arXiv subjects

Christoph Klewe

Publications and source records attributed to Christoph Klewe.

At least 19 recordsLinked to original sources

arXiv2026

Charge transfer and competing symmetry breaking drive orbital reconstruction and emergent ferromagnetism in insulating oxide superlattices

Electron correlation, hopping, and ligand-to-metal charge transfer collectively lead to diverse electronic and magnetic phenomena in 3$d$ transition-metal oxides, where directional d orbitals make hopping highly sensitive to symmetry-dependent orbital overlap. Heterostructure engineering with atomically flat interfaces adds symmetry-breaking charge transfer as a further route to emergent behavior, yet whether interfacial mismatch between constituent oxides of a superlattice shapes ground states independent of epitaxial strain remains unresolved. Here we examine superlattices combining NdNiO$_3$ with Mott-insulating NdMnO$_3$. Varying layer thickness and combining transport with X-ray spectroscopy, we show that electron transfer from NdMnO$_3$ to NdNiO$_3$ drives a room-temperature insulating state with a distinct electronic structure, accompanied by a reversal in orbital symmetry beyond simple strain considerations, underscoring the interface's central role. These reconstructions stabilize an emergent ferromagnetic insulating state arising from interfacial Ni$^{2+}$-O-Mn$^{4+}$ superexchange. Our results establish a pathway to interface-engineered ferromagnetic insulating phases via competing interactions, with potential for spin-insulatronic applications.

cond-mat.mtrl-sci↗

arXiv2026

Tuning perpendicular magnetic anisotropy in ultra-low damping Li$_{0.5}$Al$_{x}$Fe$_{(2.5-x)}$O$_4$ thin films for efficient spin-orbit torque switching

Ultra-thin magnetic insulator films that simultaneously exhibit ultra-low magnon damping, perpendicular magnetic anisotropy (PMA), and low spin-orbit torque (SOT) switching current densities are highly desirable, albeit challenging, for next-generation spintronic technologies that exploit spin waves to transport information without dissipative charge currents. Here, we demonstrate this combination of properties in ferrimagnetic spinel Li$_{0.5}$Al$_{x}$Fe$_{(2.5-x)}$O$_4$ (LAFO) thin films. Through this model system, we find that PMA can be tuned by epitaxial strain in the form of chemical composition and substrate choice and that low SOT switching current densities correlate with small but finite PMA. Ultra-low damping is stabilized primarily by having only Fe$^{3+}$ as magnetically active cations with secondary effects due to increased disorder from Al substitution distribution. SOT efficiency is governed by interface quality and independent of chemical composition. By varying the Al concentration, we systematically tune the saturation magnetization and magnetic anisotropy while maintaining ultra-low Gilbert damping parameters as low as $2\times10^{-4}$ and composition-independent damping-like SOT efficiencies. We identify an optimal composition LAFO x=0.7 (Li$_{0.5}$Al$_{0.7}$Fe$_{1.8}$O$_4$), which combines ultra-low damping, stable PMA with small anisotropy fields, and low critical current densities for SOT switching, establishing it as a promising material platform for energy-efficient spin-wave and spintronic devices.

cond-mat.mtrl-sci↗

arXiv2026

Low-Temperature Suppression of Intertwined Orders in La$_{1/3}$Sr$_{2/3}$FeO$_{3}$ Thin Films

The strong coupling between spin, charge, and lattice degrees of freedom in perovskite oxides leads to an array of exotic phenomena, giving these materials rich phase diagrams that can include coupled orders. This is exemplified by the A-site doped ferrite La$_{1/3}$Sr$_{2/3}$FeO$_{3}$ (LSFO), which exhibits a coupled paramagnetic-antiferromagnetic and charge ordering phase transition at $\sim$190 K that has been well studied in thin films, bulk, and polycrystalline samples. However, the low temperature behavior of LSFO thin films below $\sim$100 K has not been thoroughly explored. This work uses several X-ray scattering and spectroscopy techniques to directly probe LSFO's magnetic and charge order down to low temperature. Using resonant X-ray scattering, we observe a complete suppression of LSFO's known antiferromagnetic and charge order below $\sim$25 K. Further spectroscopy and coherent scattering measurements provide insight into LSFO's electronic structure and domain dynamics in this new low temperature phase, and we propose possible explanations for the observed order suppression based on reduced dimensionality of domains in our thin films. Our findings provide insight into the effects of competing interactions in strongly correlated materials, particularly those with coupled orders.

cond-mat.str-el↗

arXiv2026

Coupled phase transitions in crystalline solids with extreme chemical disorder

Structural phase transitions often couple to magnetic and electronic degrees of freedom, enabling emergent phenomena in solids. In high-entropy oxides (HEOs), which typically stabilize in highly symmetric cubic phases, such transitions are considered rare due to the extreme chemical disorder-analogous to the behavior observed in high-entropy alloys. This raises a fundamental question: can the rich physics of coupled phase transitions persist in such disordered systems? Here, we show that targeted design of compositionally complex oxides (CCOs) can trigger symmetry-lowering transitions, with spinel-type materials serving as a representative case. For instance, [Mn$_{0.2}$Co$_{0.2}$Ni$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$]Cr$_2$O$_4$, having two Jahn-Teller (J-T) active ions, undergoes two successive coupled structural transitions upon cooling: an orbital-driven transition at 100 K and a magnetism-driven transition at 40 K. Systematic substitution of $A$-site cations reveals that both Ni and Cu are essential for these transitions. Element specific local structure investigations uncover distinct and opposing local distortions around Ni and Cu, while Mn, Co, and Zn remain largely undistorted. These results establish that CCOs can host coupled phase transitions through `cooperation via competition' among local distortions in a chemically disordered lattice. This discovery expands the design principles for complex oxides, introducing a new paradigm for tuning structural and functional properties in high-entropy systems beyond conventional symmetry constraints.

cond-mat.mtrl-sci↗

arXiv2026

Topological textures and emergent altermagnetic signatures in ultrathin BiFeO3

Magnetoelectric multiferroics, materials with intrinsically coupled electric polarization and magnetic order, promise ultralow-power switching, nonvolatile memory, and energy-efficient signal transduction. Yet practical deployment demands ultrathin films down to the atomic limit, where both orders typically degrade. Maintaining both order parameters at the thinnest scales in complex oxides remains a tremendous challenge, as uncompensated bound charge drives nanoscale depolarization in most ferroelectrics, while off-stoichiometry, reduced anisotropy, and charge transfer can produce magnetic dead layers in ultrathin oxides at substrate interfaces. Here, we realize a multiferroic phase of BiFeO3 that not only sustains both order parameters at room temperature with no dead layer but also exhibits signatures of emergent altermagnetism in the four-unit-cell, ultrathin limit. First-principles calculations, spin symmetry analysis, atomic-resolution imaging, and angle-resolved magnetic imaging reveal that short-circuit electrostatic boundary conditions, together with epitaxial strain, drive a continuous second-order, thickness-driven phase transition that enables the formation of multiferroic topological textures. Moreover, the imposed boundary conditions stabilize a d-wave altermagnetic time-reversal symmetry breaking, with corresponding signatures observed in magnetic circular dichroism. Collectively, these results establish a pathway to stabilize unconventional multiferroicity at device-relevant thicknesses, reframing scaling limits for oxide electronics.

cond-mat.mtrl-sci↗

arXiv2026

Absence of magnetic order in epitaxial RuO2 revealed by X-ray linear dichroism

Recently, the topic of altermagnetism has attracted tremendous attention and RuO2 have been demonstrated to be one of the most promising altermagnetic candidates. However, disputes still remain on the existence of magnetic order in RuO2. Here in this work, we employ X-ray linear dichroism (XLD), a widely utilized technique for characterizing antiferromagnets, in conjunction with photoemission electron microscopy and multiple scattering calculation to provide clear evidence of the absence of magnetic order in epitaxial RuO2 films. The observed XLD signal is nearly invariant with temperature and independent on cooling field direction, in stark contrast to the substantial magnetic order-related XLD signal predicted by multiple scattering calculation. This finding strongly suggests a nonmagnetic origin for RuO2. Furthermore, we observed significantly distinct XLD signals at the Ru M3 and O K edges in RuO2 films grown on TiO2 substrate with different surface orientations, which can be attributed to the low-symmetry crystal field. These results unequivocally demonstrate the absence of magnetic order in RuO2 and establishes XLD measurement as a robust technique for probing the low-symmetry magnetic materials.

cond-mat.mtrl-sci↗

arXiv2025

Evolution of electronic and magnetic properties in Mn- and Co-alloyed ferromagnetic kagome metal Fe3Sn2

Kagome metals are an intriguing class of quantum materials as the presence of both flat bands and Dirac points provides access to functional properties present in strongly correlated and topological materials. To fully harness these electronic features, the ability to tune the Fermi level relative to the band positions is needed. Here we explore the structural, electronic and magnetic impacts of substitutional alloying within ferromagnetic kagome metal Fe3Sn2 in thin films grown by molecular beam epitaxy. Transition metals Mn and Co are chosen as substitutes for Fe to reduce or increase the d-band electron count, thereby moving the Fermi level accordingly. We find that Co is not incorporated into the Fe3Sn2 structure but instead results in a two-phase Fe-Co and (Fe,Co)Sn composite. In contrast, Fe3-xMnxSn2 films are realized with x up to 1.0, retaining crystalline quality comparable to the parent phase. The incorporation of Mn repositions the flat bands relative to the Fermi level in a manner consistent with hole-doping, as revealed by hard x-ray photoemission and density functional theory. The Fe3-xMnxSn2 films retain room temperature ferromagnetism, with x-ray magnetic circular dichroism measurements confirming that the Fe and Mn moments are ferromagnetically aligned. The ability to hole-dope this magnetic kagome metal provides a platform for tuning properties such as anomalous Hall and Nernst responses.

cond-mat.mtrl-sci↗

arXiv2025

Anisotropic Strain Engineering in La0.7Sr0.3MnO3/LaFeO3 Superlattice: Structural Relaxation and Domain Formation

Anisotropic strain engineering in epitaxial oxide films provides new opportunities to control the antiferromagnetic and structural properties crucial for advancements of antiferromagnetic spintronics. Here we report on a (La0.7Sr0.3MnO3/LaFeO3)4 superlattice grown on (101)o DyScO3 substrate which imposes significant anisotropic in-plane strain. Reciprocal space mapping reveals selective strain relaxation along the tensile in-plane [010]o axis, while compression along the perpendicular in-plane [-101]o axis remains strained. Scanning precession electron diffraction and higher-order Laue zone analysis show that the relaxation is accommodated by structural domain formation in the LaFeO3 layers, initiating from the second bilayer and propagating out-of-plane. These domains minimise structural defects and correlate with the substrate step edges. X-ray magnetic dichroism measurements reveal bulk-like in-plane antiferromagnetic order with polydomain signature as previously reported. Our findings reveal the presence of structural domains coexisting with antiferromagnetic polydomain states, showing a strain-domain-magnetism relationship that provides insights for applications of strain engineering in spintronics applications.

cond-mat.mtrl-sci↗

arXiv2025

Absence of detectable spin and orbital pumping from Ni to Nb by out-of-plane ferromagnetic resonance

Excited ferromagnets can pump spin angular momentum, along with possibly orbital angular momentum. Among elemental ferromagnets, Ni has been proposed to exhibit substantial orbital pumping relative to spin pumping. Here, we search for a signature of orbital pumping by Ni, specifically by comparing out-of-plane ferromagnetic resonance in heterostructures without Ni (FeV/Nb) and with Ni (FeV-Ni/Nb). The FeV/Nb series shows a clear increase in Gilbert damping with the Nb sink thickness, attributed to spin pumping from FeV to Nb. Surprisingly, the FeV-Ni/Nb series exhibits no such damping increase, revealing no significant spin or orbital pumping from Ni to Nb. Our results offer a fresh perspective on angular-momentum transfer in Ni-based heterostructures, suggesting that the interpretation of some strong orbitronic effects may require further consideration.

cond-mat.mes-hall↗

arXiv2025

Electronic origin of delicate antiferromagnetism in Fe$_{x}$NbS$_2$

Among the family of intercalated transition-metal dichalcogenides (TMDs), Fe$_{x}$NbS$_2$ is found to possess unique current-induced resistive switching behaviors, tunable antiferromagnetic states, and a commensurate charge order, all of which are tied to a critical Fe doping of $x_c$ = 1/3. However, the electronic origin of such extreme stoichiometry sensitivities remains unclear. Combining angle-resolved photoemission spectroscopy (ARPES) with density functional theory (DFT) calculations, we identify and characterize a dramatic eV-scale electronic restructuring that occurs across the $x_c$. Moment-carrying Fe 3$d_{z^2}$ electrons manifest as narrow bands within 200 meV of the Fermi level, distinct from other transition metal intercalated TMD magnets. These states strongly hybridize with itinerant electrons in TMD layer, rapidly lose coherence above $x_c$ due to correlation-driven effects. This sudden quasiparticle decoherence collapses the Fe-Nb hybridization, which explicitly suppresses the out-of-plane effective Fe-Fe exchange interaction, driving the transformation of the magnetic ground state from an antiferromagnetic stripe phase to a zigzag phase. These observations resemble the exceptional electronic and magnetic sensitivity of strongly correlated systems, and demonstrate that quantifying orbital-specific hybridization via ARPES offers an alternative pathway to evaluate effective magnetic exchange in metallic magnets, complementing inelastic neutron and resonant x-ray scattering probes.

cond-mat.str-el↗

arXiv2025

Janus-faced influence of oxygen vacancy in high entropy oxide films with Mott electrons

Contrary to traditional approaches, high entropy oxides (HEOs) strategically employ cationic disorder to engineer tunable functionalities. This disorder, stemming from multiple elements at the same crystallographic site, disrupts local symmetry and induces local distortions. By examining a series of single-crystalline [La$_{0.2}$Pr$_{0.2}$Nd$_{0.2}$Sm$_{0.2}$Eu$_{0.2}$]NiO$_{3-δ}$ thin films, we demonstrate herein that the creation of oxygen vacancies (OVs) further offers a powerful means of tailoring electronic behavior of HEOs by concurrently introducing disorder in the oxygen sublattice and doping electrons into the system. Increasing OV concentration leads to a monotonic increase in room-temperature sheet resistance. A striking feature is the Janus-faced response of the metal-insulator transition (MIT) to OVs due to the interplay among correlation energy scales, electron doping, and disorder. Unlike the monotonous influence of OV observed for the MIT in VO$_2$ and V$_2$O$_3$, initial OV doping lowers the MIT temperature here, whereas higher OV levels completely suppress the metallic phase. Magnetotransport measurements further reveal weak localization, strong localization as a function of $δ$. Moreover, the disorder on both $RE$ and oxygen sublattices is responsible for the Mott-Anderson insulator state. These findings surpass the scope of the recently featured `electron antidoping' effect and demonstrate the promising opportunity to utilize OV engineering of HEOs for Mottronics and optoelectronics applications.

cond-mat.str-el↗

arXiv2025

Interfacial reconstruction effects in insulating double perovskite Nd$_2$NiMnO$_6$/SrTiO$_3$ and Nd$_2$NiMnO$_6$/NdGaO$_3$ thin films

Ferromagnetic insulating (FMI) double perovskite oxides (DPOs) $A_2BB'$O$_6$ with near-room-temperature Curie temperatures are promising candidates for ambient-temperature spintronics applications. To realize their potential, epitaxial stabilization of DPO films and understanding the effect of multiple broken symmetries across the film/substrate interface are crucial. This study investigates ultrathin films of the FMI Nd$_2$NiMnO$_6$ (NNMO) grown on SrTiO$_3$ (STO) and NdGaO$_3$ (NGO) substrates. By comparing growth on these substrates, we examine the influence of polarity and structural symmetry mismatches, which are absent in the NGO system. The interface exhibits immeasurable resistance in both cases. Using synchrotron X-ray diffraction, we show that films have three octahedral rotational domains because of the structural symmetry mismatch with the STO substrate. Furthermore, our coherent Bragg rod analysis of specular X-ray diffraction reveals a significant modification of the out-of-plane lattice parameter within a few unit cells at the film/substrate interface and the surface. This arises from polarity compensation and surface symmetry breaking, respectively. These structural alterations influence the Mn orbital symmetry, a dependence that we further confirm through X-ray linear dichroism measurements. Since the ferromagnetism in insulating DPOs is mediated by orbital-dependent superexchange interactions [Phys. Rev. Lett. 100, 186402 (2008)], our study provides a framework for understanding the evolution of magnetism in ultrathin geometry.

cond-mat.mtrl-sci↗

arXiv2025

Local structural distortions drive magnetic molecular field in compositionally complex spinel oxide

Understanding how local distortions determine the functional properties of high entropy materials, containing five or more elements at a crystallographic site, is an open challenge. We address this for a compositionally complex spinel oxide (Mn$_{0.2}$Co$_{0.2}$Ni$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$)Cr$_2$O$_4$ ($A^5$Cr$_2$O$_4$). By comparatively examining extended X-ray absorption fine structure on $A^5$Cr$_2$O$_4$ and its parent counterparts $A$Cr$_2$O$_4$ along with density functional theory calculations for multiple configurations, we find that the element-specific distortions go beyond the first neighbor. Specifically, the strong Jahn-Teller distortion present in CuCr$_2$O$_4$ is found to be completely suppressed in $A^5$Cr$_2$O$_4$. Instead, there is a broad distribution of Cu-O and Cu-Cr bond distances while other $A$-O distances acquire certain specific values. This study demonstrates the additional flexibility of a cationic sublattice in maintaining a uniform long-range structure, in contrast to previous reports showing only the accommodative anionic sublattice. Remarkably, despite the presence of multiple magnetic ions and variable bond lengths, the mean field magnetic interactions of $A^5$Cr$_2$O$_4$ exhibit a striking resemblance to those of NiCr$_2$O$_4$. This compelling observation originates from the comparability of bond lengths around Cr in both materials. Our study paves the way for a deeper understanding of the impact of local structural distortions in compositionally complex quantum materials, enabling the targeted design with tailored properties.

cond-mat.mtrl-sci↗

arXiv2025

Site-selective polar compensation of Mott electrons in a double perovskite heterointerface

Double perovskite oxides (DPOs) with two transition metal ions ($A_2$$BB^\prime$O$_6$) offer a fascinating platform for exploring exotic physics and practical applications. Studying these DPOs as ultrathin epitaxial thin films on single crystalline substrates can add another dimension to engineering electronic, magnetic, and topological phenomena. Understanding the consequence of polarity mismatch between the substrate and the DPO would be the first step towards this broad goal. We investigate this by studying the interface between a prototypical insulating DPO Nd$_2$NiMnO$_6$ and a wide-band gap insulator SrTiO$_3$. The interface is found to be insulating in nature. By combining several experimental techniques and density functional theory, we establish a site-selective charge compensation process that occurs explicitly at the Mn site of the film, leaving the Ni sites inert. We further demonstrate that such surprising selectivity, which cannot be explained by existing mechanisms of polarity compensation, is directly associated with their electronic correlation energy scales. This study establishes the crucial role of Mott physics in polar compensation process and paves the way for designer doping strategies in complex oxides.

cond-mat.mtrl-sci↗

arXiv2025

Spin frustration and unconventional spin twisting state in van der Waals ferromagnet/antiferromagnet heterostructures

Atomically flat surfaces of van der Waals (vdW) materials pave an avenue for addressing a long-standing fundamental issue of how a perfectly compensated antiferromagnet (AFM) surface frustrates a ferromagnetic (FM) overlayer in FM/AFM heterostructures. By revealing the AFM and FM spin structures separately in vdW Fe5GeTe2/NiPS3 heterostructures, we find that C-type in-plane AFM NiPS3 develops three equivalent AFM domains which are robust against external magnetic field and magnetic coupling with Fe5GeTe2. Consequently, spin frustration at the Fe5GeTe2/NiPS3 interface was shown to develop a perpendicular Fe5GeTe2 magnetization in the interfacial region that switches separately from the bulk of the Fe5GeTe2 magnetizations. In particular, we discover an unconventional spin twisting state that the Fe5GeTe2 spins twist from perpendicular direction near the interface to in-plane direction away from the interface in Fe5GeTe2/NiPS3. Our finding of the twisting spin texture is a unique property of spin frustration in van der Waals magnetic heterostructures.

cond-mat.mtrl-sci↗

arXiv2023

Spectral Evidence for Local-Moment Ferromagnetism in van der Waals Metals Fe$_3$GaTe$_2$ and Fe$_3$GeTe$_2$

Magnetism in two-dimensional (2D) materials has attracted considerable attention recently for both fundamental understanding of magnetism and their tunability towards device applications. The isostructural Fe$_3$GeTe$_2$ and Fe$_3$GaTe$_2$ are two members of the Fe-based van der Waals (vdW) ferromagnet family, but exhibit very different Curie temperatures (T$_C$) of 210 K and 360 K, respectively. Here, by using angle-resolved photoemission spectroscopy and density functional theory, we systematically compare the electronic structures of the two compounds. Qualitative similarities in the Fermi surface can be found between the two compounds, with expanded hole pockets in Fe$_3$GaTe$_2$ suggesting additional hole carriers compared to Fe$_3$GeTe$_2$. Interestingly, we observe no band shift in Fe$_3$GaTe$_2$ across its T$_C$ of 360 K, compared to a small shift in Fe$_3$GeTe$_2$ across its T$_C$ of 210 K. The weak temperature-dependent evolution strongly deviates from the expectations of an itinerant Stoner mechanism. Our results suggest that itinerant electrons have minimal contributions to the enhancement of T$_C$ in Fe$_3$GaTe$_2$ compared to Fe$_3$GeTe$_2$, and that the nature of ferromagnetism in these Fe-based vdW ferromagnets must be understood with considerations of the electron correlations.

cond-mat.str-el↗

arXiv2023

Suppression of Spin Pumping at Metal Interfaces

An electrically conductive metal typically transmits or absorbs a spin current. Here, we report on evidence that interfacing two metal thin films can suppress spin transmission and absorption. We examine spin pumping in ferromagnet/spacer/ferromagnet heterostructures, in which the spacer -- consisting of metallic Cu and Cr thin films -- separates the ferromagnetic spin-source and spin-sink layers. The Cu/Cr spacer largely suppresses spin pumping -- i.e., neither transmitting nor absorbing a significant amount of spin current -- even though Cu or Cr alone transmits a sizable spin current. The antiferromagnetism of Cr is not essential for the suppression of spin pumping, as we observe similar suppression with Cu/V spacers where V is a nonmagnetic analogue of Cr. We speculate that diverse combinations of spin-transparent metals may form interfaces that suppress spin pumping, although the underlying mechanism remains unclear. Our work may stimulate a new perspective on understanding and engineering spin transport in metallic multilayers.

cond-mat.mtrl-sci↗

arXiv2023

Orthorhombic distortion drives orbital ordering in an antiferromagnetic 3$d^1$ Mott insulator

The orbital, which represents the shape of the electron cloud, very often strongly influences the manifestation of various exotic phenomena, e.g., magnetism, metal-insulator transition, colossal magnetoresistance, unconventional superconductivity etc. in solid-state systems. The observation of the antiferromagnetism in $RE$TiO$_3$ ($RE$=rare earth) series has been puzzling since the celebrated Kugel-Khomskii model of spin-orbital super exchange predicts ferromagnetism in an orbitally degenerate $d^1$ systems. Further, the existence of the orbitally ordered vs. orbital liquid phase in both antiferromagnetic and paramagnetic phase have been unsettled issues thus far. To address these long-standing questions, we investigate single crystalline film of PrTiO$_3$. Our synchrotron X-ray diffraction measurements confirm the retention of bulk-like orthorhombic ($D_{2h}$) symmetry in the thin film geometry. We observe similar X-ray linear dichroism signal in both paramagnetic and antiferromagnetic phase, which can be accounted by ferro orbital ordering (FOO). While the presence of $D_{2h}$ crystal field does not guarantee lifting of orbital degeneracy always, we find it to be strong enough in these rare-earth titanates, leading to the FOO state. Thus, our work demonstrates the orthorhombic distortion is the driving force for the orbital ordering of antiferromagnetic $RE$TiO$_3$.

cond-mat.str-el↗