lattice ones. Time-resolved measurements now show that the insulator-to-metal transition in a thin-film Mott insulator is preceded by lattice reconfiguration.
With strong correlations between lattice, spin, and charge degrees of freedom, the layered ruthenate Ca2RuO4 has attracted considerable interest over the past few decades due to its metal-insulator transition, antiferromagnetic-to-ferromagnetic transition, metamagnetic transition, and orbital ordering. Much effort has been devoted to manipulating its crystalline structure through epitaxial strain, chemical substitution, and pressure to clarify the underlying many-body physics and related quantum critical phenomena. Here we report a comprehensive proton intercalation study of Ca2RuO4 thin films and investigate their magneto-transport properties arising from structural deformations and carrier doping. It reveals a rich phase diagram with distinct electronic and magnetic ground states. Specifically, with increasing gate voltage during ionic liquid gating, the film first evolves from an insulating state into a metallic state and then gradually turns towards an exotic Mott insulator. Furthermore, we observed an emergent metamagnetic transition from a canted antiferromagnetic to a nearly ferromagnetic state, a characteristic feature conventionally triggered by external magnetic field, but here with electron doping. Our first-principles calculations reveal that these unexpected features could be attributed to the proton evolution-induced synergistic structural distortion and electron doping during ionic liquid gating. Our findings highlight the important role of both lattice and charge degrees of freedom in the intriguing electronic states of Ca2RuO4 and provide an effective approach to uncover different properties in quantum materials.
In bulk Sr_2RuO_4, the strong sensitivity of the superconducting transition temperature T_c to nonmagnetic impurities provides robust evidence for a superconducting order parameter that changes sign around the Fermi surface. In superconducting epitaxial thin-film Sr_2RuO_4, the relationship between T_c and the residual resistivity ρ_0, which in bulk samples is taken to be a proxy for the low-temperature elastic scattering rate, is far less clear. Using high-energy electron irradiation to controllably introduce point disorder into bulk single-crystal and thin-film Sr_2RuO_4, we show that T_c is suppressed in both systems at nearly identical rates. This suggests that part of ρ_0 in films comes from defects that do not contribute to superconducting pairbreaking, and establishes a quantitative link between the superconductivity of bulk and thin-film samples.
Mott metal-insulator transitions possess electronic, magnetic, and structural degrees of freedom promising next generation energy-efficient electronics. We report a previously unknown, hierarchically ordered state during a Mott transition and demonstrate correlated switching of functional electronic properties. We elucidate in-situ formation of an intrinsic supercrystal in a Ca2RuO4 thin film. Machine learning-assisted X-ray nanodiffraction together with electron microscopy reveal multi-scale periodic domain formation at and below the film transition temperature (TFilm ~ 200-250 K) and a separate anisotropic spatial structure at and above TFilm. Local resistivity measurements imply an intrinsic coupling of the supercrystal orientation to the material's anisotropic conductivity. Our findings add an additional degree of complexity to the physical understanding of Mott transitions, opening opportunities for designing materials with tunable electronic properties.
It has been suggested that Ba3In2O6might be a high-Tcsuperconductor. Experimental investigation of the properties of Ba3In2O6was long inhibited by its instability in air. Recently epitaxial Ba3In2O6with a protective capping layer was demonstrated, which finally allows its electronic characterization. The optical bandgap of Ba3In2O6is determined to be 2.99 eV in-the (001) plane and 2.83 eV along thec-axis direction by spectroscopic ellipsometry. First-principles calculations were carried out, yielding a result in good agreement with the experimental value. Various dopants were explored to induce (super-)conductivity in this otherwise insulating material. NeitherA- norB-site doping proved successful. The underlying reason is predominately the formation of oxygen interstitials as revealed by scanning transmission electron microscopy and first-principles calculations. Additional efforts to induce superconductivity were investigated, including surface alkali doping, optical pumping, and hydrogen reduction. To probe liquid-ion gating, Ba3In2O6was successfully grown epitaxially on an epitaxial SrRuO3bottom electrode. So far none of these efforts induced superconductivity in Ba3In2O6,leaving the answer to the initial question of whether Ba3In2O6is a high-Tcsuperconductor to be 'no' thus far.
A hallmark of many unconventional superconductors is the presence of many-body interactions that give rise to broken-symmetry states intertwined with superconductivity. Recent resonant soft X-ray scattering experiments report commensurate 3 a 0 charge density wave order in infinite-layer nickelates, which has important implications regarding the universal interplay between charge order and superconductivity in both cuprates and nickelates. Here we present X-ray scattering and spectroscopy measurements on a series of NdNiO 2+ x samples, which reveal that the signatures of charge density wave order are absent in fully reduced, single-phase NdNiO 2 . The 3 a 0 superlattice peak instead originates from a partially reduced impurity phase where excess apical oxygens form ordered rows with three-unit-cell periodicity. The absence of any observable charge density wave order in NdNiO 2 highlights a crucial difference between the phase diagrams of cuprate and nickelate superconductors.
The growing interest in the growth and study of thin films of low-dimensional metallic delafossites, with the general formula ABO2, is driven by their potential to exhibit electronic and magnetic characteristics that are not accessible in bulk systems. The layered structure of these compounds introduces unique surface states as well as electronic and structural reconstructions, making the investigation of their surface behavior pivotal to understanding their intrinsic electronic structure. In this work, we study the surface phenomena of epitaxially grown PtCoO2, PdCoO2, and PdCrO2 films, utilizing a combination of molecular-beam epitaxy and angle-resolved photoemission spectroscopy. Through precise control of surface termination and treatment, we discover a pronounced 3×3 surface reconstruction in PtCoO2 films and PdCoO2 films, alongside a 2 × 2 surface reconstruction observed in PdCrO2 films. These reconstructions have not been reported in prior studies of delafossites. Furthermore, our computational investigations demonstrate the BO2 surface’s relative stability compared to the A-terminated surface and the significant reduction in surface energy facilitated by the reconstruction of the A-terminated surface. These experimental and theoretical insights illuminate the complex surface dynamics in metallic delafossites, paving the way for future explorations of their distinctive properties in low-dimensional studies.
We conduct local magnetic measurements on superconducting thin-film samples of Sr$\mathrm{_2}$RuO$\mathrm{_4}$ using scanning Superconducting Quantum Interference Device (SQUID) susceptometry. From the diamagnetic response, we extract the magnetic penetration depth, $\lambda$, which exhibits a quadratic temperature dependence at low temperatures. Although a quadratic dependence in high-purity bulk samples has been attributed to non-local electrodynamics, our analysis suggests that in our thin-film samples the presence of scattering is the origin of the quadratic dependence. While we observe micron-scale variations in the diamagnetic response and superconducting transition temperature, the form of the temperature dependence of $\lambda$ is independent of position. Finally, we characterize flux trapping in superconducting rings lithographically fabricated from the thin films, paving the way to systematic device-based tests of the superconducting order parameter in Sr$\mathrm{_2}$RuO$\mathrm{_4}$.
Molecular-beam epitaxy enables ultrathin functional materials to be combined in heterostructures to create emergent phenomena at the interface. Magnetic skyrmions are an example of an exciting phase found in such heterostructures. SrRuO3 and SrRuO3-based heterostructures have been at the center of the debate on whether a hump-like feature appearing in Hall resistivities is sufficient evidence to prove the presence of skyrmions in a material. To address the ambiguity, we synthesize a model heterostructure with engineered Berry curvature that combines, in parallel, a positive anomalous Hall effect (AHE) channel (a Sr0.6Ca0.4RuO3 layer) with a negative AHE channel (a SrRuO3 layer). We demonstrate that the two opposite AHE channels can be combined to artificially reproduce a “hump-like” feature, which closely resembles the hump-like feature typically attributed to the topological Hall effect and the presence of chiral spin textures, such as skyrmions. We compare our heterostructure with a parallel resistor model, where the inputs are the AHE data from individual Sr0.6Ca0.4RuO3 and SrRuO3 films. To check for the presence of skyrmions, we measure the current dependence, angle dependence, and minor loop dependence of Rhump in the heterostructure. Despite the clear hump, no evidence of skyrmions is found.