Efficient ultrafast field-driven spin current generation for spintronic terahertz frequency conversion.

Efficient generation and control of spin currents launched by terahertz (THz) radiation with subsequent ultrafast spin-to-charge conversion is the current challenge for the next generation of high-speed communication and data processing units. Here, we demonstrate that THz light can efficiently drive coherent angular momentum transfer in nanometer-thick ferromagnet/heavy-metal heterostructures. This process is non-resonant and does neither require external magnetic fields nor cryogenics. The efficiency of this process is more than one order of magnitude higher as compared to the recently observed THz-induced spin pumping in MnF2 antiferromagnet. The coherently driven spin currents originate from the ultrafast spin Seebeck effect, caused by a THz-induced temperature imbalance in electronic and magnonic temperatures and fast relaxation of the electron-phonon system. Owing to the fact that the electron-phonon relaxation time is comparable with the period of a THz wave, the induced spin current results in THz second harmonic generation and THz optical rectification, providing a spintronic basis for THz frequency mixing and rectifying components.

Tailoring Exchange-Dominated Synthetic Layered Antiferromagnets: From Collective Magnetic Reversal to Exchange Bias.

Not only since the progressive reduction of structure sizes in modern micro- and nanotechnology, surface and interface effects have played an ever-increasing role and nowadays often dominate the behavior of entire systems. Therefore, understanding the nature of surface and interface effects and being able to fully control them is of fundamental importance, in particular in modern thin-film technology. In this study, it is revealed how Co/Pt multilayer-based synthetic antiferromagnets (SAFs) with perpendicular magnetic anisotropy in the regime of dominating antiferromagnetic interlayer exchange can be employed to control the collective magnetic reversal via systematically altering surface and interface effects. The specifically designed samples and experiments highlight the superior tunability of synthetic systems as compared to their intrinsic stoichiometric counterparts, where the antiferromagnetism is directly tied to the indivisible discrete atomic nature and crystal structure of the materials. Thus, it is demonstrated that in SAFs, it becomes possible to energetically heal the broken magnetic symmetry at the surface, thereby enabling either on demand suppression or controlled enhancement of respective surface and interface effects, as demonstrated here in this study for the surface spin-flop and the exchange bias effect.

Role of vibrational properties and electron-phonon coupling on thermal transport across metal-dielectric interfaces with ultrathin metallic interlayers.

We systematically analyze the influence of 5 nm thick metal interlayers inserted at the interface of several sets of different metal-dielectric systems to determine the parameters that most influence interface transport. Our results show that despite the similar Debye temperatures of Al2O3and AlN substrates, the thermal boundary conductance measured for the Au/Al2O3system with Ni and Cr interlayers is ∼2× and >3× higher than the corresponding Au/AlN system, respectively. We also show that for crystalline SiO2(quartz) and Al2O3substrates having highly dissimilar Debye temperature, the measured thermal boundary conductance between Al/Al2O3and Al/SiO2are similar in the presence of Ni and Cr interlayers. We suggest that comparing the maximum phonon frequency of the acoustic branches is a better parameter than the Debye temperature to predict the change in the thermal boundary conductance. We show that the electron-phonon coupling of the metallic interlayers also alters the heat transport pathways in a metal-dielectric system in a nontrivial way. Typically, interlayers with large electron-phonon coupling strength can increase the thermal boundary conductance by dragging electrons and phonons into equilibrium quickly. However, our results show that a Ta interlayer, having a high electron-phonon coupling, shows a low thermal boundary conductance due to the poor phonon frequency overlap with the top Al layer. Our experimental work can be interpreted in the context of diffuse mismatch theory and can guide the selection of materials for thermal interface engineering.

Resonance behavior of embedded and freestanding microscale ferromagnets.

The ferromagnetic resonance of a disordered A2 Fe60Al40 ferromagnetic stripe, of dimensions 5 µm × 1 µm × 32 nm, has been observed in two vastly differing surroundings: in the first case, the ferromagnetic region was surrounded by ordered B2 Fe60Al40, and in the second case it was free standing, adhering only to the oxide substrate. The embedded ferromagnet possesses a periodic magnetic domain structure, which transforms to a single domain structure in the freestanding case. The two cases differ in their dynamic response, for instance, the resonance field for the uniform (k = 0) mode at ~ 14 GHz excitation displays a shift from 209 to 194 mT, respectively for the embedded and freestanding cases, with the external magnetic field applied along the long axis. The resonant behavior of a microscopic ferromagnet can thus be finely tailored via control of its near-interfacial surrounding.

Cooperative Effect of Electron Spin Polarization in Chiral Molecules Studied with Non-Spin-Polarized Scanning Tunneling Microscopy.

Polyalanine molecules (PA) with an α-helix conformation have recently attracted a great deal of interest, as the propagation of electrons through the chiral backbone structure comes along with spin polarization of the transmitted electrons. By means of scanning tunneling microscopy and spectroscopy under ambient conditions, PA molecules adsorbed on surfaces of epitaxial magnetic Al2O3/Pt/Au/Co/Au nanostructures with perpendicular anisotropy were studied. Thereby, a correlation between the PA molecules ordering at the surface with the electron tunneling across this hybrid system as a function of the substrate magnetization orientation as well as the coverage density and helicity of the PA molecules was observed. The highest spin polarization values, P, were found for well-ordered self-assembled monolayers and with a defined chemical coupling of the molecules to the magnetic substrate surface, showing that the current-induced spin selectivity is a cooperative effect. Thereby, P deduced from the electron transmission along unoccupied molecular orbitals of the chiral molecules is larger as compared to values derived from the occupied molecular orbitals. Apparently, the larger orbital overlap results in a higher electron mobility, yielding a higher P value. By switching the magnetization direction of the Co layer, it was demonstrated that the non-spin-polarized STM can be used to study chiral molecules with a submolecular resolution, to detect properties of buried magnetic layers and to detect the spin polarization of the molecules from the change in the magnetoresistance of such hybrid structures.

Collaborative Filler Network for Enhancing the Performance of BaTiO3/PDMS Flexible Piezoelectric Polymer Composite Nanogenerators.

Wearable sensors are gaining attention in human health monitoring applications, even if their usability is limited due to battery need. Flexible nanogenerators (NGs) converting biomechanical energy into electrical energy offer an interesting solution, as they can supply the sensors or extend the battery lifetime. Herein, flexible generators based on lead-free barium titanate (BaTiO3) and a polydimethylsiloxane (PDMS) polymer have been developed. A comparative study was performed to investigate the impact of multiwalled carbon nanotubes (MWCNTs) via structural, morphological, electrical, and electromechanical measurements. This study demonstrated that MWCNTs boosts the performance of the NG at the percolation threshold. This enhancement is attributed to the enhanced conductivity that promotes charge transfer and enhanced mechanical property and piezoceramics particles distribution. The nanogenerator delivers a maximum open-circuit voltage (VOC) up to 1.5 V and output power of 40 nW, which is two times higher than NG without MWCNTs. Additionally, the performance can be tuned by controlling the composite thickness and the applied frequency. Thicker NG shows a better performance, which enlarges their potential use for harvesting biomechanical energy efficiently up to 11.22 V under palm striking. The voltage output dependency on temperature was also investigated. The results show that the output voltage changes enormously with the temperature.

Magnetic Configuration Driven Femtosecond Spin Dynamics in Synthetic Antiferromagnets.

Ultrafast demagnetization in diverse materials has sparked immense research activities due to its captivating richness and contested underlying mechanisms. Among these, the two most celebrated mechanisms have been the spin-flip scattering (SFS) and spin transport (ST) of optically excited carriers. In this work, we have investigated femtosecond laser-induced ultrafast demagnetization in perpendicular magnetic anisotropy-based synthetic antiferromagnets (p-SAFs) where [Co/Pt]n-1/Co multilayer blocks are separated by Ru or Ir spacers. Our investigation conclusively shows that the ST of optically excited carriers can have a significant contribution to the ultrafast demagnetization in addition to SFS processes. Moreover, we have also achieved an active control over the individual mechanisms by specially designing the SAF samples and altering the external magnetic field and excitation fluence. Our study provides a vital understanding of the underlying mechanism of ultrafast demagnetization in synthetic antiferromagnets, which will be crucial in future research and applications of antiferromagnetic spintronics.

Highly Tunable Magnetic and Magnetotransport Properties of Exchange Coupled Ferromagnet/Antiferromagnet-Based Heterostructures.

Antiferromagnets (AFMs) with zero net magnetization are proposed as active elements in future spintronic devices. Depending on the critical film thickness and measurement temperature, bimetallic Mn-based alloys and transition-metal oxide-based AFMs can host various coexisting ordered, disordered, and frustrated AFM phases. Such coexisting phases in the exchange coupled ferromagnetic (FM)/AFM-based heterostructures can result in unusual magnetic and magnetotransport phenomena. Here, we integrate chemically disordered AFM γ-IrMn3 thin films with coexisting AFM phases into complex exchange coupled MgO(001)/γ-Ni3Fe/γ-IrMn3/γ-Ni3Fe/CoO heterostructures and study the structural, magnetic, and magnetotransport properties in various magnetic field cooling states. In particular, we unveil the impact of rotating the relative orientation of the thermally disordered and reversible AFM moments with respect to the irreversible AFM moments on the magnetic and magnetotransport properties of the exchange coupled heterostructures. We further reveal that the persistence of thermally disordered and reversible AFM moments is crucial for achieving highly tunable magnetic properties and multilevel magnetoresistance states. We anticipate that the presented approach and the heterostructure architecture can be utilized in future spintronic devices to manipulate the thermally disordered and reversible AFM moments at the nanoscale.

Laser induced crystallization of Co-Fe-B films.

Local crystallization of ferromagnetic layers is crucial in the successful realization of miniaturized tunneling magnetoresistance (TMR) devices. In the case of Co-Fe-B TMR devices, used most successfully so far in applications and devices, Co-Fe-B layers are initially deposited in an amorphous state and annealed post-deposition to induce crystallization in Co-Fe, thereby increasing the device performance. In this work, first direct proof of locally triggered crystallization of 10 nm thick Co-Fe-B films by laser irradiation is provided by means of X-ray diffraction (XRD) using synchrotron radiation. A comparison with furnace annealing is performed for benchmarking purposes, covering different annealing parameters, including temperature and duration in the case of furnace annealing, as well as laser intensity and scanning speed for the laser annealing. Films of Co-Fe-B with different stoichiometry sandwiched between a Ru and a Ta or MgO layer were systematically assessed by XRD and SQUID magnetometry in order to elucidate the crystallization mechanisms. The transformation of Co-Fe-B films from amorphous to crystalline is revealed by the presence of pronounced CoFe(110) and/or CoFe(200) reflexes in the XRD θ-2θ scans, depending on the capping layer. For a certain window of parameters, comparable crystallization yields are obtained with furnace and laser annealing. Samples with an MgO capping layer required a slightly lower laser intensity to achieve equivalent Co-Fe crystallization yields, highlighting the potential of laser annealing to locally enhance the TMR ratio.

Ion-Irradiation-Induced Cobalt/Cobalt Oxide Heterostructures: Printing 3D Interfaces.

Interfaces separating ferromagnetic (FM) layers from non-ferromagnetic layers offer unique properties due to spin-orbit coupling and symmetry breaking, yielding effects such as exchange bias, perpendicular magnetic anisotropy, spin-pumping, spin-transfer torques, and conversion between charge and spin currents and vice versa. These interfacial phenomena play crucial roles in magnetic data storage and transfer applications, which require the formation of FM nanostructures embedded in non-ferromagnetic matrices. Here, we investigate the possibility of creating such nanostructures by ion irradiation. We study the effect of lateral confinement on the ion-irradiation-induced reduction of nonmagnetic metal oxides (e.g., antiferro- or paramagnetic) to form ferromagnetic metals. Our findings are later exploited to form three-dimensional magnetic interfaces between Co, CoO, and Pt by spatial-selective irradiation of CoO/Pt multilayers. We demonstrate that the mechanical displacement of O atoms plays a crucial role in the reduction from insulating, non-ferromagnetic cobalt oxides to metallic cobalt. Metallic cobalt yields both perpendicular magnetic anisotropy in the generated Co/Pt nanostructures and, at low temperatures, exchange bias at vertical interfaces between Co and CoO. If pushed to the limit of ion-irradiation technology, this approach could, in principle, enable the creation of densely packed, atomic-scale ferromagnetic point-contact spin-torque oscillator (STO) networks or conductive channels for current-confined-path-based current perpendicular-to-plane giant magnetoresistance read heads.

Spectroscopic ellipsometry and magneto-optical Kerr effect spectroscopy study of thermally treated Co60Fe20B20 thin films.

We report the optical and magneto-optical properties of amorphous and crystalline Co60Fe20B20 films with thicknesses in the range of 10 nm to 20 nm characterized using spectroscopy ellipsometry (SE) and magneto-optical Kerr effect (MOKE) spectroscopy. We derived the spectral dependence of the dielectric tensor from experimental data for samples prior and after annealing in vacuum. The features of the dielectric function can be directly related to the transitions between electronic states and the observed changes upon annealing can be ascribed to an increase of the crystalline ordering of CoFeB.

Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution.

Resonant X-ray absorption, where an X-ray photon excites a core electron into an unoccupied valence state, is an essential process in many standard X-ray spectroscopies. With increasing X-ray intensity, the X-ray absorption strength is expected to become nonlinear. Here, we report the onset of such a nonlinearity in the resonant X-ray absorption of magnetic Co/Pd multilayers near the Co L[Formula: see text] edge. The nonlinearity is directly observed through the change of the absorption spectrum, which is modified in less than 40 fs within 2 eV of its threshold. This is interpreted as a redistribution of valence electrons near the Fermi level. For our magnetic sample this also involves mixing of majority and minority spins, due to sample demagnetization. Our findings reveal that nonlinear X-ray responses of materials may already occur at relatively low intensities, where the macroscopic sample is not destroyed, providing insight into ultrafast charge and spin dynamics.

Synthesis of Mg and Zn diolates and their use in metal oxide deposition.

The synthesis of complexes [M(OCHMeCH2NMeCH2)2] (5, M = Mg; 7, M = Zn) is described. Treatment of MeHNCH2CH2NMeH (1) with 2-methyloxirane (2) gave diol (HOCHMeCH2NMeCH2)2 (3), which upon reaction with equimolar amounts of MR2 (4, M = Mg, R = Bu; 6, M = Zn, R = Et) gave 5 and 7. The thermal behavior and vapor pressure of 5 and 7 were investigated to show whether they are suited as CVD (= chemical vapor deposition) and/or spin-coating precursors for MgO or ZnO layer formation. Thermogravimetric (TG) studies revealed that 5 and 7 decompose between 80-530 °C forming MgO and ZnO as evidenced by PXRD studies. In addition, TG-MS-coupled experiments were carried out with 7 proving that decomposition occurs by M-O, C-O, C-N and C-C bond cleavages, as evidenced from the detection of fragments such as CH4N+, C2H4N+, C2H5N+, CH2O+, C2H2O+ and C2H3O+. The vapor pressure of 7 was measured at 10.4 mbar at 160 °C, while 5 is non-volatile. The layers obtained by CVD are dense and conformal with a somewhat granulated surface morphology as evidenced by SEM studies. In addition, spin-coating experiments using 5 and 7 as precursors were applied. The corresponding MO layer thicknesses are between 7-140 nm (CVD) or 80 nm and 65 nm (5, 7; spin-coating). EDX and XPS measurements confirm the formation of MgO and ZnO films, however, containing 12-24 mol% (CVD) or 5-9 mol% (spin-coating) carbon. GIXRD studies verify the crystalline character of the deposited layers obtained by CVD and the spin-coating processes.

High-frequency measurements of thermophysical properties of thin films using a modified broad-band frequency domain thermoreflectance approach.

In this work, we present the implementation of a new method to perform high-frequency thermoreflectance measurements on thin films. The so-called differential broad-band frequency domain thermoreflectance method follows broad-band frequency domain thermoreflectance developed previously [Regner et al., Rev. Sci. Instrum. 84(6), 064901 (2013)], without the use of expensive electro-optic modulators. Two techniques are introduced to recover the thermal phase of interest and to separate it from the unwanted instrumental contributions to the recorded phase. Measuring a differential thermal phase by either varying the spot size or offsetting the pump and probe beams, the thermophysical properties of materials can be extracted. This approach enables the study of nanoscale heat transport where non-equilibrium phenomena are dominating.

Model-based magnetization retrieval from holographic phase images.

The phase shift of the electron wave is a useful measure for the projected magnetic flux density of magnetic objects at the nanometer scale. More important for materials science, however, is the knowledge about the magnetization in a magnetic nano-structure. As demonstrated here, a dominating presence of stray fields prohibits a direct interpretation of the phase in terms of magnetization modulus and direction. We therefore present a model-based approach for retrieving the magnetization by considering the projected shape of the nano-structure and assuming a homogeneous magnetization therein. We apply this method to FePt nano-islands epitaxially grown on a SrTiO3 substrate, which indicates an inclination of their magnetization direction relative to the structural easy magnetic [001] axis. By means of this real-world example, we discuss prospects and limits of this approach.

Magnetic Switching in Granular FePt Layers Promoted by Near-Field Laser Enhancement.

Light-matter interaction at the nanoscale in magnetic materials is a topic of intense research in view of potential applications in next-generation high-density magnetic recording. Laser-assisted switching provides a pathway for overcoming the material constraints of high-anisotropy and high-packing density media, though much about the dynamics of the switching process remains unexplored. We use ultrafast small-angle X-ray scattering at an X-ray free-electron laser to probe the magnetic switching dynamics of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. We observe that the combination of laser excitation and applied static magnetic field, 1 order of magnitude smaller than the coercive field, can overcome the magnetic anisotropy barrier between "up" and "down" magnetization, enabling magnetization switching. This magnetic switching is found to be inhomogeneous throughout the material with some individual FePt nanoparticles neither switching nor demagnetizing. The origin of this behavior is identified as the near-field modification of the incident laser radiation around FePt nanoparticles. The fraction of not-switching nanoparticles is influenced by the heat flow between FePt and a heat-sink layer.

Influence of chemical ordering on the thermal conductivity and electronic relaxation in FePt thin films in heat assisted magnetic recording applications.

We report on the out-of-plane thermal conductivities of tetragonal L10 FePt (001) easy-axis and cubic A1 FePt thin films via time-domain thermoreflectance over a temperature range from 133 K to 500 K. The out-of-plane thermal conductivity of the chemically ordered L10 phase with alternating Fe and Pt layers is ~23% greater than the thermal conductivity of the disordered A1 phase at room temperature and below. However, as temperature is increased above room temperature, the thermal conductivities of the two phases begin to converge. Molecular dynamics simulations on model FePt structures support our experimental findings and help shed more light into the relative vibrational thermal transport properties of the L10 and A1 phases. Furthermore, unlike the varying temperature trends in the thermal conductivities of the two phases, the electronic scattering rates in the out-of-plane direction of the two phases are similar for the temperature range studied in this work.

Rapid preparation of electron beam induced deposition Co magnetic force microscopy tips with 10 nm spatial resolution.

Magnetic force microscope Co spike tips with lateral magnetic resolution of 10 nm have been prepared. The Co spikes are grown by electron beam induced deposition of Co from Co(2)(CO)(8) gas precursor. The high resolution Co spikes are fabricated at the spot of a tightly focused electron beam on the tip of commercial atomic force microscope cantilevers. Qualitative investigations indicate that a spike grown on a planar base of Co improves the signal to noise.

Femtosecond single-shot imaging of nanoscale ferromagnetic order in Co/Pd multilayers using resonant x-ray holography.

We present the first single-shot images of ferromagnetic, nanoscale spin order taken with femtosecond x-ray pulses. X-ray-induced electron and spin dynamics can be outrun with pulses shorter than 80 fs in the investigated fluence regime, and no permanent aftereffects in the samples are observed below a fluence of 25 mJ/cm(2). Employing resonant spatially muliplexed x-ray holography results in a low imaging threshold of 5 mJ/cm(2). Our results open new ways to combine ultrafast laser spectroscopy with sequential snapshot imaging on a single sample, generating a movie of excited state dynamics.

Magnetic imaging at linearly polarized x-ray sources.

We present a method for high-resolution magnetic imaging at linearly polarized partially coherent x-ray sources. The magnetic imaging was realized via Fourier transform holography. In order to achieve elliptical x-ray polarization, three different filters were designed based on the x-ray magnetic circular dichroism effect. We present proof-of-principle images of magnetic nanostructures and discuss the application of the method for future experiments at free-electron laser sources.