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G. Christiani

Publications and source records attributed to G. Christiani.

At least 19 recordsLinked to original sources

Evolution of spin excitations in superconducting La$_{2-x}$Ca$_{x}$CuO$_{4-\delta}$ from the underdoped to the heavily overdoped regime

We investigate high-energy spin excitations in hole-doped La$_{2-x}$Ca$_{x}$CuO$_{4-\delta}$ films across a broad Ca doping range $x = 0.05-0.50$ using resonant inelastic x-ray scattering (RIXS). Polarization analysis and incident-photon energy detuning measurements confirm the persistence of collective paramagnon excitations up to $x = 0.50$. Consistent with previous studies on other cuprate families, we observe a pronounced crossover near $x = 0.15$, where paramagnon spectral weight is transferred to incoherent spin-flip excitations associated with the particle-hole continuum. The overall behavior of paramagnons in LCCO resembles that in other hole-doped cuprates and appears insensitive to the persistence of superconductivity at high doping levels in LCCO - up to at least $x = 0.50$, as demonstrated in prior work. These findings support the view that high-energy magnetic excitations probed by RIXS are not a major contributor to superconducting pairing, in line with theories of spin-fluctuation mediated superconductivity.

cond-mat.supr-con

Imprinted atomic displacements drive spin-orbital order in a vanadate perovskite

Perovskites with the generic composition ABO$_3$ exhibit an enormous variety of quantum states such as magnetism, orbital order, ferroelectricity and superconductivity. Their flexible and comparatively simple structure allows for facile chemical substitution and cube-on-cube combination of different compounds in atomically sharp epitaxial heterostructures. However, already in the bulk, the diverse physical properties of perovskites and their anisotropy are determined by small deviations from the ideal perovskite structure, which are difficult to control. Here we show that directional imprinting of atomic displacements in the antiferromagnetic Mott insulator YVO$_3$ is achieved by depositing epitaxial films on different facets of an isostructural substrate. These facets were chosen such that other control parameters, including strain and polarity mismatch with the overlayer, remain unchanged. We use polarized Raman scattering and spectral ellipsometry to detect signatures of staggered orbital and magnetic order, and demonstrate distinct spin-orbital ordering patterns on different facets. These observations can be attributed to the influence of specific octahedral rotation and cation displacement patterns, which are imprinted by the substrate facet, on the covalency of the bonds and the superexchange interactions in YVO$_3$. Well beyond established strain-engineering strategies, our results show that substrate-induced templating of lattice distortion patterns constitutes a powerful pathway for materials design.

cond-mat.mtrl-sci

Interplay between electronic and lattice superstructures in La$_{2-x}$Ca$_{x}$CuO$_{4}$

Complex oxides are well known to develop oxygen ordering patterns with well defined periodicities, but their interplay with electronic correlations remains largely unexplored. Here, we report resonant and non-resonant x-ray diffraction data indicating a four-unit-cell periodic superstructure related to oxygen vacancy ordering in La$_{2-x}$Ca$_{x}$CuO$_{4}$ films with doping levels from the underdoped ($x = 0.15$) to the extremely overdoped ($x = 0.50$) regime. Whereas the lattice superstructure is temperature independent up to 300 K, a strongly temperature dependent electronic charge density wave (CDW) is observed in the underdoped and slightly overdoped regimes ($x\leq0.20$). The periodicity, in-plane and out-of-plane correlation lengths of the CDW are locked in by the lattice superstructure. Our results highlight the necessity to consider lattice and electronic energetics on equal footing in the high-temperature oxygen-disordered phase to explain oxygen ordering phenomena in complex oxides.

cond-mat.str-el

Coupling of electronic and structural degrees of freedom in vanadate superlattices

Heterostructuring provides different ways to manipulate the orbital degrees of freedom and to tailor orbital occupations in transition metal oxides. However, the reliable prediction of these modifications remains a challenge. Here, we present a detailed investigation of the relationship between the crystal and electronic structure in YVO$_3$-LaAlO$_3$ superlattices by combining ab initio theory, scanning transmission electron microscopy, and x-ray diffraction. Density functional theory simulations including an on-site Coulomb repulsion term, accurately predict the crystal structure and in conjunction with x-ray diffraction, provide an explanation for the lifting of degeneracy of the vanadium $d_{xz}$ and $d_{yz}$ orbitals, that was recently observed in this system. In addition, we unravel the combined effects of electronic confinement and octahedral connectivity by disentangling their impact from that of epitaxial strain. Our results demonstrate that the specific orientation of the substrate and the thickness of the YVO$_3$ slabs in the multilayer, can be utilized to reliably engineer orbital polarization.

cond-mat.str-el

Control of the metal-insulator transition in NdNiO$_3$ thin films through the interplay between structural and electronic properties

Heteroepitaxy offers a new type of control mechanism for the crystal structure, the electronic correlations, and thus the functional properties of transition-metal oxides. Here, we combine electrical transport measurements, high-resolution scanning transmission electron microscopy (STEM), and density functional theory (DFT) to investigate the evolution of the metal-to-insulator transition (MIT) in NdNiO$_3$ films as a function of film thickness and NdGaO$_3$ substrate crystallographic orientation. We find that for two different substrate facets, orthorhombic (101) and (011), modifications of the NiO$_6$ octahedral network are key for tuning the transition temperature $T_{\text{MIT}}$ over a wide temperature range. A comparison of films of identical thickness reveals that growth on [101]-oriented substrates generally results in a higher $T_{\text{MIT}}$, which can be attributed to an enhanced bond-disproportionation as revealed by the DFT+$U$ calculations, and a tendency of [011]-oriented films to formation of structural defects and stabilization of non-equilibrium phases. Our results provide insights into the structure-property relationship of a correlated electron system and its evolution at microscopic length scales and give new perspectives for the epitaxial control of macroscopic phases in metal-oxide heterostructures.

cond-mat.mtrl-sci

Approaching two-dimensional superconductivity in ultrathin DyBa$_2$Cu$_3$O$_{7-δ}$

The temperature dependence of the superfluid density $ρ_s(T)$ has been measured for a series of ultrathin MBE-grown DyBa$_2$Cu$_3$O$_{7-δ}$ superconducting (SC) films by sub-mm wave interferometry combined with time-domain THz spectroscopy and IR ellipsometry. We find that all films 10 u.c. and thicker show the same universal temperature dependence of $ρ_s(T)$, which follows the critical behavior characteristic of single crystal YBa$_2$Cu$_3$O$_{7-δ}$ as $T$ approaches $T_c$. In 7 u.c. thick films, $ρ_s(T)$ declines steeply upon approaching $T_c$, as expected for the Berezinskii-Kosterlitz-Thouless vortex unbinding transition. Our analysis provides evidence for a sharply defined 4 u.c. non-SC interfacial layer, leaving a quasi-2D SC layer on top. We propose that the SC state in this interfacial layer is suppressed by competing (possibly charge) order.

cond-mat.supr-con

Inhomogeneous ferromagnetism mimics signatures of the topological Hall effect in SrRuO$_3$ films

Topological transport phenomena in magnetic materials are a major topic of current condensed matter research. One of the most widely studied phenomena is the ``topological Hall effect'' (THE), which is generated via spin-orbit interactions between conduction electrons and topological spin textures such as skyrmions. We report a comprehensive set of Hall effect and magnetization measurements on epitaxial films of the prototypical ferromagnetic metal SrRuO$_3$ the magnetic and transport properties of which were systematically modulated by varying the concentration of Ru vacancies. We observe Hall effect anomalies that closely resemble signatures of the THE, but a quantitative analysis demonstrates that they result from inhomogeneities in the ferromagnetic magnetization caused by a non-random distribution of Ru vacancies. As such inhomogeneities are difficult to avoid and are rarely characterized independently, our results call into question the identification of topological spin textures in numerous prior transport studies of quantum materials, heterostructures, and devices. Firm conclusions regarding the presence of such textures must meet stringent conditions such as probes that couple directly to the non-collinear magnetization on the atomic scale.

cond-mat.str-el

Electronic and vibrational signatures of ruthenium vacancies in Sr$_2$RuO$_4$ thin films

The synthesis of stoichiometric Sr$_2$RuO$_4$ thin films has been a challenge because of the high volatility of ruthenium oxide precursors, which gives rise to ruthenium vacancies in the films. Ru vacancies greatly affect the transport properties and electronic phase behavior of Sr$_2$RuO$_4$, but their direct detection is difficult due to their atomic dimensions and low concentration. We applied polarized X-ray absorption spectroscopy at the oxygen K-edge and confocal Raman spectroscopy to Sr$_2$RuO$_4$ thin films synthesized under different conditions. The results show that these methods can serve as sensitive probes of the electronic and vibrational properties of Ru vacancies, respectively. The intensities of the vacancy-related spectroscopic features extracted from these measurements are well correlated with the transport properties of the films. The methodology introduced here can thus help to understand and control the stoichiometry and transport properties in films of Sr$_2$RuO$_4$ and other ruthenates.

cond-mat.supr-con

Observation of superconducting current in a mesa-heterostructure with an interlayer of the strontium iridate film with strong spin-orbit interaction

The superconducting current has been observed in mesa-heterostructures Nb/Au/Sr2IrO4/YBa2Cu3Ox with Sr2IrO4 interlayer thickness d=5 and 7 nm and in-plane sizes L=10-50 mcm. A strontium iridate, Sr2IrO4, is known as a canted antiferromagnetic insulator at low temperatures and characterized also by the strong spin-orbit interaction due to the impact of the IrO2 plane. The superconducting critical current density jC =0.3 A/cm^2 for the case d=7 nm was observed at T=4.2K. The temperature dependences of the superconducting critical current IC(T) and the voltage position on the I-V curve of the gap singularity of the Nb electrode show an increase with decreasing temperature and corresponds to the expected BCS behavior of the Nb energy gap. The critical current is very sensitive to the influence of an external magnetic field and reduces twice at an external magnetic field (H=0.2 Oe for L=40-50 mcm) comparable with the earth magnetic field; The magnetic field dependence IC(H) at low H was narrower than the Fraunhofer pattern about 1.5 times. Both the integer and fractional Shapiro steps at voltages V=(m/n)(h/2e)fe were observed under microwave radiation at frequencies fe=38 GHz and fe=50 GHz. Fractional Shapiro steps (m/n=1/2, 3/2) may point on the presence of the second harmonic in the superconducting current-phase relation.

cond-mat.supr-con

Stabilization of three-dimensional charge order in YBa$_2$Cu$_3$O$_{6+x}$ via epitaxial growth

Incommensurate charge order (CO) has been identified as the leading competitor of high-temperature superconductivity in all major families of layered copper oxides, but the perplexing variety of CO states in different cuprates has confounded investigations of its impact on the transport and thermodynamic properties. The three-dimensional (3D) CO observed in YBa$_2$Cu$_3$O$_{6+x}$ in high magnetic fields is of particular interest, because quantum transport measurements have revealed detailed information about the corresponding Fermi surface. Here we use resonant X-ray scattering to demonstrate 3D-CO in underdoped YBa$_2$Cu$_3$O$_{6+x}$ films grown epitaxially on SrTiO$_3$ in the absence of magnetic fields. The resonance profiles indicate that Cu sites in the charge-reservoir layers participate in the CO state, and thus efficiently transmit CO correlations between adjacent CuO$_2$ bilayer units. The results offer fresh perspectives for experiments elucidating the influence of 3D-CO on the electronic properties of cuprates without the need to apply high magnetic fields.

cond-mat.str-el

Tailoring the electronic properties of Ca$_2$RuO$_4$ via epitaxial strain

We report the synthesis of Ca$_2$RuO$_4$ thin films on NdCaAlO$_{4}$ (110), LaAlO$_3$ (100) and LaSrAlO$_4$ (001) substrates and show that epitaxial strain induces a transition from the Mott-insulating phase of bulk Ca$_2$RuO$_4$ into a metallic phase. Magnetometry and spin-polarized neutron reflectometry reveal a low-temperature, small-moment ferromagnetic state in metallic Ca$_2$RuO$_4$ films.

cond-mat.str-el

Digital modulation of the nickel valence state in a cuprate-nickelate heterostructure

Layer-by-layer oxide molecular beam epitaxy has been used to synthesize cuprate-nickelate multilayer structures of composition (La$_2$CuO$_4$)$_m$/LaO/(LaNiO$_3$)$_n$. In a combined experimental and theoretical study, we show that these structures allow a clean separation of dopant and doped layers. Specifically, the LaO layer separating cuprate and nickelate blocks provides an additional charge that, according to density functional theory calculations, is predominantly accommodated in the interfacial nickelate layers. This is reflected in an elongation of bond distances and changes in valence state, as observed by scanning transmission electron microscopy and x-ray absorption spectroscopy. Moreover, the predicted charge disproportionation in the nickelate interface layers leads to a thickness-dependent metal-to-insulator transition for $n=2$, as observed in electrical transport measurements. The results exemplify the perspectives of charge transfer in metal-oxide multilayers to induce doping without introducing chemical and structural disorder.

cond-mat.str-el

Transfer of magnetic order and anisotropy through epitaxial integration of 3$d$ and 4$f$ spin systems

Resonant x-ray scattering at the Dy $M_5$ and Ni $L_3$ absorption edges was used to probe the temperature and magnetic field dependence of magnetic order in epitaxial LaNiO$_3$-DyScO$_3$ superlattices. For superlattices with 2 unit cell thick LaNiO$_3$ layers, a commensurate spiral state develops in the Ni spin system below 100 K. Upon cooling below $T_{ind} = 18$ K, Dy-Ni exchange interactions across the LaNiO$_3$-DyScO$_3$ interfaces induce collinear magnetic order of interfacial Dy moments as well as a reorientation of the Ni spins to a direction dictated by the strong magneto-crystalline anisotropy of Dy. This transition is reversible by an external magnetic field of 3 T. Tailored exchange interactions between rare-earth and transition-metal ions thus open up new perspectives for the manipulation of spin structures in metal-oxide heterostructures and devices.

cond-mat.str-el

Comparative study of LaNiO$_3$/LaAlO$_3$ heterostructures grown by pulsed laser deposition and oxide molecular beam epitaxy

Variations in growth conditions associated with different deposition techniques can greatly affect the phase stability and defect structure of complex oxide heterostructures. We synthesized superlattices of the paramagnetic metal LaNiO3 and the large band gap insulator LaAlO3 by atomic layer-by-layer molecular beam epitaxy (MBE) and pulsed laser deposition (PLD) and compared their crystallinity, microstructure as revealed by high-resolution transmission electron microscopy images and resistivity. The MBE samples show a higher density of stacking faults, but smoother interfaces and generally higher electrical conductivity. Our study identifies the opportunities and challenges of MBE and PLD growth and serves as a general guide for the choice of deposition technique for perovskite oxides.

cond-mat.str-el

Long-range charge density wave proximity effect at cuprate-manganate interfaces

The interplay between charge density waves (CDWs) and high-temperature superconductivity is currently under intense investigation. Experimental research on this issue is difficult because CDW formation in bulk copper-oxides is strongly influenced by random disorder, and a long-range-ordered CDW state in high magnetic fields is difficult to access with spectroscopic and diffraction probes. Here we use resonant x-ray scattering in zero magnetic field to show that interfaces with the metallic ferromagnet La$_{2/3}$Ca$_{1/3}$MnO$_3$ greatly enhance CDW formation in the optimally doped high-temperature superconductor YBa$_2$Cu$_3$O$_{6+δ}$ ($\bf δ\sim 1$), and that this effect persists over several tens of nm. The wavevector of the incommensurate CDW serves as an internal calibration standard of the charge carrier concentration, which allows us to rule out any significant influence of oxygen non-stoichiometry, and to attribute the observed phenomenon to a genuine electronic proximity effect. Long-range proximity effects induced by heterointerfaces thus offer a powerful method to stabilize the charge density wave state in the cuprates, and more generally, to manipulate the interplay between different collective phenomena in metal oxides.

cond-mat.str-el

Interfacial roughness and proximity effects in superconductor/ferromagnet CuNi/Nb heterostructures

We report an investigation of the structural and electronic properties of hybrid superconductor/ferromagnet (S/F) bilayers of composition Nb/Cu$_{60}$Ni$_{40}$ prepared by magnetron sputtering. X-ray and neutron reflectometry show that both the overall interfacial roughness and vertical correlations of the roughness of different interfaces are lower for heterostructures deposited on Al$_2$O$_3$(1$\bar{1}$02) substrates than for those deposited on Si(111). Mutual inductance experiments were then used to study the influence of the interfacial roughness on the superconducting transition temperature, $T_C$. These measurements revealed a $\sim$ 4% higher $T_C$ in heterostructures deposited on Al$_2$O$_3$, compared to those on Si. We attribute this effect to a higher mean-free path of electrons in the S layer, caused by a suppression of diffusive scattering at the interfaces. However, the dependence of the $T_C$ on the thickness of the ferromagnetic layer is not significantly different in the two systems, indicating a weak influence of the interfacial roughness on the transparency for Cooper pairs.

cond-mat.str-el

Interrelation of epitaxial strain and oxygen deficiency in La0.7Ca0.3MnO3-δ thin films

The interrelation between the epitaxial strain and oxygen deficiency in La0.7Ca0.3MnO3-δ thin films was studied in terms of structural and functional properties. The films with a thickness of 1000Å were prepared using a PLD system equipped with a RHEED facility and a pyrometric film temperature control. The epitaxial strain and the oxygen deficiency in the samples were systematically modified using three different substrates: SrTiO3, (LaAlO3)0.3-(Sr2AlTaO6)0.7 and LaSrAlO4, and four different oxygen pressures during film growth ranging from 0.27mbar to 0.1mbar. It could be demonstrated that the oxygen incorporation depends on the epitaxial strain: oxygen vacancies were induced to accommodate tensile strain whereas the compressive strain suppressed the generation of oxygen vacancies.

cond-mat.mtrl-sci

Dimensionality-tuned electronic structure of nickelate superlattices explored by soft-x-ray angle resolved photoelectron spectroscopy

The electronic and magnetic properties of epitaxial LaNiO3/LaAlO3 superlattices can be tuned by layer thickness and substrate-induced strain. Here, we report on direct measurements of the k-space-resolved electronic structure of buried nickelate layers in superlattices under compressive strain by soft x-ray photoemission. After disentangling strong extrinsic contributions to the angle-dependent signal caused by photoelectron diffraction, we are able to extract Fermi surface information from our data. We find that with decreasing LaNiO3 thickness down to two unit cells (2 uc) quasiparticle coherence becomes strongly reduced, in accord with the dimension-induced metal-to-insulator transition seen in transport measurements. Nonetheless, on top of a strongly incoherent background a residual Fermi surface can be identified in the 2 uc superlattice whose nesting properties are consistent with the spin-density wave (SDW) instability recently reported. The overall behavior of the Ni 3d spectra and the absence of a complete gap opening indicate that the SDW phase is dominated by strong order parameter fluctuations.

cond-mat.str-el