arXiv subjects

Matthias Hepting

Publications and source records attributed to Matthias Hepting.

At least 19 recordsLinked to original sources

arXiv2026

Unveiling orbital landscapes in strongly correlated bulk nickelates with $s$-NIXS

We leverage $s$-orbital non-resonant inelastic X-ray scattering ($s$-NIXS) to perform orbital imaging on three bulk rare-earth nickelates spanning a range of formal nickel valence (3$d$ electron filling) from Ni$^{3+}$ (3$d^7$) to Ni$^{1+}$ (3$d^9$). Our results directly reveal the ground states of these compounds all with minimal theoretical input. In particular, we demonstrate the low-spin orbital configuration of trivalent LaNiO$_3$, the $d_{x^2-y^2}$ configuration of monovalent LaNiO$_2$, and resolve the effective $e_g$ crystal field splitting in the distorted octahedral environment of divalent La$_2$NiO$_4$. This work illustrates the potential of $s$-NIXS to study the ground state and excited states of strongly correlated materials without needing complex theoretical analysis of spectroscopic data.

cond-mat.str-el↗

arXiv2026

Imaging stripe dynamics in trilayer nickelate La$_4$Ni$_3$O$_{10}$

Since the discovery of high-temperature superconductivity in nickelate superconductors, it is an open question how closely the superconducting state resembles that of cuprate superconductors. One salient feature of the phase diagram of the high-temperature cuprate superconductors is stripe order. Despite their prevalence, real-space imaging has been limited to the charge sector. Here we use spin-polarised scanning tunnelling microscopy to visualize the local magnetic and charge distribution emerging due to a stripe order in the trilayer nickelate La$_4$Ni$_3$O$_{10}$. The stripe order exhibits a four unit cell periodicity, closely resembling that seen in cuprates, and opens a near-complete $\sim66\mathrm{meV}$ gap at the Fermi level. Crucially, discrete phase slips can be triggered by tunneling electrons above a $\sim 20\mathrm{meV}$ threshold, allowing imaging of stripe dynamics at the atomic scale. These results highlight the importance of correlation physics driving stripe-like orders in lanthanum nickelates with striking similarities to the cuprates.

cond-mat.str-el↗

arXiv2026

Strongly correlated model of acousticlike plasmons persisting across the phase diagram of cuprate superconductors

Layered two-dimensional electron systems exhibit both optical and acousticlike plasmons around the Brillouin-zone center. In the layered cuprate La$_{2-x}$Sr$_x$CuO$_4$, resonant inelastic x-ray scattering (RIXS) has detected corresponding acousticlike plasmons in a low-energy regime comparable to that of other collective excitations associated with distinct regions of the cuprate phase diagram. This overlap in energy scale raises the question of whether the acousticlike plasmons are significantly influenced by phase-specific electronic phenomena, including the pseudogap, charge and spin order, superconductivity, and strange-metal behavior. Here we show that a single parameter set of the layered $t$-$J$-$V$ model, which incorporates strong correlations and the long-range Coulomb interaction $V$, consistently describes the acousticlike plasmon dispersion across all currently available RIXS data from the underdoped to the heavily overdoped regime. This transferability of a single parameter set exceeds that of earlier theoretical descriptions and supports a picture in which strong correlations persist into the heavily overdoped regime, while the collective plasmon mode exhibits only limited sensitivity to the phase-specific electronic phenomena that distinguish different regions of the phase diagram.

cond-mat.str-el↗

arXiv2026

Anisotropic magnetoelastic coupling in the honeycomb magnet Na$_3$Co$_2$SbO$_6$

We present magnetization and dilatometry measurements on the honeycomb cobaltate Na$_3$Co$_2$SbO$_6$ and map out its detailed field-temperature phase diagram down to sub-Kelvin temperatures. Our data for in-plane magnetic fields show a strongly anisotropic $c^{*}$-axis lattice response, which is dominated by the variation of Co--O--Co bond angles according to \textit{ab initio} calculations. At $T = 0.4$~K, the magnetization $M(B)$ exhibits step-like features that are also highly anisotropic. In the case of $B \parallel b$, a small hysteresis observed around the second field-induced magnetic transition ($B_{c2}$) indicates its first-order character, whereas divergence of the magnetic Gr\"uneisen parameter at $B_{c2}$ is suppressed upon cooling and signals the absence of quantum critical behavior upon entering the field-polarized state. None of our thermodynamic measurements provide evidence for a field-induced quantum spin liquid state near or above $B_{c2}$.

cond-mat.str-el↗

arXiv2025

Magnetism of the alternating monolayer-trilayer phase of La$_3$Ni$_2$O$_7$

Understanding the magnetic ground state of Ruddlesden-Popper nickelates is crucial, as these materials exhibit superconductivity under high pressure and host competing electronic orders that may play a key role in the pairing mechanism. In this work, we investigate the magnetic properties of the alternating monolayer-trilayer phase of La$_3$Ni$_2$O$_7$ (1313-La$_3$Ni$_2$O$_7$) using muon-spin rotation/relaxation ($\mu$SR) under both ambient and hydrostatic pressure conditions. The monolayer-trilayer phase develops incommensurate magnetic order below approximately 150 K, with a mean ordering temperature of $T_{SDW} \simeq 123$ K and a transition width of $\Delta T_{SDW} \simeq 15$ K. The abrupt onset of the internal magnetic field indicates a first-order-like transition. Hydrostatic pressure ($p$) suppresses the magnetic ordering temperature at a rate of $dT_{SDW}/d p \simeq -3.9$ K/GPa, demonstrating a progressive destabilization of the ordered state. By comparison with the bilayer 2222-La$_3$Ni$_2$O$_7$ and the trilayer 3333-La$_4$Ni$_3$O$_{10}$ systems, and within a unified phenomenological framework, systematic trends are identified linking the pressure dependence of $T_{SDW}$, the (in)commensurability of the magnetic order, and the character of the magnetic transition. These trends consistently indicate a gradual reduction of electronic correlation strength from the bilayer to the monolayer-trilayer and trilayer nickelates. This hierarchy suggests that the higher superconducting transition temperature observed in the 2222 phase may be closely connected to its more strongly correlated electronic nature. These results position the alternating monolayer-trilayer 1313-La$_3$Ni$_2$O$_7$ as an intermediate member linking the magnetic behavior of the bilayer 2222-La$_3$Ni$_2$O$_7$ and the trilayer 3333-La$_4$Ni$_3$O$_{10}$ Ruddlesden-Popper compounds.

cond-mat.supr-con↗

arXiv2025

Comparative Raman study of Ruddlesden-Popper nickelates and the monolayer-trilayer polymorph

Ruddlesden-Popper (RP) nickelates have attracted intense interest following the discovery of superconductivity in several members of the series, including bilayer (BL) La$_3$Ni$_2$O$_7$, trilayer (TL) La$_4$Ni$_3$O$_{10}$, and structural polymorphs composed of monolayer-bilayer or monolayer-trilayer (ML-TL) units. However, an inherent propensity of the RP series to form intergrown phases during single-crystal synthesis, together with spatial variations in oxygen stoichiometry, has complicated the determination of their intrinsic material properties. As a consequence, conflicting reports have emerged on both their electronic phase transitions and lattice dynamics. In this work, we perform a comparative study of the phononic and electronic Raman responses of high-quality ML-TL single crystals and contrast them with those of other RP nickelates, using samples with optimized oxygen content. We establish several Raman spectral features that enable unambiguous phase identification across the series. Moreover, we uncover characteristics in the phononic and electronic Raman response of ML-TL that are not reflected in the pure ML and TL compounds. We attribute these differences to a distinctive electronic structure arising from self-doping and confinement effects induced by the ML unit within the ML-TL lattice architecture.

cond-mat.str-el↗

arXiv2025

Lattice dynamics of the infinite-layer nickelate LaNiO$_2$

Infinite-layer (IL) nickelates have rapidly emerged as a new class of superconductors. However, due to the technical challenges of their topotactic synthesis, they have so far been realized primarily as thin films or polycrystalline powder samples, limiting comprehensive investigations of fundamental physical properties such as the lattice dynamics. Here, we present a time-of-flight inelastic neutron scattering study on a sample composed of a large number of co-aligned bulk crystals of the IL nickelate LaNiO$_2$. We observe several dispersive phonon branches, which are in good agreement with lattice dynamical calculations based on density-functional perturbation theory. In addition, we compare the characteristics of selected LaNiO$_2$ phonon modes to those of isostructural cuprate superconductors. Our findings provide a reference point for future experimental and theoretical efforts aimed at understanding the interplay between lattice dynamics and electronic properties in IL nickelates.

cond-mat.str-el↗

arXiv2025

Direct Evidence of Metal-Ligand Redox in Li-ion Battery Positive Electrodes

Describing Li-ion battery positive electrodes in terms of distinct transition metal or oxygen redox regimes can lead to confusion in understanding metal-ligand hybridisation, oxygen dimerisation, and degradation. There is a pressing need to study the electronic structure of these materials and determine the role each cation and anion plays in charge compensation. Here, we employ transition metal L-edge X-ray Resonance Photoemission Spectroscopy in conjunction with Single Impurity Anderson models, Self-consistent Real Space Multiple Scattering spectral simulations, and Dynamical Mean-Field theory calculations to directly evaluate the redox mechanisms in (de-)lithiated battery electrodes. This approach reconciles the redox description of two canonical cathodes -- LiMn$_{0.6}$Fe$_{0.4}$PO$_{4}$ and LiNiO$_{2}$ -- in terms of varying degrees of charge transfer using the established Zaanen-Sawatzky-Allen framework, common to condensed matter physics. In LiMn$_{0.6}$Fe$_{0.4}$PO$_{4}$, the absence of charge transfer means capacity arises due to the depopulation of metal $\textit{3d}$ states, i.e. conventional metal redox. Whereas, in LiNiO$_{2}$, charge transfer dominates and redox occurs through the formation and elimination of ligand hole states. This work clarifies the role of oxygen in Ni-rich system and provides a framework to explain how capacity can be extracted from oxygen-dominated states in highly covalent systems without needing to invoke dimerisation.

cond-mat.mtrl-sci↗

arXiv2024

Non-volatile multi-state electrothermal resistive switching in a strongly correlated insulator thin-film device

Strongly correlated insulators, such as Mott or charge-transfer insulators, exhibit a strong temperature dependence in their resistivity. Consequently, self-heating effects can lead to electrothermal instabilities in planar thin film devices of these materials. When the electrical bias current exceeds a device-specific threshold, the device can switch from a high- to a low-resistance state through the formation of metallic filaments. However, since the current and temperature redistribution effects that create these filaments are sustained by local Joule heating, a reduction of the bias current below a second (lower) threshold leads to the disappearance of filaments, and the device switches back into the high-resistance state. Hence, electrothermal resistive switching is usually volatile. Here, on the contrary, we report on non-volatile resistive switching in a planar $\mathrm{NdNiO}_3$ thin-film device. By combining electrical transport measurements with optical wide-field microscopy, we provide evidence for a metallic filament that persists even after returning the bias current to zero. We attribute this effect to the pronounced hysteresis between the cooling and heating branches in the resistance vs. temperature dependence of the device. At least one hundred intermediate resistance states can be prepared, which are persistent as long as the base temperature is kept constant. Further, the switching process is non-destructive, and thermal cycling can reset the device to its pristine state.

physics.app-ph↗

arXiv2024

Unraveling nano-scale effects of topotactic reduction in LaNiO$_2$ crystals

Infinite-layer nickelates stand as a promising frontier in the exploration of unconventional superconductivity. Their synthesis through topotactic oxygen reduction from the parent perovskite phase remains a complex and elusive process. This study delves into the nano-scale effects of the topotactic lattice transformation within LaNiO$_2$ crystals. Leveraging high-resolution scanning transmission electron microscopy and spectroscopy, our investigations uncover a panorama of structural alterations, including grain boundaries and coherent twin boundaries, triggered by reduction-induced transformations. In addition, our analyses unveil the formation of an oxygen-rich disordered transition phase encircling impurities and pervading crystalline domains, and the internal strain is accommodated by grain boundary formation. By unraveling these nano-scale effects, our findings provide insights into the microscopic intricacies of the topotactic reduction process elucidating the transition from the perovskite to the infinite-layer phase within nickelate bulk crystals.

cond-mat.mtrl-sci↗

arXiv2024

Spin-orbit excitons in a correlated metal: Raman scattering study of Sr2RhO4

Using Raman spectroscopy to study the correlated 4$d$-electron metal Sr$_2$RhO$_4$, we observe pronounced excitations at 220 meV and 240 meV with $A_\mathrm{1g}$ and $B_\mathrm{1g}$ symmetries, respectively. We identify them as transitions between the spin-orbit multiplets of the Rh ions, in close analogy to the spin-orbit excitons in the Mott insulators Sr$_2$IrO$_4$ and $α$-RuCl$_3$. This observation provides direct evidence for the unquenched spin-orbit coupling in Sr$_2$RhO$_4$. A quantitative analysis of the data reveals that the tetragonal crystal field $Δ$ in Sr$_2$RhO$_4$ has a sign opposite to that in insulating Sr$_2$IrO$_4$, which enhances the planar $xy$ orbital character of the effective $J=1/2$ wave function. This supports a metallic ground state, and suggests that $c$-axis compression of Sr$_2$RhO$_4$ may transform it into a quasi-two-dimensional antiferromagnetic insulator.

cond-mat.str-el↗

arXiv2024

Electronic structure of the alternating monolayer-trilayer phase of La3Ni2O7

Recent studies of La$_3$Ni$_2$O$_7$ have identified a bilayer (2222) structure and an unexpected alternating monolayer-trilayer (1313) structure, both of which feature signatures of superconductivity near 80 K under high pressures. Using angle-resolved photoemission spectroscopy, we measure the electronic structure of 1313 samples. In contrast to the previously studied 2222 structure, we find that the 1313 structure hosts a flat band with a markedly different binding energy, as well as an additional electron pocket and band splittings. By comparison to local-density approximation calculations, we find renormalizations of the Ni-$d_{z^2}$ and Ni-$d_{x^2-y^2}$ derived bands to be about 5 to 7 and about 4 respectively, suggesting strong correlation effects. These results reveal important differences in the electronic structure brought about by the distinct structural motifs with the same stoichiometry. Such differences may be relevant to the putative high temperature superconductivity.

cond-mat.supr-con↗

arXiv2023

Unconventional crystal structure of the high-pressure superconductor La$_3$Ni$_2$O$_7$

The discovery of high-temperature superconductivity in La$_3$Ni$_2$O$_7$ at pressures above 14 GPa has spurred extensive research efforts. Yet, fundamental aspects of the superconducting phase, including the possibility of a filamentary character, are currently subjects of controversial debates. Conversely, a crystal structure with NiO$_6$ octahedral bilayers stacked along the $c$-axis direction was consistently posited in initial studies on La$_3$Ni$_2$O$_7$. Here we reassess this structure in optical floating zone-grown La$_3$Ni$_2$O$_7$ single crystals that show signs of filamentary superconductivity. Employing scanning transmission electron microscopy and single-crystal x-ray diffraction under high pressures, we observe multiple crystallographic phases in these crystals, with the majority phase exhibiting alternating monolayers and trilayers of NiO$_6$ octahedra, signifying a profound deviation from the previously suggested bilayer structure. Using density functional theory, we disentangle the individual contributions of the monolayer and trilayer structural units to the electronic band structure of La$_3$Ni$_2$O$_7$, providing a firm basis for advanced theoretical modeling and future evaluations of the potential of the monolayer-trilayer structure for hosting superconductivity.

cond-mat.supr-con↗

arXiv2023

Topotactically induced oxygen vacancy order in nickelate single crystals

The strong structure-property coupling in rare-earth nickelates has spurred the realization of new quantum phases in rapid succession. Recently, topotactic transformations have provided a new platform for the controlled creation of oxygen vacancies and, therewith, for the exploitation of such coupling in nickelates. Here, we report the emergence of oxygen vacancy ordering in Pr$_{0.92}$Ca$_{0.08}$NiO$_{2.75}$ single crystals obtained via a topotactic reduction of the perovskite phase Pr$_{0.92}$Ca$_{0.08}$NiO$_{3}$, using CaH$_2$ as the reducing agent. We unveil a brownmillerite-like ordering pattern of the vacancies by high-resolution scanning transmission electron microscopy, with Ni ions in alternating square-pyramidal and octahedral coordination along the pseudocubic [100] direction. Furthermore, we find that the crystal structure acquires a high level of internal strain, where wavelike modulations of polyhedral tilts and rotations accommodate the large distortions around the vacancy sites. Our results suggest that atomic-resolution electron microscopy is a powerful method to locally resolve unconventional crystal structures that result from the topotactic transformation of complex oxide materials.

cond-mat.mtrl-sci↗

arXiv2023

Synthesis and physical properties of LaNiO$_2$ crystals

Infinite-layer (IL) nickelates are an emerging family of superconductors whose similarities and differences to cuprate superconductors are under intense debate. To date, the IL phase of nickelates can only be reached via topotactic oxygen reduction of the perovskite phase, using H$_2$ gas or reducing agents such as CaH$_2$. While the topotactic reduction method has been widely employed on thin film and polycrystalline powder samples, the reduction of La$_{1-x}$Ca$_x$NiO$_3$ single-crystals with lateral dimensions up to 150 $μ$m was achieved only recently, using an indirect contact method with CaH$_2$. Here we report the topotactic transformation of much larger LaNiO$_3$ crystals with lateral dimensions of more than one millimeter, via direct contact with CaH$_2$. We characterize the crystalline, magnetic, and electronic properties of the obtained IL LaNiO$_{2}$ crystals by powder and single-crystal x-ray diffraction (XRD), magnetometry, electrical transport, and x-ray photoelectron spectroscopy (XPS) measurements. The amount of incorporated topotactic hydrogen due to the reduction process is determined by a gas extraction method. In addition, we investigate the evolution of the lattice parameters under hydrostatic pressure up to 12 GPa, using high-resolution synchrotron XRD. Furthermore, we provide a direct comparison of several physical properties of the LaNiO$_{2}$ crystals to their powder and thin film counterparts.

cond-mat.supr-con↗

arXiv2022

Investigation of hydrogen incorporations in bulk infinite-layer nickelates

Infinite-layer (IL) nickelates are an emerging class of superconductors, where the Ni$^{1+}$ valence state in a square planar NiO$_2$ coordination can only be reached via topotactic reduction of the perovskite phase. However, this topotactic soft chemistry with hydrogenous reagents is still at a stage of rapid development, and there is a number of open issues, especially considering the possibility of hydrogen incorporation. Here we study the time dependence of the topotactic transformation of LaNiO$_3$ to LaNiO$_2$ for powder samples with x-ray diffraction and gas extraction techniques. While the hydrogen content of the powder increases with time, neutron diffraction shows no negative scattering of hydrogen in the LaNiO$_2$ crystal lattice. The extra hydrogen appears to be confined to grain boundaries or secondary-phase precipitates. The average crystal structure, and possibly also the physical properties, of the primary LaNiO$_2$ phase are therefore not noticeably affected by hydrogen residues created by the topotactic transformation.

cond-mat.str-el↗

arXiv2021

Topotactic transformation of single-crystals: from perovskite to infinite-layer nickelates

Topotactic transformations between related crystal structures are a powerful emerging route for the synthesis of novel quantum materials. Whereas most such "soft chemistry" experiments have been carried out on polycrystalline powders or thin films, the topotactic modification of single crystals -- the gold standard for physical property measurements on quantum materials -- has proven remarkably difficult. Here, we report the topotactic reduction of La$_{1-x}$Ca$_{x}$NiO$_3$ single-crystals to La$_{1-x}$Ca$_{x}$NiO$_{2+δ}$ using CaH$_2$ as the reducing agent. The transformation from the three-dimensional perovskite to the quasi-two-dimensional infinite-layer phase was thoroughly characterized by X-ray diffraction, electron microscopy, Raman spectroscopy, magnetometry, and electrical transport measurements. Our work demonstrates that the infinite-layer structure can be realized as a bulk phase in crystals with micrometer-sized single-domains. The electronic properties of these specimens resemble those of epitaxial thin films rather than powders with similar compositions.

cond-mat.supr-con↗

arXiv2019

Complex magnetic order in nickelate slabs

Magnetic ordering phenomena have a profound influence on the macroscopic properties of correlated-electron materials, but their realistic prediction remains a formidable challenge. An archetypical example is the ternary nickel oxide system RNiO3 (R = rare earth), where the period-four magnetic order with proposals of collinear and non-collinear structures and the amplitude of magnetic moments on different Ni sublattices have been subjects of debate for decades. Here we introduce an elementary model system - NdNiO3 slabs embedded in a non-magnetic NdGaO3 matrix - and use polarized resonant x-ray scattering (RXS) to show that both collinear and non-collinear magnetic structures can be realized, depending on the slab thickness. The crossover between both spin structures is correctly predicted by density functional theory and can be qualitatively understood in a low-energy spin model. We further demonstrate that the amplitude ratio of magnetic moments in neighboring NiO6 octahedra can be accurately determined by RXS in combination with a correlated double cluster model. Targeted synthesis of model systems with controlled thickness and synergistic application of polarized RXS and ab-initio theory thus provide new perspectives for research on complex magnetism, in analogy to two-dimensional materials created by exfoliation.

cond-mat.str-el↗