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U. Starke

Publications and source records attributed to U. Starke.

18 recordsLinked to original sources

Floating zone growth at high oxygen pressures in Ruddlesden-Popper bilayer nickelate Y$_{y}$Sr$_{3-y}$Ni$_{2-x}$Al$_{x}$O$_{7-\delta}$

With the discovery of superconductivity under pressure in the Ruddlesden-Popper (RP) bilayer La$_3$Ni$^{2.5+}_2$O$_7$ and trilayer La$_4$Ni$^{2.66+}_3$O$_{10}$, a new field of nickelate superconductors opened up. In this respect, Sr-Ni-O RP-type phases represent alternative systems that exist with partial cation substitution. We demonstrate that by Y-doping in Sr$_{3}$Ni$_{2-x}$Al$_{x}$O$_7$ (SNAO), as Y$_{y}$Sr$_{3-y}$Ni$_{2-x}$Al$_{x}$O$_7$ (YSNAO), the drawback of an insulating ground state is overcome, and a significant decrease in resistivity is achieved with crystals exhibiting semiconducting behavior. We employ optical floating zone (OFZ) growth at 10 bar oxygen partial pressure to explore the phase formation in a narrow region of Y-Sr-Ni-Al-O and investigate via DFT the general stability of the pure Sr-Ni-O scenario. Using extensive diffraction and spectroscopy, as well as transport and magnetization measurements, the structural, chemical, electrical, and magnetic properties of the as-grown and reduced compounds were investigated. The optimal growth of YSNAO allows for large high quality crystals suitable for neutron studies. In the Al-free growth, a known $n=1$ RP system with Sr$_{1.66}$Y$_{0.33}$NiO$_{4-\delta}$, from which the first single crystals were obtained, was further confirmed, opening the door for future exploration of \textit{A}-site substituted RP-type phases without Ni-site disorder.

cond-mat.supr-con

Lithographically-controlled liquid metal diffusion in graphene: Fabrication and magneto-transport signatures of superconductivity

Metal intercalation in epitaxial graphene enables the emergence of proximity-induced superconductivity and modified quantum transport properties. However, systematic transport studies of intercalated graphene have been hindered by challenges in device fabrication, including processing-induced deintercalation and instability under standard lithographic techniques. Here, we introduce a lithographically controlled intercalation approach that enables the scalable fabrication of gallium-intercalated quasi-freestanding bilayer graphene (QFBLG) Hall bar devices. By integrating lithographic structuring with subsequent intercalation through dedicated intercalation channels, this method ensures precise control over metal incorporation while preserving device integrity. Magneto-transport measurements reveal superconductivity with a critical temperature Tc,onset ~ 3.5 K and the occurrence of a transverse resistance, including both symmetric and antisymmetric field components, which is attributed to the symmetric-in-field component to non-uniform currents. These results establish an advanced fabrication method for intercalated graphene devices, providing access to systematic investigations of confined 2D superconductivity and emergent electronic phases in van der Waals heterostructures.

cond-mat.mtrl-sci

Phase formation in hole- and electron-doped rare-earth nickelate single crystals

The recent discovery of superconductivity in hole-doped infinite-layer nickelates has triggered a great interest in the synthesis of novel nickelate phases, which have primarily been examined in thin film samples. Here, we report the high-pressure optical floating zone (OFZ) growth of various perovskite and perovskite-derived rare-earth nickelate single-crystals, and investigate the effects of hole-, electron-, and self-doping. For hole-doping with Ca and Sr, we observe phase separations during the growth process when a substitution level of 8% is exceeded. A similar trend emerges for electron-doping with Ce and Zr. Employing lower doping levels allows us to grow sizeable crystals in the perovskite phase, which exhibit significantly different electronic and magnetic properties than the undoped parent compounds, such as a decreased resistivity and a suppressed magnetic response. Our insights into the doping-dependent phase formation and the resulting properties of the synthesized crystals reveal limitations and opportunities for the exploration and manipulation of electronic states in rare-earth nickelates.

cond-mat.str-el

Probing the interlayer coupling in 2$H$-NbS$_2$ via soft x-ray angle-resolved photoemission spectroscopy

In the large family of two-dimensional (2D) layered materials including graphene, its honeycomb analogs, and transition-metal dichalcogenides, the interlayer coupling plays a rather intriguing role. On the one hand, the weak van der Waals interaction that holds the layers together endows these compounds with quasi-2D properties, which might imply small interlayer effects on the electronically active bands. On the other hand, the oft-witnessed differences in electronic, optical, and magnetic behaviors of monolayers, bilayers, and multilayers of the same compound must have as their microscopic origin the detailed interlayer hopping parameters. Given the few experimental reports that have attempted to explicitly extract these parameters, we employ soft-x-ray angle-resolved photoemission spectroscopy (SX-ARPES) to probe the interlayer coupling in superconducting 2$H$-NbS$_2$. We visualize the S 3$p_z$ bands that disperse with respect to the out-of-plane momentum and introduce a simple tight-binding model to extract the interlayer hopping parameters. From first-principles calculations, we clarify how atomic distances and the proper accounting for screening via hybrid functionals influence these bands. The knowledge of interlayer hopping parameters is particularly pertinent in NbS$_2$, where recent experiments have uncovered fingerprints of finite-momentum superconductivity in the bulk material and heterostructures.

cond-mat.supr-con

Unusual Valence State in the Antiperovskites Sr$_3$SnO and Sr$_3$PbO Revealed by X-ray Photoelectron Spectroscopy

The class of antiperovskite compounds $A_3B$O ($A$ = Ca, Sr, Ba; $B$ = Sn, Pb) has attracted interest as a candidate 3D Dirac system with topological surface states protected by crystal symmetry. A key factor underlying the rich electronic structure of $A_3B$O is the unusual valence state of $B$, i.e., a formal oxidation state of $-4$. Practically, it is not obvious whether anionic $B$ can be stabilized in thin films, due to its unusual chemistry, as well as the polar surface of $A_3B$O, which may render the growth-front surface unstable. We report X-ray photoelectron spectroscopy (XPS) measurements of single-crystalline films of Sr$_3$SnO and Sr$_3$PbO grown by molecular beam epitaxy (MBE). We observe shifts in the core-level binding energies that originate from anionic Sn and Pb, consistent with density functional theory (DFT) calculations. Near the surface, we observe additional signatures of neutral or cationic Sn and Pb, which may point to an electronic or atomic reconstruction with possible impact on putative topological surface states.

cond-mat.mes-hall

Spin splitting and strain in epitaxial monolayer WSe$_2$ on graphene

We present the electronic and structural properties of monolayer WSe$_{2}$ grown by pulsed-laser deposition on monolayer graphene (MLG) on SiC. The spin splitting in the WSe$_{2}$ valence band at $\overline{\mathrm{K}}$ was $Δ_\mathrm{SO}=0.469\pm0.008$ eV by angle-resolved photoemission spectroscopy (ARPES). Synchrotron-based grazing-incidence in-plane X-ray diffraction (XRD) revealed the in-plane lattice constant of monolayer WSe$_{2}$ to be $a_\mathrm{WSe_2}=3.2757\pm0.0008 \mathrm{Å}$. This indicates a lattice compression of -0.19 % from bulk WSe$_{2}$. By using experimentally determined graphene lattice constant ($a_\mathrm{MLG}=2.4575\pm0.0007 \mathrm{Å}$), we found that a 3$\times$3 unit cell of the slightly compressed WSe$_{2}$ is perfectly commensurate with a 4$\times$4 graphene lattice with a mismatch below 0.03 %, which could explain why the monolayer WSe$_{2}$ is compressed on MLG. From XRD and first-principles calculations, however, we conclude that the observed size of strain is negligibly small to account for a discrepancy in $Δ_\mathrm{SO}$ found between exfoliated and epitaxial monolayers in earlier ARPES. In addition, angle-resolved, ultraviolet and X-ray photoelectron spectroscopy shed light on the band alignment between WSe$_{2}$ and MLG/SiC and indicate electron transfer from graphene to the WSe$_{2}$ monolayer. As further revealed by atomic force microscopy, the WSe$_{2}$ island size depends on the number of carbon layers on top of the SiC substrate. This suggests that the epitaxy of WSe$_{2}$ favors the weak van der Waals interactions with graphene while it is perturbed by the influence of the SiC substrate and its carbon buffer layer.

cond-mat.mtrl-sci

Room temperature strain-induced Landau levels in graphene on a wafer-scale platform

Graphene is a powerful playground for studying a plethora of quantum phenomena. One of the remarkable properties of graphene arises when it is strained in particular geometries and the electrons behave as if they were under the influence of a magnetic field. Previously, these strain-induced pseudomagnetic fields have been explored on the nano- and micrometer-scale using scanning probe and transport measurements. Heteroepitaxial strain, in contrast, is a wafer-scale engineering method. Here, we show that pseudomagnetic fields can be generated in graphene through wafer-scale epitaxial growth. Shallow triangular nanoprisms in the SiC substrate generate strain-induced uniform fields of 41 T. This enables the observation of strain-induced Landau levels at room temperature, as detected by angle-resolved photoemission spectroscopy, and confirmed by model calculations and scanning tunneling microscopy measurements. Our work demonstrates the feasibility of exploiting strain-induced quantum phases in two-dimensional Dirac materials on a wafer-scale platform, opening the field to new applications.

cond-mat.mtrl-sci

Introducing strong correlation effects into graphene by gadolinium intercalation

Exotic ordered ground states driven by electronic correlations are expected to be induced in monolayer graphene when doped to the Van Hove singularity. Such doping levels are reached by intercalating Gd in graphene on SiC(0001), resulting in a strong homogeneity and stability. The electronic spectrum now exhibits severe renormalizations. Flat bands develop which is driven by electronic correlations according to our theoretical studies. Due to strong electron-phonon coupling in this regime, polaron replica bands develop. Thus, interesting ordered ground states should be made accessible.

cond-mat.str-el

Enhanced electron-phonon coupling in graphene with periodically distorted lattice

Electron-phonon coupling directly determines the stability of cooperative order in solids, including superconductivity, charge and spin density waves. Therefore, the ability to enhance or reduce electron-phonon coupling by optical driving may open up new possibilities to steer materials' functionalities, potentially at high speeds. Here we explore the response of bilayer graphene to dynamical modulation of the lattice, achieved by driving optically-active in-plane bond stretching vibrations with femtosecond mid-infrared pulses. The driven state is studied by two different ultrafast spectroscopic techniques. Firstly, TeraHertz time-domain spectroscopy reveals that the Drude scattering rate decreases upon driving. Secondly, the relaxation rate of hot quasi-particles, as measured by time- and angle-resolved photoemission spectroscopy, increases. These two independent observations are quantitatively consistent with one another and can be explained by a transient three-fold enhancement of the electron-phonon coupling constant. The findings reported here provide useful perspective for related experiments, which reported the enhancement of superconductivity in alkali-doped fullerites when a similar phonon mode was driven.

cond-mat.mtrl-sci

Observation of Dirac surface states in the noncentrosymmetric superconductor BiPd

Materials with strong spin-orbit coupling (SOC) have in recent years become a subject of intense research due to their potential applications in spintronics and quantum information technology. In particular, in systems which break inversion symmetry, SOC facilitates the Rashba-Dresselhaus effect, leading to a lifting of spin degeneracy in the bulk and intricate spin textures of the Bloch wave functions. Here, by combining angular resolved photoemission (ARPES) and low temperature scanning tunneling microscopy (STM) measurements with relativistic first-principles band structure calculations, we examine the role of SOC in single crystals of noncentrosymmetric BiPd. We report the detection of several Dirac surface states, one of which exhibits an extremely large spin splitting. Unlike the surface states in inversion-symmetric systems, the Dirac surface states of BiPd have completely different properties at opposite faces of the crystal and are not trivially linked by symmetry. The spin-splitting of the surface states exhibits a strong anisotropy by itself, which can be linked to the low in-plane symmetry of the surface termination.

cond-mat.mtrl-sci

Intercalation of graphene on SiC(0001) via ion-implantation

Electronic devices based on graphene technology are catching on rapidly and the ability to engineer graphene properties at the nanoscale is becoming, more than ever, indispensable. Here, we present a new procedure of graphene functionalization on SiC(0001) that paves the way towards the fabrication of complex graphene electronic chips. The procedure resides on the well-known ion-implantation technique. The efficiency of the working principle is demonstrated by the intercalation of the epitaxial graphene layer on SiC(0001) with Bi atoms, which was not possible following standard procedures. Our results put forward the ion-beam lithography to nanostructure and functionalize desired graphene chips.

cond-mat.mes-hall

Tracking primary thermalization events in graphene with photoemission at extreme timescales

Direct and inverse Auger scattering are amongst the primary processes that mediate the thermalization of hot carriers in semiconductors. These two processes involve the annihilation or generation of an electron-hole pair by exchanging energy with a third carrier, which is either accelerated or decelerated. Inverse Auger scattering is generally suppressed, as the decelerated carriers must have excess energies higher than the band gap itself. In graphene, which is gapless, inverse Auger scattering is instead predicted to be dominant at the earliest time delays. Here, $<8$ femtosecond extreme-ultraviolet pulses are used to detect this imbalance, tracking both the number of excited electrons and their kinetic energy with time- and angle-resolved photoemission spectroscopy. Over a time window of approximately 25 fs after absorption of the pump pulse, we observe an increase in conduction band carrier density and a simultaneous decrease of the average carrier kinetic energy, revealing that relaxation is in fact dominated by inverse Auger scattering. Measurements of carrier scattering at extreme timescales by photoemission will serve as a guide to ultrafast control of electronic properties in solids for PetaHertz electronics.

cond-mat.mtrl-sci

X-ray and neutron reflectometry study of copper surface reconstruction caused by implantation of high-energy oxygen ions

Combination of neutron and X-ray reflectometry was used to study the vertical structure of 100 nm-thin copper films with implanted oxygen ions of energy E = [10-30] keV and doses D=[0.2-5.4]x$10^{16}$ $cm^{-2}$. The study shows that oxygen ion implantation with an energy of E = 30 keV leads to the formation of a 3 nm thick layer on the surface. Density and copper/oxygen stoichiometry of the observed surface layer are close to $Cu_2O$ oxide. We attribute the $Cu_2O$ oxide formation to highly mobilized copper atoms generated by stimulated ion implantation.

cond-mat.mtrl-sci

Approaching ideal graphene: The structure of hydrogen-intercalated graphene on 6H-SiC(0001)

We measure the adsorption height of hydrogen-intercalated quasi-free-standing monolayer graphene on the (0001) face of 6H silicon carbide by the normal incidence x-ray standing wave technique. A density functional calculation for the full ($6 \sqrt{3} \times 6 \sqrt{3}$)-R30$^\circ$ unit cell, based on a van der Waals corrected exchange correlation functional, finds a purely physisorptive adsorption height in excellent agreement with experiments, a very low buckling of the graphene layer, a very homogeneous electron density at the interface and the lowest known adsorption energy per atom for graphene on any substrate. A structural comparison to other graphenes suggests that hydrogen intercalated graphene on 6H-SiC(0001) approaches ideal graphene.

cond-mat.mtrl-sci

Influence of the degree of decoupling of graphene on the properties of transition metal adatoms

We investigate the adsorption sites of $3d$ transition metal (TM) adatoms by means of low-temperature scanning tunneling microscopy and spectroscopy. Co and Ni adatoms were adsorbed on two types of graphene on SiC(0001), i.e. pristine epitaxial monolayer graphene (MLG) and quasi-free-standing monolayer graphene (QFMLG). In the case of QFMLG, two stable adsorption sites are identified, while in the case of MLG, only one adsorption site is observed. Our experimental results reveal the decoupling efficiency as a crucial parameter for determining the adsorption site as well as the electronic properties of $3d$ transition metal atoms on graphene. Furthermore, we show that Co atoms adsorbed on QFMLG are strong scattering potentials for Dirac fermions and cause intervalley scattering in their vicinity.

cond-mat.mes-hall

Adatoms and clusters of 3d transition metals on graphene: Electronic and magnetic configurations

We investigate the electronic and magnetic properties of single Fe, Co, and Ni atoms and clusters on monolayer graphene (MLG) on SiC(0001) by means of scanning tunneling microscopy (STM), x-ray absorption spectroscopy, x-ray magnetic circular dichroism (XMCD), and ab initio calculations. STM reveals different adsorption sites for Ni and Co adatoms. XMCD proves Fe and Co adatoms to be paramagnetic and to exhibit an out-of-plane easy axis in agreement with theory. In contrast, we experimentally find a nonmagnetic ground state for Ni monomers while an increasing cluster size leads to sizeable magnetic moments. These observations are well reproduced by our calculations and reveal the importance of hybridization effects and intra-atomic charge transfer for the properties of adatoms and clusters on MLG.

cond-mat.mes-hall

Quasi-free Standing Epitaxial Graphene on SiC by Hydrogen Intercalation

Quasi-free standing epitaxial graphene is obtained on SiC(0001) by hydrogen intercalation. The hydrogen moves between the 6root3 reconstructed initial carbon layer and the SiC substrate. The topmost Si atoms which for epitaxial graphene are covalently bound to this buffer layer, are now saturated by hydrogen bonds. The buffer layer is turned into a quasi-free standing graphene monolayer with its typical linear pi-bands. Similarly, epitaxial monolayer graphene turns into a decoupled bilayer. The intercalation is stable in air and can be reversed by annealing to around 900 degrees Celsius.

cond-mat.mtrl-sci

LEED Holography applied to a complex superstructure: a direct view of the adatom cluster on SiC(111)-(3x3)

For the example of the SiC(111)-(3x3) reconstruction we show that a holographic interpretation of discrete Low Energy Electron Diffraction (LEED) spot intensities arising from ordered, large unit cell superstructures can give direct access to the local geometry of a cluster around an elevated atom, provided there is only one such prominent atom per surface unit cell. By comparing the holographic images obtained from experimental and calculated data we illuminate validity, current limits and possible shortcomings of the method. In particular, we show that periodic vacancies such as cornerholes may inhibit the correct detection of the atomic positions. By contrast, the extra diffraction intensity due to slight substrate reconstructions, as for example buckling, seems to have negligible influence on the images. Due to the spatial information depth of the method the stacking of the cluster can be imaged down to the fourth layer. Finally, it is demonstrated how this structural knowledge of the adcluster geometry can be used to guide the dynamical intensity analysis subsequent to the holographic reconstruction and necessary to retrieve the full unit cell structure.

cond-mat.mtrl-sci