arXiv subjects

E. Arenholz

Publications and source records attributed to E. Arenholz.

At least 19 recordsLinked to original sources

arXiv2023

Observation of Coherently Coupled Cation Spin Dynamics in an Insulating Ferrimagnetic Oxide

Many technologically useful magnetic oxides are ferrimagnetic insulators, which consist of chemically distinct cations. Here, we examine the spin dynamics of different magnetic cations in ferrimagnetic NiZnAl-ferrite (Ni$_{0.65}$Zn$_{0.35}$Al$_{0.8}$Fe$_{1.2}$O$_4$) under continuous microwave excitation. Specifically, we employ time-resolved x-ray ferromagnetic resonance to separately probe Fe$^{2+/3+}$ and Ni$^{2+}$ cations on different sublattice sites. Our results show that the precessing cation moments retain a rigid, collinear configuration to within $\approx$2$^\circ$. Moreover, the effective spin relaxation is identical to within $<$10% for all magnetic cations in the ferrite. We thus validate the oft-assumed ``ferromagnetic-like'' dynamics in resonantly driven ferrimagnetic oxides, where the magnetic moments from different cations precess as a coherent, collective magnetization.

cond-mat.mtrl-sci↗

arXiv2019

Possible Scale Invariant Linear Magnetoresistance in Pyrochlore Iridates Bi$_2$Ir$_2$O$_7$

We report the observation of a linear magnetoresistance in single crystals and epitaxial thin films of the pyrochlore iridate Bi$_2$Ir$_2$O$_7$. The linear magnetoresistance is positive and isotropic at low temperatures, without any sign of saturation up to 35 Tesla. As temperature increases, the linear field dependence gradually evolves to a quadratic field dependence. The temperature and field dependence of magnetoresistance of Bi$_2$Ir$_2$O$_7$ bears strikingly resemblance to the scale invariant magnetoresistance observed in the strange metal phase in high Tc cuprates. However, the residual resistivity of Bi$_2$Ir$_2$O$_7$ is more than two orders of magnitude higher than the curpates. Our results suggest that the correlation between linear magnetoresistance and quantum fluctuations may exist beyond high temperature superconductors.

cond-mat.str-el↗

arXiv2019

Quantum spin liquids by geometric lattice design

On a lattice composed of triangular plaquettes where antiferromagnetic exchange interactions between localized spins cannot be simultaneously satisfied, the system becomes geometrically frustrated with magnetically disordered phases remarkably different from a simple paramagnet. Spin liquid belongs to one of these exotic states, in which a macroscopic degeneracy of the ground state gives rise to the rich spectrum of collective phenomena. Here, we report on the discovery of a new magnetic state in the heterostructures derived from a single unit cell (111)-oriented spinel CoCr2O4 sandwiched between nonmagnetic Al2O3 spacers. The artificial quasi-two-dimensional material composed of three triangle and one kagome atomic planes shows a degree of magnetic frustration which is almost two orders of magnitude enlarged compared to the bulk crystals. Combined resonant X-ray absorption and torque magnetometry measurements confirm that the designer system exhibits no sign of spin ordering down to 30 mK, implying a possible realization of a quantum spin liquid state in the two dimensional limit.

cond-mat.str-el↗

arXiv2019

Coherent ac spin current transmission across an antiferromagnetic CoO insulator

The recent discovery of spin-current transmission through antiferromagnetic (AFM) insulating materials opens up unprecedented opportunities for fundamental physics and spintronics applications. The great mystery currently surrounding this topic is: how could THz AFM magnons mediate a GHz spin current? This mis-match of frequencies becomes particularly critical for the case of coherent ac spin-current, raising the fundamental question of whether a GHz ac spin-current can ever keep its coherence inside an AFM insulator and so drive the spin precession of another FM layer coherently? Utilizing element- and time-resolved x-ray pump-probe measurements on Py/Ag/CoO/Ag/Fe75Co25/MgO(001) heterostructures, we demonstrate that a coherent GHz ac spin current pumped by the permalloy (Py) ferromagnetic resonance (FMR) can transmit coherently across an antiferromagnetic CoO insulating layer to drive a coherent spin precession of the FM Fe75Co25 layer. Further measurement results favor thermal magnons rather than evanescent spin waves as the mediator of the coherent ac spin current in CoO.

physics.app-ph↗

arXiv2019

Emergent magnetic state in (111)-oriented quasi-two-dimensional spinel oxides

We report on the emergent magnetic state of (111)-oriented CoCr2O4 ultrathin films sandwiched by Al2O3 in the quantum confined geometry. At the two-dimensional crossover, polarized neutron reflectometry reveals an anomalous enhancement of the total magnetization compared to the bulk value. Synchrotron x-ray magnetic circular dichroism (XMCD) demonstrates the appearance of long-range ferromagnetic ordering of spins on both Co and Cr sublattices. Brillouin function analyses further corroborates that the observed phenomena are due to the strongly altered magnetic frustration, manifested by the onset of a Yafet-Kittel type ordering as the new ground state in the ultrathin limit, which is unattainable in the bulk.

cond-mat.str-el↗

arXiv2019

Interface-engineered hole doping in Sr2IrO4/LaNiO3 heterostructure

The relativistic Mott insulator Sr2IrO4 driven by large spin-orbit interaction is known for the Jeff = 1/2 antiferromagnetic state which closely resembles the electronic structure of parent compounds of superconducting cuprates. Here, we report the realization of hole-doped Sr2IrO4 by means of interfacial charge transfer in Sr2IrO4/LaNiO3 heterostructures. X-ray photoelectron spectroscopy on Ir 4f edge along with the X-ray absorption spectroscopy at Ni L2 edge confirmed that 5d electrons from Ir sites are transferred onto Ni sites, leading to markedly electronic reconstruction at the interface. Although the Sr2IrO4/LaNiO3 heterostructure remains non-metallic, we reveal that the transport behavior is no longer described by the Mott variable range hopping mode, but by the Efros-Shklovskii model. These findings highlight a powerful utility of interfaces to realize emerging electronic states of the Ruddlesden-Popper phases of Ir-based oxides.

cond-mat.str-el↗

arXiv2018

The interfacial spin modulation of graphene on Fe(111)

When Fe, which is a typical ferromagnet using d- or f-orbital states, is combined with 2D materials such as graphene, it offers many opportunities for spintronics. The origin of 2D magnetism is from magnetic insulating behaviors, which could result in magnetic excitations and also proximity effects. However, the phenomena were only observed at extremely low temperatures. Fe and graphene interfaces could control spin structures in which they show a unique atomic spin modulation and magnetic coupling through the interface. Another reason for covering graphene on Fe is to prevent oxidation under ambient conditions. We investigated the engineering of spin configurations by growing monolayer graphene on an Fe(111) single crystal surface and observed the presence of sharply branched, 3D tree-like domain structures. Magnetization by a sweeping magnetic field (m-H) revealed that the interface showed canted magnetization in the in-plane (IP) orientation. Moreover, graphene could completely prevent the oxidation of the Fe surface. The results indicate possible control of the spin structures at the atomic scale and the interface phenomena in the 2D structure. The study introduces a new approach for room temperature 2D magnetism.

cond-mat.mes-hall↗

arXiv2018

Decoupling carrier concentration and electron-phonon coupling in oxide heterostructures observed with resonant inelastic x-ray scattering

We report the observation of multiple phonon satellite features in ultra thin superlattices of form $n$SrIrO$_3$/$m$SrTiO$_3$ using resonant inelastic x-ray scattering. As the values of $n$ and $m$ vary the energy loss spectra show a systematic evolution in the relative intensity of the phonon satellites. Using a closed-form solution for the cross section, we extract the variation in the electron-phonon coupling strength as a function of $n$ and $m$. Combined with the negligible carrier doping into the SrTiO$_3$ layers, these results indicate that tuning of the electron-phonon coupling can be effectively decoupled from doping. This work showcases both a feasible method to extract the electron-phonon coupling in superlattices and unveils a potential route for tuning this coupling which is often associated with superconductivity in SrTiO$_3$-based systems.

cond-mat.str-el↗

arXiv2018

Nature of the metal-insulator transition in few-unit-cell-thick LaNiO3 films

The nature of the metal insulator transition in thin films and superlattices of LaNiO3 with only few unit cells in thickness remains elusive despite tremendous effort. Quantum confinement and epitaxial strain have been evoked as the mechanisms, although other factors such as growth-induced disorder, cation non-stoichiometry, oxygen vacancies, and substrate-film interface quality may also affect the observable properties in the ultrathin films. Here we report results obtained for near-ideal LaNiO3 films with different thicknesses and terminations grown by atomic layer-by-layer laser molecular beam epitaxy on LaAlO3 substrates. We find that the room-temperature metallic behavior persists until the film thickness is reduced to an unprecedentedly small 1.5 unit cells (NiO2 termination). Electronic structure measurements using x-ray absorption spectroscopy and first-principles calculation suggest that oxygen vacancies existing in the films also contribute to the metal insulator transition.

cond-mat.mtrl-sci↗

arXiv2018

Resolving interfacial charge transfer in titanate superlattices using resonant X-ray reflectometry

Charge transfer in oxide heterostructures can be tuned to promote emergent interfacial states, and accordingly, has been the subject of intense study in recent years. However, accessing the physics at these interfaces, which are often buried deep below the sample surface, remains difficult. Addressing this challenge requires techniques capable of measuring the local electronic structure with high-resolution depth dependence. Here, we have used linearly-polarized resonant X-ray reflectometry (RXR) as a means to visualize charge transfer in oxide superlattices with atomic layer precision. From our RXR measurements, we extract valence depth profiles of SmTiO$_3$ (SmTO)/SrTiO$_3$ (STO) heterostructures with STO quantum wells varying in thickness from 5 SrO planes down to a single, atomically thin SrO plane. At the polar-nonpolar SmTO/STO interface, an electrostatic discontinuity leads to approximately half an electron per areal unit cell transferred from the interfacial SmO layer into the neighboring STO quantum well. We observe this charge transfer as a suppression of the t$_{2g}$ absorption peaks that minimizes contrast with the neighboring SmTO layers at those energies and leads to a pronounced absence of superlattice peaks in the reflectivity data. Our results demonstrate the sensitivity of RXR to electronic reconstruction at the atomic scale, and establish RXR as a powerful means of characterizing charge transfer at buried oxide interfaces.

cond-mat.str-el↗

arXiv2018

Anomalous orbital structure in two-dimensional titanium dichalcogenides

Generally, lattice distortions play a key role in determining the ground states of materials. Although it is well known that trigonal distortions are generic to most two-dimensional transition metal dichalcogenides, the impact of this structural distortion on the electronic structure has not been understood conclusively. Here, by using a combination of polarization dependent X-ray absorption spectroscopy (XAS), X-ray photoelectron spectroscopy (XPS) and atomic multiplet cluster calculations, we have investigated the electronic structure of titanium dichalcogenides TiX2 (X=S, Se, Te), where the magnitude of the trigonal distortion increase monotonically from S to Se and Te. Our results reveal the presence of an anomalous and large crystal filed splitting. This unusual kind of crystal field splitting is likely responsible for the unconventional electronic structure of TiX2 compounds. Our results also indicate the drawback of the distorted crystal field picture in explaining the observed electronic ground state of these materials and emphasize the key importance of metal-ligand hybridization and electronic correlation in defining the electronic structures near Fermi energy.

cond-mat.mtrl-sci↗

arXiv2018

Electronic properties of ultra-thin YCrO3 films

We report on the heteroepitaxial stabilization of YCrO3 ultra-thin films on LSAT (001) substrate. Using a combination of resonant X-ray absorption spectroscopy (XAS) and atomic multiplet cluster calculation, the electronic structure of YCrO3 thin film was investigated. Polarization dependent Cr L3,2 edge XAS measurement reveal the presence of an anomalous orbital polarization uncharacteristic of a 3d3 electronic system. Atomic multiplet calculations demonstrate the critical importance of charge transfer energy, Coulomb correlation strength and hopping interaction in stabilizing this unusual orbital polarized state likely connected to the bulk multiferroicity.

cond-mat.mtrl-sci↗

arXiv2018

Artificial two-dimensional polar metal at room temperature

Polar metals, commonly defined by the coexistence of polar crystal structure and metallicity, are thought to be scarce because the long-range electrostatic fields favoring the polar structure are expected to be fully screened by the conduction electrons of a metal. Moreover, reducing from three to two dimensions, it remains an open question whether a polar metal can exist. Here we report on the realization of a room temperature two-dimensional polar metal of the B-site type in tri-color (tri-layer) superlattices BaTiO$_3$/SrTiO$_3$/LaTiO$_3$. A combination of atomic resolution scanning transmission electron microscopy with electron energy loss spectroscopy, optical second harmonic generation, electrical transport, and first-principles calculations have revealed the microscopic mechanisms of periodic electric polarization, charge distribution, and orbital symmetry. Our results provide a route to creating all-oxide artificial non-centrosymmetric quasi-two-dimensional metals with exotic quantum states including coexisting ferroelectric, ferromagnetic, and superconducting phases.

cond-mat.mtrl-sci↗

arXiv2017

Synthesis and electronic properties of Ruddlesden-Popper strontium iridate epitaxial thin films stabilized by control of growth kinetics

We report on the selective fabrication of high-quality Sr$_2$IrO$_4$ and SrIrO$_3$ epitaxial thin films from a single polycrystalline Sr$_2$IrO$_4$ target by pulsed laser deposition. Using a combination of X-ray diffraction and photoemission spectroscopy characterizations, we discover that within a relatively narrow range of substrate temperature, the oxygen partial pressure plays a critical role in the cation stoichiometric ratio of the films, and triggers the stabilization of different Ruddlesden-Popper (RP) phases. Resonant X-ray absorption spectroscopy measurements taken at the Ir $L$-edge and the O $K$-edge demonstrate the presence of strong spin-orbit coupling, and reveal the electronic and orbital structures of both compounds. These results suggest that in addition to the conventional thermodynamics consideration, higher members of the Sr$_{n+1}$Ir$_n$O$_{3n+1}$ series can possibly be achieved by kinetic control away from the thermodynamic limit. These findings offer a new approach to the synthesis of ultra-thin films of the RP series of iridates and can be extended to other complex oxides with layered structure.

cond-mat.str-el↗

arXiv2017

Electron Accumulation and Emergent Magnetism in LaMnO3/SrTiO3 Heterostructures

Emergent phenomena at polar-nonpolar oxide interfaces have been studied intensely in pursuit of next-generation oxide electronics and spintronics. Here we report the disentanglement of critical thicknesses for electron reconstruction and the emergence of ferromagnetism in polar-mismatched LaMnO3/SrTiO3 (001) heterostructures. Using a combination of element-specific X-ray absorption spectroscopy and dichroism, and first-principles calculations, interfacial electron accumulation and ferromagnetism have been observed within the polar, antiferromagnetic insulator LaMnO3. Our results show that the critical thickness for the onset of electron accumulation is as thin as 2 unit cells (UC), significantly thinner than the observed critical thickness for ferromagnetism of 5 UC. The absence of ferromagnetism below 5 UC is likely induced by electron over-accumulation. In turn, by controlling the doping of the LaMnO3, we are able to neutralize the excessive electrons from the polar mismatch in ultrathin LaMnO3 films and thus enable ferromagnetism in films as thin as 3 UC, extending the limits of our ability to synthesize and tailor emergent phenomena at interfaces and demonstrating manipulation of the electronic and magnetic structures of materials at the shortest length scales.

cond-mat.mtrl-sci↗

arXiv2016

Anomalous orbital structure in a spinel-perovskite interface $γ$-Al$_2$O$_3$/SrTiO$_3$

In all archetypical reported (001)-oriented perovskite heterostructures, it has been deduced that the preferential occupation of two-dimensional electron gases is in-plane $d_\textrm{xy}$ state. In sharp contrast to this, the investigated electronic structure of a spinel-perovskite heterostructure $γ$-Al$_2$O$_3$/SrTiO$_3$ by resonant soft X-ray linear dichroism, demonstrates that the preferential occupation is out-of-plane $d_\textrm{xz}$/$d_\textrm{yz}$ states for interfacial electrons. Moreover, the impact of strain further corroborates that this anomalous orbital structure can be linked to the altered crystal field at the interface and symmetry breaking of the interfacial structural units. Our findings provide another interesting route to engineer emergent quantum states with deterministic orbital symmetry.

cond-mat.mtrl-sci↗

arXiv2016

Direct detection of pure spin-current by x-ray pump-probe measurements

By synchronizing a microwave waveform with the synchrotron x-ray pulses, we use the ferromagnetic resonance (FMR) of the Py (Ni81Fe19) layer in a Py/Cu/Cu75Mn25/Cu/Co multilayer to pump a pure spin current into the Cu75Mn25 spacer layer, and then directly probe the spin current in the Cu75Mn25 layer by a time-resolved x-ray magnetic circular dichroism (XMCD). This element-specific pump-probe measurement unambiguously identifies the AC spin current in the Cu75Mn25 layer. In addition, phase resolved x-ray measurements reveal a characteristic bipolar phase behavior of the Co spins that is a fingerprint of spin-current driven spin precession.

cond-mat.mtrl-sci↗

arXiv2016

Measurement of collective excitations in VO$_2$ by resonant inelastic X-ray scattering

Vanadium dioxide is of broad interest as a spin-1/2 electron system that realizes a metal-insulator transition near room temperature, due to a combination of strongly correlated and itinerant electron physics. Here, resonant inelastic X-ray scattering is used to measure the excitation spectrum of charge, spin, and lattice degrees of freedom at the vanadium L-edge under different polarization and temperature conditions. These spectra reveal the evolution of energetics across the metal-insulator transition, including the low temperature appearance of a strong candidate for the singlet-triplet excitation of a vanadium dimer.

cond-mat.str-el↗