The spin polarization of palladium on magneto-electric Cr2O3.

While induced spin polarization of a palladium (Pd) overlayer on antiferromagnetic and magneto-electric Cr2O3(0001) is possible because of the boundary polarization at the Cr2O3(0001), in the single domain state, the Pd thin film appears to be ferromagnetic on its own, likely as a result of strain. In the conduction band, we find the experimental evidence of ferromagnetic spin polarized in Pd thin films on a Cr2O3(0001) single crystal, especially in the thin limit, Pd thickness of around 1-4 nm. Indeed there is significant spin polarization in 10 Å thick Pd films on Cr2O3(0001) at 310 K, i.e. above the Néel temperature of bulk Cr2O3. While Cr2O3(0001) has surface moments that tend to align along the surface normal, for Pd on Cr2O3, the spin polarization contains an in-plane component. Strain in the Pd adlayer on Cr2O3(0001) appears correlated to the spin polarization measured in spin polarized inverse photoemission spectroscopy. Further evidence for magnetization of Pd on Cr2O3is provided by measurement of the exchange bias fields in Cr2O3/Pd(buffer)/[Co/Pd]nexchange bias systems. The magnitude of the exchange bias field is, over a wide temperature range, virtually unaffected by the Pd thickness variation between 1 and 2 nm.

Correction: Nanoscale imaging of antiferromagnetic domains in epitaxial films of Cr2O3 via scanning diamond magnetic probe microscopy.

[This corrects the article DOI: 10.1039/D2RA06440E.].

Molecular transistors as substitutes for quantum information applications.

Applications of quantum information science (QIS) generally rely on the generation and manipulation of qubits. Still, there are ways to envision a device with a continuous readout, but without the entangled states. This concise perspective includes a discussion on an alternative to the qubit, namely the solid-state version of the Mach-Zehnder interferometer, in which the local moments and spin polarization replace light polarization. In this context, we provide some insights into the mathematics that dictates the fundamental working principles of quantum information processes that involve molecular systems with large magnetic anisotropy. Transistors based on such systems lead to the possibility of fabricating logic gates that do not require entangled states. Furthermore, some novel approaches, worthy of some consideration, exist to address the issues pertaining to the scalability of quantum devices, but face the challenge of finding the suitable materials for desired functionality that resemble what is sought from QIS devices.

Graphene on Chromia: A System for Beyond-Room-Temperature Spintronics.

Evidence of robust spin-dependent transport in monolayer graphene, deposited on the (0001) surface of the antiferromagnetic (AFM)/magneto-electric oxide chromia (Cr2 O3 ), is provided. Measurements performed in the non-local spin-Hall geometry reveal a robust signal that is present at zero external magnetic field and which is significantly larger than any possible ohmic contribution. The spin-related signal persists well beyond the Néel temperature (≈307 K) that defines the transition between the AFM and paramagnetic states, remaining visible at the highest studied temperature of close to 450 K. This robust character is consistent with prior theoretical studies of the graphene/Cr2 O3 system, predicting that the lifting of sub-lattice symmetry in the graphene shall induce an effective spin-orbit term of ≈40 meV. Overall, the results indicate that graphene-on-chromia heterostructures are a highly promising framework for the implementation of spintronic devices, capable of operation well beyond room temperature.

Nanoscale imaging of antiferromagnetic domains in epitaxial films of Cr2O3 via scanning diamond magnetic probe microscopy.

We report direct imaging of boundary magnetization associated with antiferromagnetic domains in magnetoelectric epitaxial Cr2O3 thin films using diamond nitrogen vacancy microscopy. We found a correlation between magnetic domain size and structural grain size which we associate with the domain formation process. We performed field cooling, i.e., cooling from above to below the Néel temperature in the presence of a magnetic field, which resulted in the selection of one of the two otherwise degenerate 180° domains. Lifting of such a degeneracy is achievable with a magnetic field alone due to the Zeeman energy of a weak parasitic magnetic moment in Cr2O3 films that originates from defects and the imbalance of the boundary magnetization of opposing interfaces. This boundary magnetization couples to the antiferromagnetic order parameter enabling selection of its orientation. Nanostructuring the Cr2O3 film with mesa structures revealed reversible edge magnetic states with the direction of magnetic field during field cooling.

Voltage controlled Néel vector rotation in zero magnetic field.

Multi-functional thin films of boron (B) doped Cr2O3 exhibit voltage-controlled and nonvolatile Néel vector reorientation in the absence of an applied magnetic field, H. Toggling of antiferromagnetic states is demonstrated in prototype device structures at CMOS compatible temperatures between 300 and 400 K. The boundary magnetization associated with the Néel vector orientation serves as state variable which is read via magnetoresistive detection in a Pt Hall bar adjacent to the B:Cr2O3 film. Switching of the Hall voltage between zero and non-zero values implies Néel vector rotation by 90 degrees. Combined magnetometry, spin resolved inverse photoemission, electric transport and scanning probe microscopy measurements reveal B-dependent TN and resistivity enhancement, spin-canting, anisotropy reduction, dynamic polarization hysteresis and gate voltage dependent orientation of boundary magnetization. The combined effect enables H = 0, voltage controlled, nonvolatile Néel vector rotation at high-temperature. Theoretical modeling estimates switching speeds of about 100 ps making B:Cr2O3 a promising multifunctional single-phase material for energy efficient nonvolatile CMOS compatible memory applications.

Observation of Quantum Anomalous Hall Effect and Exchange Interaction in Topological Insulator/Antiferromagnet Heterostructure.

Integration of a quantum anomalous Hall insulator with a magnetically ordered material provides an additional degree of freedom through which the resulting exotic quantum states can be controlled. Here, an experimental observation is reported of the quantum anomalous Hall effect in a magnetically-doped topological insulator grown on the antiferromagnetic insulator Cr2 O3 . The exchange coupling between the two materials is investigated using field-cooling-dependent magnetometry and polarized neutron reflectometry. Both techniques reveal strong interfacial interaction between the antiferromagnetic order of the Cr2 O3 and the magnetic topological insulator, manifested as an exchange bias when the sample is field-cooled under an out-of-plane magnetic field, and an exchange spring-like magnetic depth profile when the system is magnetized within the film plane. These results identify antiferromagnetic insulators as suitable candidates for the manipulation of magnetic and topological order in topological insulator films.

Electromagnon excitation in cupric oxide measured by Fabry-Pérot enhanced terahertz Mueller matrix ellipsometry.

Here we present the use of Fabry-Pérot enhanced terahertz (THz) Mueller matrix ellipsometry to measure an electromagnon excitation in monoclinic cupric oxide (CuO). As a magnetically induced ferroelectric multiferroic, CuO exhibits coupling between electric and magnetic order. This gives rise to special quasiparticle excitations at THz frequencies called electromagnons. In order to measure the electromagnons in CuO, we exploit single-crystal CuO as a THz Fabry-Pérot cavity to resonantly enhance the excitation's signature. This enhancement technique enables the complex index of refraction to be extracted. We observe a peak in the absorption coefficient near 0.705 THz and 215 K, which corresponds to the electromagnon excitation. This absorption peak is observed along only one major polarizability axis in the monoclinic a-c plane. We show the excitation can be represented using the Lorentz oscillator model, and discuss how these Lorentz parameters evolve with temperature. Our findings are in excellent agreement with previous characterizations by THz time-domain spectroscopy (THz-TDS), which demonstrates the validity of this enhancement technique.

Elastic properties of superconductors and materials with weakly correlated spins.

It is shown that in the ergodic regime, the temperature dependence of Young's modulus is solely determined by the magnetic properties of a material. For the large class of materials with paramagnetic or diamagnetic response, simple functional forms of the temperature derivative of Young's modulus are derived and compared with experimental data and empirical results. Superconducting materials in the Meissner phase are ideal diamagnets. As such, they display remarkable elastic properties. Constant diamagnetic susceptibility gives rise to a temperature independent elastic modulus for ceramic and single crystalline superconductors alike. The thermodynamic approach established in this report, paves the way to tailor elastic material parameters through the design of magnetic properties.

Low temperature growth of cobalt on Cr2O3(0 0 0 1).

The thickness and temperature dependence of in situ grown cobalt thin films on Cr2O3(0 0 0 1) single crystalline substrate has been studied by low energy electron microscopy (LEEM). The LEEM images indicate that growth of thin Co films (⩽5 monolayers) on chromia at 100 K tends to be continuous and flat with suppressed island growth compared to films grown on chromia at room temperature and above (to ~440 K). Low energy electron diffraction indicates that disorder builds and crystallinity of the cobalt thin film decreases with increased film thickness. Compared with cobalt thin films on Al2O3(0 0 0 1) single crystalline substrate, cobalt thin films on Cr2O3(0 0 0 1) show larger magnetic contrast in magnetic force microscopy indicating enhancement of perpendicular anisotropy induced by Cr2O3.

The surface stability of Cr2O3(0 0 0 1).

The surface of chromia (Cr2O3) has a surface electronic structure distinct from the bulk and a packing density distinct from the bulk. More than a demarcation between the solid and the vacuum, the surface differs from the bulk of chromia, not just because of a partial occupancy of chromium sites, but also because of an increased number of unoccupied surface oxygen sites (vacancy sites), evident in angle-resolved core level photoemission. In spite of the structural differences that exist at the surface, there is, as yet, no evidence that these complications affect the surface Debye temperature beyond the most simple of assumptions regarding the lower coordination of the surface. Using low-energy electron diffraction (LEED), the effective surface Debye temperature (∼490 K) is found to be lower than the bulk (∼645 K) Debye temperature of Cr2O3(0 0 0 1). This surface effective Debye temperature, indicative of vibrations along the surface normal, uncorrected for anharmonic effects, has a value reduced from the effective bulk Debye temperature yet close to the value √2 expected from a simple mean field argument.

Magnetoelectric Fe2TeO6 thin films.

We demonstrate that Fe2TeO6 is a magnetoelectric antiferromagnet with voltage-controllable boundary magnetization. This provides experimental evidence of the theoretical prediction that boundary magnetization is a universal property of magnetoelectric antiferromagnets including boundary magnetization at a surface orthogonal to the polar direction. Highly (110) textured Fe2TeO6 thin films were grown by pulsed laser deposition, terminating in Te-O at the (110) surface due to a surface reconstruction. Magnetic dc susceptibility measurements of both Fe2TeO6 powder and thin film samples confirm antiferromagnetic long-range order. Finally, measurements of x-ray magnetic circular dichroism combined with photoemission electron microscopy (XMCD-PEEM) provide a lower bound to the spin and angular magnetic moment of the surface Fe ions.

Graphene mediated domain formation in exchange coupled graphene/Co3O4(111)/Co(0001) trilayers.

Graphene grown directly on Co3O4(111)/Co(0001) by molecular beam epitaxy exhibits extrinsic p-type doping, as demonstrated by photoemission and conductivity measurements. Trilayer heterostructures of graphene/Co3O4(111)/Co(0001) reveal an unconventional magneto-optical Kerr hysteresis with vanishing remanence for temperatures up to 400 K. Magnetic force microscopy measurements demonstrate that the vanishing remanence is due to a complex domain state, indicating substrate-induced graphene spin polarization. The domain formation of the Co magnetization is in strong contrast to the magnetic behavior of Co in Co/Co3O4 bilayers. This suggests that the Co3O4 interlayer mediates the variable Co magnetization and induced graphene spin polarization, with possible retroaction of graphene on the Co film.

Asymmetric magnetoresistance in an exchange bias Co/CoO bilayer.

Magnetoresistance (MR) measurements are carried out on a Co(8 nm)/CoO(3.5 nm) bilayer in the exchange bias (EB) state prepared by molecular beam epitaxy. With the applied magnetic field parallel to the current, the EB MR curves show an asymmetric behavior about the minimum, in contrast to the symmetric one for non-EB systems. We generalize a well-known analytical expression used for the field dependence of the MR of paramagnets. Our generalization incorporates coercivity and EB in a new phenomenological MR expression. Excellent fits of the latter to the experimental MR data are achieved, showing the way to use MR techniques for the quantitative characterization of EB systems. Furthermore, the temperature dependence of the EB field obtained from MR loops can be described with a power law, which yields a value of 96.6 K for the EB blocking temperature, which is significantly below the Néel temperature of 293 K for bulk CoO.

When measured spin polarization is not spin polarization.

Spin polarization is an unusually ambiguous scientific idiom and, as such, is rarely well defined. A given experimental methodology may allow one to quantify a spin polarization but only in its particular context. As one might expect, these ambiguities sometimes give rise to inappropriate interpretations when comparing the spin polarizations determined through different methods. The spin polarization of CrO(2) and Cr(2)O(3) illustrate some of the complications which hinders comparisons of spin polarization values.

Imaging and control of surface magnetization domains in a magnetoelectric antiferromagnet.

We report the direct observation of surface magnetization domains of the magnetoelectric Cr(2)O(3) using photoemission electron microscopy with magnetic circular dichroism contrast and magnetic force microscopy. The domain pattern is strongly affected by the applied electric field conditions. Zero-field cooling results in an equal representation of the two domain types, while electric-field cooling selects one dominant domain type. These observations confirm the existence of surface magnetization, required by symmetry in magnetoelectric antiferromagnets.

Robust isothermal electric control of exchange bias at room temperature.

Voltage-controlled spin electronics is crucial for continued progress in information technology. It aims at reduced power consumption, increased integration density and enhanced functionality where non-volatile memory is combined with high-speed logical processing. Promising spintronic device concepts use the electric control of interface and surface magnetization. From the combination of magnetometry, spin-polarized photoemission spectroscopy, symmetry arguments and first-principles calculations, we show that the (0001) surface of magnetoelectric Cr(2)O(3) has a roughness-insensitive, electrically switchable magnetization. Using a ferromagnetic Pd/Co multilayer deposited on the (0001) surface of a Cr(2)O(3) single crystal, we achieve reversible, room-temperature isothermal switching of the exchange-bias field between positive and negative values by reversing the electric field while maintaining a permanent magnetic field. This effect reflects the switching of the bulk antiferromagnetic domain state and the interface magnetization coupled to it. The switchable exchange bias sets in exactly at the bulk Néel temperature.

Magnetoelectric switching of exchange bias.

The perpendicular exchange bias field, H(EB), of the magnetoelectric heterostructure Cr2O3(111)/(Co/Pt)(3) changes sign after field cooling to below the Néel temperature of Cr2O3 in either parallel or antiparallel axial magnetic and electric freezing fields. The switching of H(EB) is explained by magnetoelectrically induced antiferromagnetic single domains which extend to the interface, where the direction of their end spins controls the sign of H(EB). Novel applications in magnetoelectronic devices seem possible.