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Y. E. Suyolcu

Publications and source records attributed to Y. E. Suyolcu.

8 recordsLinked to original sources

Multiorbital character of the density wave in trilayer nickelate superconductors

Ruddlesden-Popper nickelates exhibit high-temperature superconductivity closely intertwined with charge and spin density waves. However, fundamental questions persist regarding the interplay between the associated density wave (DW) fluctuations and superconductivity, as well as the orbital character and symmetry underlying the DW instabilities. Here we utilize polarized Raman scattering to investigate the phononic and electronic Raman responses of the trilayer nickelate La$_4$Ni$_3$O$_{10}$ across its concomitant charge and spin density wave transitions. In addition to distinct phonon anomalies occurring below the transition temperature, we observe a depletion of continuum spectral weight up to 114 meV and a pronounced peak centered at this energy. By combining momentum-selective information from polarized electronic Raman scattering with Raman-response model calculations based on a multiorbital Raman vertex in a reconstructed two-orbital DW state involving both Ni-3$d_{x^2 - y^2}$ and Ni-3$d_{z^2}$ orbitals, we identify 114 meV as the energy scale $2Δ_\mathrm{DW}$ of the DW gap, characterized by incoherent opening and non-mean-field behavior. Furthermore, the model calculations reveal that the corresponding $2Δ_\mathrm{DW}$ peak has a multiorbital origin, requiring both orbital contributions and their mixing beyond single-orbital projections, thus shedding light on the nature of the DW instabilities in La$_4$Ni$_3$O$_{10}$.

cond-mat.str-el↗

High temperature transitions in Ruddlesden-Popper nickelates La$_{n+1}$Ni$_{n}$O$_{3n+1}$

The discovery of superconductivity at $15\,\mathrm{K}$ in the infinite-layer nickelate $(\mathrm{Nd},\mathrm{Sr})\mathrm{NiO}_2$, followed by superconductivity at $80\,\mathrm{K}$ in the Ruddlesden--Popper phase $\mathrm{La}_3\mathrm{Ni}_2\mathrm{O}_7$, has ushered in a new era of nickelate research. Despite this progress, large discrepancies between reports exist. Here, we investigate the complete series of bulk-stable $\mathrm{La}_{n+1}\mathrm{Ni}_n\mathrm{O}_{3n+1}$ compounds using a comprehensive set of experimental techniques, including PXRD, single-crystal XRD, electron microscopy, heat capacity, differential scanning calorimetry, magnetic susceptibility, and transport measurements, over a broad temperature range from $2$ to $1000\,\mathrm{K}$. By studying high-quality single crystals, we identify a previously underappreciated high-temperature phase transition in Ruddlesden--Popper nickelates $\mathrm{La}_{n+1}\mathrm{Ni}_n\mathrm{O}_{3n+1}$ distinct from the one going to a tetragonal phase.

cond-mat.supr-con↗

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

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$_{4-δ}$, 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↗

Investigation of spin excitations and charge order in bulk crystals of the infinite-layer nickelate LaNiO$_2$

Recent x-ray spectroscopic studies have revealed spin excitations and charge density waves in thin films of infinite-layer (IL) nickelates. However, clarifying whether the origin of these phenomena is intrinsic to the material class or attributable to impurity phases in the films has presented a major challenge. Here we utilize topotactic methods to synthesize bulk crystals of the IL nickelate LaNiO$_2$ with crystallographically oriented surfaces. We examine these crystals using resonant inelastic x-ray scattering (RIXS) at the Ni $L_3$-edge to elucidate the spin and charge correlations in the bulk of the material. While we detect the presence of prominent spin excitations in the crystals, fingerprints of charge order are absent at the ordering vectors identified in previous in thin-film studies. These results contribute to the understanding of the bulk properties of LaNiO$_2$ and establish topotactically synthesized crystals as viable complementary specimens for spectroscopic investigations.

cond-mat.str-el↗

Evolution of plasmon excitations across the phase diagram of the cuprate superconductor La$_{2-x}$Sr$_{x}$CuO$_4$

We use resonant inelastic x-ray scattering (RIXS) at the O $K$- and Cu $K$-edges to investigate the doping- and temperature dependence of low-energy plasmon excitations in La$_{2-x}$Sr$_{x}$CuO$_4$. We observe a monotonic increase of the energy scale of the plasmons with increasing doping $x$ in the underdoped regime, whereas a saturation occurs above optimal doping $x \gtrsim 0.16$ and persists at least up to $x = 0.4$. Furthermore, we find that the plasmon excitations show only a marginal temperature dependence, and possible effects due to the superconducting transition and the onset of strange metal behavior are either absent or below the detection limit of our experiment. Taking into account the strongly correlated character of the cuprates, we show that layered $t$-$J$-$V$ model calculations accurately capture the increase of the plasmon energy in the underdoped regime. However, the computed plasmon energy continues to increase even for doping levels above $x \gtrsim 0.16$, which is distinct from the experimentally observed saturation, and reaches a broad maximum around $x = 0.55$. We discuss whether possible lattice disorder in overdoped samples, a renormalization of the electronic correlation strength at high dopings, or an increasing relevance of non-planar Cu and O orbitals could be responsible for the discrepancy between experiment and theory for doping levels above $x = 0.16$.

cond-mat.supr-con↗

Crystallization of heavy fermions via epitaxial strain in spinel LiV$_{2}$O$_{4}$ thin film

The mixed-valent spinel LiV$_{2}$O$_{4}$ is known as the first oxide heavy-fermion system. There is a general consensus that a subtle interplay of charge, spin, and orbital degrees of freedom of correlated electrons plays a crucial role in the enhancement of quasi-particle mass, but the specific mechanism has remained yet elusive. A charge-ordering (CO) instability of V$^{3+}$ and V$^{4+}$ ions that is geometrically frustrated by the V pyrochlore sublattice from forming a long-range CO down to $T$ = 0 K has been proposed as a prime candidate for the mechanism. To uncover the hidden CO instability, we applied epitaxial strain from a substrate on single-crystalline thin films of LiV$_{2}$O$_{4}$. Here we show a strain-induced crystallization of heavy fermions in a LiV$_{2}$O$_{4}$ film on MgO, where a charge-ordered insulator comprising of a stack of V$^{3+}$ and V$^{4+}$ layers along [001], the historical Verwey-type ordering, is stabilized by the in-plane tensile and out-of-plane compressive strains from the substrate. Our discovery of the [001] Verwey-type CO, together with previous realizations of a distinct [111] CO, evidence the close proximity of the heavy-fermion state to degenerate CO states mirroring the geometrical frustration of the pyrochlore lattice, which supports the CO instability scenario for the mechanism behind the heavy-fermion formation.

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↗

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↗