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Alexander J. Grutter

Publications and source records attributed to Alexander J. Grutter.

At least 19 recordsLinked to original sources

Electrical manipulation and detection of perpendicular altermagnetic order via proximitized Dirac semimetal

Altermagnets, which combine antiferromagnetic-like magnetic compensation with ferromagnetic-like broken time-reversal symmetry, hold great promise for high-density and ultrafast spintronic applications. However, the detection and switching of perpendicular altermagnetic order are fundamentally constrained by magnetic symmetry, restricting both fundamental studies and practical implementation. We realize robust electrical reading and deterministic switching of perpendicular altermagnetic order by designing a Dirac semimetal/altermagnet heterostructure of PtTe2/CrSb. This engineered interface enables anomalous Hall readout via altermagnetic proximity effect and delivers efficient spin-orbit torque for manipulating the epitaxial perpendicular Neel vector in CrSb. These findings significantly broaden the functional scope of altermagnetic heterostructures and pave the way for highly scalable altermagnetic memory.

cond-mat.mtrl-sci

Synthesis of Bulk Superconducting LiNbO$_2$ Crystals through CaH$_2$ Reduction

We have synthesized layered superconducting LiNbO$_2$ crystals through a bulk phase transformation from LiNbO$_3$ single crystals via CaH$_2$ reduction. As the Nb valence is reduced from 5+ to 3+, the material undergoes a structural transformation to the resulting product, LiNbO$_2$, which is accompanied by metallic behavior and a superconducting transition, Tc onset, as high as 14.4 K. Secondary ion mass spectroscopy (SIMS) and X-ray photoelectron spectroscopy (XPS) show that the resulting phase is hole-doped through de-lithiation during the reduction. Magnetization and AC susceptibility measurements from a tunnel diode resonator confirm the bulk nature of superconductivity with a superconducting volume fraction of approximately 77% and an upper critical field approaching 26 T. Our study demonstrates extreme hydride reduction as an effective method to induce phase transformations with non-topotactic pathways and can be used to synthesize bulk materials with exotic properties.

cond-mat.supr-con

Tailoring Emergent Magnetic Moment in La$_{0.7}$Sr$_{0.3}$MnO$_3$-Bi$_2$Te$_3$ Heterostructures via Interfacial Reconstructions

We report emergent magnetic behavior in heterostructures composed of (111)-oriented La$_{0.7}$Sr$_{0.3}$MnO$_3$ (LSMO) and (00$l$)-oriented Bi$_2$Te$_3$ (BT), controlled by interfacial reconstructions. When BT is deposited directly onto LSMO, an intermediate interfacial layer forms between the two materials. Polarized Neutron Reflectometry modeling reveals that this reconstructed region stabilizes a secondary magnetically ordered phase that is coupled to the underlying ferromagnetic LSMO layer. As a consequence, the heterostructures exhibit unconventional self-crossing magnetic hysteresis loops at room temperature, characterized by a reversal of the net magnetization at low applied fields. In contrast, the introduction of a tellurium seed layer results in a sharper LSMO-BT interface, while preserving the anomalous hysteresis behavior and enhancing the saturation magnetization. Element-specific X-ray absorption spectroscopy suggests that the emergent magnetic phase originates from the chemical reconstruction of manganese species. These results demonstrate that interface engineering in magnetic oxide-topological insulator heterostructures provides a pathway to control emergent magnetic coupling and emergent magnetic states in oxide-topological insulator heterostructures.

cond-mat.mtrl-sci

Surface-State-Driven Anomalous Hall Effect in Altermagnetic MnTe Films

Altermagnets have recently emerged as a new class of magnetic materials that combine compensated magnetic order with spin-split electronic band structures. In this work, we employ molecular beam epitaxy to grow MnTe thin films with controlled thickness on InP(111)A substrates. By performing angle-resolved photoemission spectroscopy measurements, we observe a large spin splitting of ~230 meV for bulk bands well below the Fermi level and identify surface states that cross the Fermi level. Electrical transport measurements reveal that a robust anomalous Hall (AH) effect persists down to 2 K and an AH sign reversal occurs near 175 K. By systematically tuning film thickness, growth conditions, and interfacial structure, we demonstrate that the AH response in MnTe films originates from the Berry curvature of surface states rather than from bulk bands. Our first-principles calculations reveal that this surface-state-driven AH effect is imprinted by the bulk altermagnetic order and remains unchanged for terminations with opposite Mn magnetic orientations. Our results establish a unique surface transport probe of bulk altermagnetism, demonstrate interface engineering as an effective route to generate and control the AH effect in altermagnets, and provide a unified understanding of the AH response in altermagentic MnTe films.

cond-mat.mtrl-sci

Emergence of unconventional magnetic order in strain-engineered RuO2/TiO2 superlattices

The spin ordering in RuO2 remains a highly debated topic, owing to its elusive nature, with reports ranging from a nonmagnetic ground state to signatures of unconventional magnetic order. Here we provide the first unambiguous, and direct evidence of unconventional magnetism in epitaxial, fully strained RuO2/TiO2 superlattices on TiO2 (110) substrate grown by hybrid molecular beam epitaxy. Polarized neutron reflectometry reveals a finite magnetic moment localized within the compressively strained RuO2 layers, consistent with predictions obtained from first-principles calculations. Complementary density functional theory and X-ray photoemission spectroscopy show that epitaxial strain drives the Ru 4d states toward the Fermi level, triggering a Stoner-type instability that stabilizes non-compensated magnetic order. These unique results reveal that RuO2 exhibits unconventional magnetic states under epitaxial strain, which are not accessible in bulk and establish strain engineering as a powerful route to uncover and control magnetic phases in RuO2 and related oxides.

cond-mat.mtrl-sci

Net Magnetization and Inhomogeneous Magnetic Order in a High-Tc Nickelate Superconductor

High-temperature and high-magnetic-field-induced re-entrant superconductivity has been discovered in the infinite-layer nickelate $\mathrm{Sm_{1-x-y} Eu_x Ca_y Ni O_2}$ (SECNO). Infinite-layer nickelates are the closest known analogues of high-$\mathrm{T}_c$ cuprate superconductors, yet they host distinct magnetic ground states. Using low-energy muon spin relaxation and polarized neutron reflectometry, we reveal the magnetic order in SECNO. We find that magnetic freezing occurs at a higher-temperature than in other nickelate compounds, and that a substantial net magnetization of 55 $\,\mathrm{kA}\,\mathrm{m}^{-1}$ $\pm10 \,\mathrm{kA}\,\mathrm{m}^{-1}$ emerges and remains largely unchanged across the superconducting transition. The magnetism in SECNO is disordered and nonuniform.

cond-mat.supr-con

Examining the Spin Structure of Altermagnetic Candidate MnTe Grown with Near Ideal Stoichiometry

Altermagnets are a recently-discovered class of materials with magnetic ordering that have a zero net magnetization and a momentum-dependent spin splitting in their band structure, arising from a collinear spin arrangement with alternating polarizations in the crystal lattice. The nickeline-structured manganese telluride ({\alpha}-MnTe) is an attractive altermagnet candidate due to its predicted large spin splitting energy and a transition temperature near 300K. In this work, we present a thorough investigation of the spin structure of {\alpha}-MnTe thin films grown by molecular beam epitaxy with very high crystal quality and low residual magnetization. The epitaxial {\alpha}-MnTe films have a full-width-at-half-maximum of 0.1{\deg} as measured by x-ray-diffraction rocking curves and a root-mean-square roughness below 1 nm. Neutron diffraction measurements confirm the antiferromagnetic order in the {\alpha}-MnTe film and show a N\'eel temperature of 307 K. Polarized neutron reflectometry detects a vanishingly small net magnetization which may be confined to the MnTe/InP interface, highlighting the near-ideal stoichiometry in the sample. In vacuo angle resolved photoemission spectroscopy reveals that the bulk band spectrum of the MnTe films is consistent with the weak altermagnetic order as theoretically predicted and observed for the high symmetry nodal plane in the center of the Brillouin zone. This study establishes optimized growth conditions for the synthesis of stoichiometric {\alpha}-MnTe thin films which exhibit exceptional structural and magnetic ordering, thereby providing a robust platform for the precise characterization of their altermagnetic properties.

cond-mat.mtrl-sci

Topotactic oxidation of Ruddlesden-Popper nickelates reveals new structural family: oxygen-intercalated layered perovskites

Layered perovskites such as the Dion-Jacobson, Ruddlesden-Popper, and Aurivillius families host a wide range of correlated electron phenomena, from high-temperature superconductivity to multiferroicity. Here we report a new family of layered perovskites, realized through topotactic oxygen intercalation of La_{n+1}Ni_{n}O_{3n+1} (n=1-4) Ruddlesden-Popper nickelate thin films grown by ozone-assisted molecular-beam epitaxy. Post-growth ozone annealing induces a large c-axis expansion - 17.8% for La_{2}NiO_{4} (n=1) - that monotonically decreases with increasing n. Surface X-ray diffraction coupled with Coherent Bragg Rod Analysis reveals that this structural expansion arises from the intercalation of approximately 0.7 oxygen atoms per formula unit into interstitial sites within the rock salt spacer layers. The resulting structures exhibit a spacer layer composition intermediate between that of the Ruddlesden-Popper and Aurivillius phases, defining a new class of layered perovskites. Oxygen-intercalated nickelates exhibit metallicity and significantly enhanced nickel-oxygen hybridization, a feature linked to high-temperature superconductivity. Our work establishes topotactic oxidation as a powerful synthetic approach to accessing highly oxidized, metastable phases across a broad range of layered oxide systems, offering new platforms to tune properties via spacer-layer chemistry.

cond-mat.mtrl-sci

Unconventional polaronic ground state in superconducting LiTi$_2$O$_4$

Geometrically frustrated lattices can display a range of correlated phenomena, ranging from spin frustration and charge order to dispersionless flat bands due to quantum interference. One particularly compelling family of such materials is the half-valence spinel Li$B_2$O$_4$ materials. On the $B$-site frustrated pyrochlore sublattice, the interplay of correlated metallic behavior and charge frustration leads to a superconducting state in LiTi$_2$O$_4$ and heavy fermion behavior in LiV$_2$O$_4$. To date, however, LiTi$_2$O$_4$ has primarily been understood as a conventional BCS superconductor despite a lattice structure that could host more exotic groundstates. Here, we present a multimodal investigation of LiTi$_2$O$_4$, combining ARPES, RIXS, proximate magnetic probes, and ab-initio many-body theoretical calculations. Our data reveals a novel mobile polaronic ground state with spectroscopic signatures that underlie co-dominant electron-phonon coupling and electron-electron correlations also found in the lightly doped cuprates. The cooperation between the two interaction scales distinguishes LiTi$_2$O$_4$ from other superconducting titanates, suggesting an unconventional origin to superconductivity in LiTi$_2$O$_4$. Our work deepens our understanding of the rare interplay of electron-electron correlations and electron-phonon coupling in unconventional superconducting systems. In particular, our work identifies the geometrically frustrated, mixed-valence spinel family as an under-explored platform for discovering unconventional, correlated ground states.

cond-mat.supr-con

Altermagnetic band splitting in 10 nm epitaxial CrSb thin films

Altermagnets are a newly identified family of collinear antiferromagnets with momentum-dependent spin-split band structure of non-relativistic origin, derived from spin-group symmetry-protected crystal structures. Among candidate altermagnets, CrSb is attractive for potential applications because of a large spin-splitting near the Fermi level and a high Neel transition temperature of around 700 K. We use molecular beam epitaxy to synthesize CrSb (0001) thin films with thicknesses ranging from 10 nm to 100 nm. Structural characterization, using reflection high energy electron diffraction, scanning transmission electron microscopy, and X-ray diffraction, demonstrates the growth of epitaxial films with good crystallinity. Polarized neutron reflectometry shows the absence of any net magnetization, consistent with antiferromagnetic order. In vacuo angle resolved photoemission spectroscopy (ARPES) measurements probe the band structure in a previously unexplored regime of film thickness, down to 10 nm. These ARPES measurements show a three-dimensional momentum-dependent band splitting of up to 0.7 eV with g-wave symmetry, consistent with that seen in prior studies of bulk single crystals. The distinct altermagnetic band structure required for potential spin-transport applications survives down to the 10 nm thin film limit at room temperature.

cond-mat.mtrl-sci

Complex Magnetic Ordering in Candidate Topological Superconductors

The search for chiral topological superconductivity in magnetic topological insulator (TI)-FeTe heterostructures is a key frontier in condensed matter physics, with potential applications in topological quantum computing. The combination of ferromagnetism, superconductivity, and topologically nontrivial surface states brings together the key elements required for chiral Majorana physics. In this work, we examine the interplay between magnetism and superconductivity at the interfaces between FeTe and a series of TI overlayers. In superconducting MnBi$_2$Te$_4$/FeTe, any interfacial suppression of antiferromagnetism must affect at most a few nanometers. On the other hand, (Bi,Sb)$_2$Te$_3$/FeTe layers exhibit near-total suppression of antiferromagnetic ordering. Ferromagnetic Cr$_x$(Bi,Sb)$_{2-x}$Te$_3$ (CBST)/FeTe bilayers exhibit net magnetization in both CBST and FeTe layers, with evidence of interactions between superconductivity and ferromagnetism. These observations identify magnetic TI/FeTe interfaces as an exceptionally robust platform to realize chiral topological superconductivity.

cond-mat.supr-con

Vertically Graded Fe-Ni Alloys with Low Damping and a Sizeable Spin-Orbit Torque

Energy-efficient spintronic devices require a large spin-orbit torque (SOT) and low damping to excite magnetic precession. In conventional devices with heavy-metal/ferromagnet bilayers, reducing the ferromagnet thickness to $\sim$1 nm enhances the SOT but dramatically increases damping. Here, we investigate an alternative approach based on a 10 nm thick single-layer ferromagnet to attain both low damping and a sizable SOT. Instead of relying on a single interface, we continuously break the bulk inversion symmetry with a vertical compositional gradient of two ferromagnetic elements: Fe with low intrinsic damping and Ni with sizable spin-orbit coupling. We find low effective damping parameters of $\alpha_\mathrm{eff} < 5\times10^{-3}$ in the FeNi alloy films, despite the steep compositional gradients. Moreover, we reveal a sizable anti-damping SOT efficiency of $|\theta_\mathrm{DL}| \approx 0.05$, even without an intentional compositional gradient. Through depth-resolved x-ray diffraction, we identify a lattice strain gradient as crucial symmetry breaking that underpins the SOT. Our findings provide fresh insights into damping and SOTs in single-layer ferromagnets for power-efficient spintronic devices.

cond-mat.mtrl-sci

Hydrogen is not necessary for superconductivity in topotactically reduced nickelates

A key open question in the study of layered superconducting nickelate films is the role that hydrogen incorporation into the lattice plays in the appearance of the superconducting state. Due to the challenges of stabilizing highly crystalline square planar nickelate films, films are prepared by the deposition of a more stable parent compound which is then transformed into the target phase via a topotactic reaction with a strongly reducing agent such as CaH$_2$. Recent studies, both experimental and theoretical, have introduced the possibility that the incorporation of hydrogen from the reducing agent into the nickelate lattice may be critical for the superconductivity. In this work, we use secondary ion mass spectrometry to examine superconducting La$_{1-x}$X$_x$NiO$_2$ / SrTiO$_3$ (X = Ca and Sr) and Nd$_6$Ni$_5$O$_{12}$ / NdGaO$_3$ films, along with non-superconducting NdNiO$_2$ / SrTiO$_3$ and (Nd,Sr)NiO$_2$ / SrTiO$_3$. We find no evidence for extensive hydrogen incorporation across a broad range of samples, including both superconducting and non-superconducting films. Theoretical calculations indicate that hydrogen incorporation is broadly energetically unfavorable in these systems, supporting our conclusion that hydrogen incorporation is not generally required to achieve a superconducting state in layered square-planar nickelates.

cond-mat.supr-con

Coexistence of Superconductivity and Antiferromagnetism in Topological Magnet MnBi2Te4 Films

The interface of two materials can harbor unexpected emergent phenomena. One example is interface-induced superconductivity. In this work, we employ molecular beam epitaxy to grow a series of heterostructures formed by stacking together two non-superconducting antiferromagnetic materials, an intrinsic antiferromagnetic topological insulator MnBi2Te4 and an antiferromagnetic iron chalcogenide FeTe. Our electrical transport measurements reveal interface-induced superconductivity in these heterostructures. By performing scanning tunneling microscopy and spectroscopy measurements, we observe a proximity-induced superconducting gap on the top surface of the MnBi2Te4 layer, confirming the interaction between superconductivity and antiferromagnetism in the MnBi2Te4 layer. Our findings will advance the fundamental inquiries into the topological superconducting phase in hybrid devices and provide a promising platform for the exploration of chiral Majorana physics in MnBi2Te4-based heterostructures.

cond-mat.supr-con

Interface-Induced Superconductivity in Magnetic Topological Insulator-Iron Chalcogenide Heterostructures

When two different electronic materials are brought together, the resultant interface often shows unexpected quantum phenomena, including interfacial superconductivity and Fu-Kane topological superconductivity (TSC). Here, we use molecular beam epitaxy (MBE) to synthesize heterostructures formed by stacking together two magnetic materials, a ferromagnetic topological insulator (TI) and an antiferromagnetic iron chalcogenide (FeTe). We discover emergent interface-induced superconductivity in these heterostructures and demonstrate the trifecta occurrence of superconductivity, ferromagnetism, and topological band structure in the magnetic TI layer, the three essential ingredients of chiral TSC. The unusual coexistence of ferromagnetism and superconductivity can be attributed to the high upper critical magnetic field that exceeds the Pauli paramagnetic limit for conventional superconductors at low temperatures. The magnetic TI/FeTe heterostructures with robust superconductivity and atomically sharp interfaces provide an ideal wafer-scale platform for the exploration of chiral TSC and Majorana physics, constituting an important step toward scalable topological quantum computation.

cond-mat.mes-hall

Skyrmion-Excited Spin Wave Fractal Network

Magnetic skyrmions exhibit unique, technologically relevant pseudo-particle behaviors which arise from their topological protection, including well-defined, three-dimensional dynamic modes that occur at microwave frequencies. During dynamic excitation, spin waves are ejected into the interstitial regions between skyrmions, creating the magnetic equivalent of a turbulent sea. However, since the spin waves in these systems have a well-defined length scale, and the skyrmions are on an ordered lattice, ordered structures from spin wave interference can precipitate from the chaos. This work uses small angle neutron scattering (SANS) to capture the dynamics in hybrid skyrmions and investigate the spin wave structure. Performing simultaneous ferromagnetic resonance and SANS, the diffraction pattern shows a large increase in low-angle scattering intensity which is present only in the resonance condition. This scattering pattern is best fit using a mass fractal model, which suggests the spin waves form a long-range fractal network. The fractal structure is constructed of fundamental units with a size that encodes the spin wave emissions and are constrained by the skyrmion lattice. These results offer critical insights into the nanoscale dynamics of skyrmions, identify a new dynamic spin wave fractal structure, and demonstrates SANS as a unique tool to probe high-speed dynamics.

cond-mat.mtrl-sci

Constraints on proximity-induced ferromagnetism in a Dirac semimetal (Cd$_3$As$_2$)/ferromagnetic semiconductor (Ga$_{1-x}$Mn$_x$Sb) heterostructure

Breaking time-reversal symmetry in a Dirac semimetal Cd$_3$As$_2$ through doping with magnetic ions or by the magnetic proximity effect is expected to cause a transition to other topological phases (such as a Weyl semimetal). To this end, we investigate the possibility of proximity-induced ferromagnetic ordering in epitaxial Dirac semimetal (Cd$_3$As$_2$)/ferromagnetic semiconductor (Ga$_{1-x}$Mn$_x$Sb) heterostructures grown by molecular beam epitaxy. We report the comprehensive characterization of these heterostructures using structural probes (atomic force microscopy, x-ray diffraction, scanning transmission electron microscopy), angle-resolved photoemission spectroscopy, electrical magneto-transport, magnetometry, and polarized neutron reflectometry. Measurements of the magnetoresistance and Hall effect in the temperature range 2 K - 20 K show signatures that could be consistent with either a proximity effect or spin-dependent scattering of charge carriers in the Cd$_3$As$_2$ channel. Polarized neutron reflectometry sets constraints on the interpretation of the magnetotransport studies by showing that (at least for temperatures above 6 K) any induced magnetization in the Cd$_3$As$_2$ itself must be relatively small ($<$ 14 emu/cm$^3$).

cond-mat.mtrl-sci

Three-Dimensional Structure of Hybrid Magnetic Skyrmions Determined by Neutron Scattering

Magnetic skyrmions are topologically protected chiral spin textures which present opportunities for next-generation magnetic data storage and logic information technologies. The topology of these structures originates in the geometric configuration of the magnetic spins - more generally described as the structure. While the skyrmion structure is most often depicted using a 2D projection of the three-dimensional structure, recent works have emphasized the role of all three dimensions in determining the topology and their response to external stimuli. In this work, grazing-incidence small-angle neutron scattering and polarized neutron reflectometry are used to determine the three-dimensional structure of hybrid skyrmions. The structure of the hybrid skyrmions, which includes a combination of Néel-like and Bloch-like components along their length, is expected to significantly contribute to their notable stability, which includes ambient conditions. To interpret the neutron scattering data, micromagnetic simulations of the hybrid skyrmions were performed, and the corresponding diffraction patterns were determined using a Born approximation transformation. The converged magnetic profile reveals the magnetic structure along with the skyrmion depth profile, including the thickness of the Bloch and Néel segments and the diameter of the core.

cond-mat.mes-hall