Gradual modification of the magnetic properties in ferromagnetic films has recently been proposed as an effective method to channel and control spin waves for the development of new functionalities in magnonic devices. Here, we investigate graded FeN films prepared by low-dose nitrogen implantation of Fe epitaxial thin films. Combining Brillouin light scattering measurements and a spin-wave theoretical approach, we show that nitrogen implantation induces a graded profile of both the in-plane and the perpendicular anisotropies along the film thickness. This graduation leads to a significant modification of the spin-wave spatial localization and generates a marked frequency asymmetry in the spin-wave dispersion. Moreover, we find that the anisotropy profile, and as a consequence the dispersion relation, can be tuned on changing the implantation dose, opening a way for the potential use of the graded Fe-N films in magnonic applications.

The dependence of the velocity of surface acoustic wave (SAW) as a function of an external applied magnetic field is investigated in a Fe thin film epitaxially grown on a piezoelectric GaAs substrate. The SAW velocity is observed to strongly depend on both the amplitude and direction of the magnetic field. To interpret the experimental data a phenomenological approach to the relative change in SAW velocity is implemented. We find that the experimental velocity variation can be well reproduced provided that the spin wave dispersion is taken into account. The validity of this phenomenological model is attested by the comparison with a quasi-exact magnetoelastic one.

We calculate the lattice-driven in-plane $(\kappa_{\parallel})$ and out-of-plane $(\kappa_{\perp})$ thermal conductivities of Bi$_2$Se$_3$ bulk, and of films of different thicknesses, using the Boltzmann equation with phonon scattering times obtained from anharmonic third order density functional perturbation theory. We compare our results for the lattice component of the thermal conductivity with published data for $\kappa_{\parallel}$ on bulk samples and with our room-temperature thermoreflectance measurements of $\kappa_{\perp}$ on films of thickness (L) ranging from 18~nm to 191~nm, where the lattice component has been extracted via the Wiedemann-Franz law. Ab-initio theoretical calculations on bulk samples, including an effective model to account for finite sample thickness and defect scattering, compare favorably both for the bulk case (from literature) and thin films (new measurements). In the low-T limit the theoretical in-plane lattice thermal conductivity of bulk Bi$_2$Se$_3$ agrees with previous measurements by assuming the occurrence of intercalated Bi$_2$ layer defects. The measured thermal conductivity monotonically decreases by reducing $L$, its value is $\kappa_{\perp}\approx 0.39\pm 0.08$~W/m$\cdot$K for $L=18$ nm and $\kappa_{\perp}=0.68\pm0.14$~W/m$\cdot$K for $L=191$ nm. We show that the decrease of room-temperature $\kappa_{\perp}$ in Bi$_2$Se$_3$ thin films as a function of sample thickness can be explained by the incoherent scattering of out-of-plane momentum phonons with the film surface. Our work outlines the crucial role of sample thinning in reducing the out-of-plane thermal conductivity.

Ferromagnetic thin films with moderate perpendicular magnetic anisotropy (PMA) are known to support weak stripe domains provided film thickness exceeds a critical value. In this work, we performed both an experimental and theoretical investigation of a peculiar phenomenon shown by weak stripe domains: namely, the stripe domains reorientation when a dc magnetic field is applied in the film plane along the direction perpendicular to the stripes axis. We focus on bct alpha ' -Fe8N1-x thin films obtained by N 2 + implantation of alpha -Fe films epitaxially grown on ZnSe/GaAs(001). By using different ion implantation and heat treatment conditions, we show that it is possible to tune the PMA values. Magnetic force microscopy and vibrating sample magnetometer measurements prove the existence of weak stripe domains at remanence, and of a threshold field for the reorientation of the stripes axis in a transversal field. Using a one-dimensional model of the magnetic stripe domains, where the essential parameter is the maximum canting angle of the stripe magnetization out of the film plane, the various contributions to the magnetic energy can be separately calculated. A linear increase of the reorientation threshold field on the PMA is obtained, in qualitative agreement with experimental data in our Fe-N films, as well as in other thin films with weak stripe domains. Finally, we find that also the rotatable anisotropy field linearly increases as a function of the PMA magnitude.

Recently, electron correlation has been shown to play an important role in unconventional plasmon generation in highly correlated electron systems. Electrons in topological insulators, on the other hand, are massless and insensitive to nonmagnetic scattering due to their protection by time-reversal symmetry, which makes these materials appealing platforms for hosting exotic plasmonic excitations. Here, using a combination of angle-dependent spectroscopic ellipsometry and angle-resolved photoemission spectroscopy as a function of temperature supported by first-principles calculations, we reveal a new pair of correlated plasmonic excitations at 1.04 and 1.52 eV and a significant Fermi level shift of 0.12 eV accompanied by spectral weight transfer in the topological insulator bismuth selenide (Bi 2 Se 3 ). Interestingly, such a spectral weight transfer over a broad energy range causes a drastic change in the charge carrier density whereby the contribution of charge carriers in the bulk starts to rival those in the surface states and Bi 2 Se 3 becomes more uniformly conducting. Our results show the importance of electronic correlations in determining the electronic structure and appearance of correlated plasmons in topological insulators and their potential applications in plasmonics.

Manganese arsenide layers epitaxially grown on GaAs(001) are known to feature a temperature dependent self-assembled microstructure of ordered stripes, alternating the ferromagnetic α and paramagnetic β phases. The surface dipolar fields generated by the α/β stripes have been used for achieving temperature controlled magnetization switching of a ferromagnetic overlayer. For this kind of application, it is advantageous to minimize the MnAs layer thickness. In this work we investigate, using x-ray scattering techniques, the presence of the ordered microstructure as a function of the MnAs layer thickness and we identify a minimum value of ∼40 nm for the formation of ordered α/β stripes in MnAs/GaAs(001). These results have an impact for envisaging magnetization-switching applications that rely on the control of the temperature—or laser-driven surface dipolar fields in MnAs-based devices.

Hybrid heterostructures, made of organic molecules adsorbed on two-dimensional metal monochalcogenide, generally unveil interfacial effects that improve the electronic properties of the single constitutive layers. Here, we investigate the interfacial electronic characteristics of the F4-TCNQ/single layer GaSe heterostructure. A sharp F4-TCNQ/GaSe interface has been obtained and characterized by X-ray photoemission spectroscopy. We demonstrate that a high electron transfer from 1TL GaSe into the adsorbed F4-TCNQ molecules takes place, thereby yielding a reduction in the excess negative charge density of GaSe. Additionally, the direct band structure determination of the heterostructure has been carried out using angle-resolved photoemission spectroscopy, shedding light on essential features such as doping and band offset at the interface. Our results indicate that the buried 1TL GaSe bellow the F4-TCNQ layer exhibits a robust inversion of the valence dispersion at the Γ point, forming a Mexican-hat-shaped dispersion with 120 ± 10 meV of depth. Our experiments also reveal that F4-TCNQ can significantly tune the electronic properties of 1TL GaSe by shifting the band offset of about 0.16 eV toward lower binding energies with respect to the Fermi level, which is a key feature for envisioning its applications in nanoelectronics.

We investigate the orthorhombic distortion and the structural dynamics of epitaxial MnAs layers on GaAs(001) using static and time-resolved x-ray diffraction. Laser-induced intensity oscillations of Bragg reflections allow us to identify the optical phonon associated with orthorhombic distortion and to follow its softening along the path towards an undistorted phase of hexagonal symmetry. The frequency of this mode falls in the THz range, in agreement with recent calculations. Incomplete softening suggests that the beta - gamma transformation deviates from a purely second-order displacive transition.

Spin waves propagation in ferromagnetic films, several tens of nanometers thick, have recently received increasing attention, in view of the development of magnonic devices operating in the GHz range of frequencies. A detailed knowledge of the dispersion curves and of the spatial characteristics of the spin-wave modes is preliminary to any technological application, particularly in the “mesoscopic range” (50–200 nm) of film thickness, where several dipole-exchange modes may appear in the spectrum, exhibiting frequency crossing and hybridization as a function of their wave number. In this work, the mutual interaction and the hybridization of the dipole-exchange spin-wave modes was investigated in a nitrogen-implanted iron (Fe-N) film, 78-nm-thick, in-plane magnetized. The spin-wave dispersion curves were measured by using Brillouin light scattering, and the experimental results were interpreted combining micromagnetic simulations and theoretical calculations in the framework of a dipole-exchange spin-wave mode approach. A noticeable hybridization between the spin-wave modes was observed, due to the simultaneous presence of a marked perpendicular magnetic anisotropy and a rather high saturation magnetization. The hybridization was found to induce a very large gap ( (cid:2)ν ≈ 5 GHz) between the low-frequency spin waves at high wave vector ( k ≈ 10 5 rad / cm). Consequently, in such a k range the simultaneous presence of two spin-wave modes with sizeable ( v g ≈ 1 . 5 km / s) but opposite group velocity was observed, opening a way for the potential use of Fe-N films in magnon spintronics.

Two-dimensional monochalcogenides (MX) have been identified as a unique and promising class of layered materials in recent years. The valence band of single-layer MX, as predicted by theory, is inverted into a bow-shaped (often referred to as an inverted sombrero) and relatively flat dispersion, which is expected to give rise to strongly correlated effects. The inversion leads to an indirect band gap, which is consistent with photoluminescence (PL) experiments, but PL provides no direct evidence of the band inversion in the valence band. Here we demonstrate for a hexagonal MX crystal, gallium selenide (GaSe), using a combination of angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT), that the valence band of monolayer (ML) GaSe exhibits a robust inversion of the valence dispersion at the Gamma point forming a bow-shaped dispersion with a depth of 120 +/- 10 meV between the double valence band maximum along the FK direction. We also demonstrate that the deeper-lying bands detected in the ARPES spectrum are consistent with DFT calculations only if spin-orbit coupling is considered. The presented ARPES evidence that spin-orbit coupling leads to the splitting of two fourfold-degenerate states into four Kramers doublets is of significance for PL measurements, as the change in energy of the second highest valence state at the Gamma point has a measurable effect on the PL energies in high-energy luminescence. We predict the optical absorption coefficients for the principal transitions in ML GaSe using a four-band k . p model parametrized from first-principles theory with spin-orbit effects considered.

Two-dimensional (2D) materials have recently been the focus of extensive research. By following a similar trend as graphene, other 2D materials, including transitionmetal dichalcogenides (MX2) and metal mono-chalcogenides (MX), show great potential for ultrathin nanoelectronic and optoelectronic devices. Despite the weak nature of interlayer forces in semiconducting MX materials, their electronic properties are highly dependent on the number of layers. Using scanning tunneling microscopy and spectroscopy, we demonstrate the tunability of the quasiparticle energy gap of few-layered gallium selenide (GaSe) directly grown on a bilayer graphene substrate by molecular beam epitaxy. Our results show that the band gap is about 3.50 +/- 0.05 eV for single-tetralayer, 3.00 +/- 0.05 eV for bi-tetralayer, and 2.30 +/- 0.05 eV for tri-tetralayer GaSe. This band-gap evolution of GaSe, particularly the shift of the valence band with respect to the Fermi level, was confirmed by angle-resolved photoemission spectroscopy (ARPES) measurements and our theoretical calculations. Moreover, we observed a charge transfer in the GaSe/graphene van der Waals (vdW) heterostructure using ARPES. These findings demonstrate the high impact on the GaSe electronic band structure and electronic properties that can be obtained by the control of 2D materials layer thickness and the graphene induced doping.

It was shown recently that the Fe magnetization reversal in the Fe/MnAs/GaAs(001) epitaxial system, attained by temperature control of the regular stripe pattern of the MnAs α- and β-phases, can also be driven by an ultrashort optical laser pulse. In the present time-resolved scattering experiment, we address the dynamics of the MnAs α-β self-organized stripe pattern induced by a 100 fs optical laser pulse, using as a probe the XUV radiation from the FERMI free-electron laser. We observe a loss in the diffraction intensity from the ordered α-β stripes that occurs at two characteristic timescales in the range of ~10−12 and ~10−10 s. We associate the first intensity drop with ultrafast electron-lattice energy exchange processes within the laser-MnAs interaction volume and the second with thermal diffusion towards the MnAs/GaAs interface. With the support of model calculations, the observed dynamics are interpreted in terms of the formation of a laterally homogeneous MnAs overlayer, the thickness of which evolves in time, correlating the MnAs microstructure dynamics with the Fe magnetization response.

Stacking two-dimensional materials in so-called van der Waals (vdW) heterostructures, like the combination of GaSe and graphene, provides the ability to obtain hybrid systems that are suitable to design optoelectronic devices. Here, we report the structural and electronic properties of the direct growth of multilayered GaSe by molecular beam epitaxy on graphene. Reflection high-energy electron diffraction images exhibited sharp streaky features indicative of a high-quality GaSe layer produced via a vdW epitaxy. Micro-Raman spectroscopy showed that, after the vdW heterointerface formation, the Raman signature of pristine graphene is preserved. However, the GaSe film tuned the charge density of graphene layer by shifting the Dirac point by about 80 meV toward lower binding energies, attesting to an electron transfer from graphene to GaSe. Angle-resolved photoemission spectroscopy (ARPES) measurements showed that the maximum of the valence band of the few layers of GaSe are located at the Γ point at a binding energy of about -0.73 eV relative to the Fermi level (p-type doping). From the ARPES measurements, a hole effective mass defined along the ΓM direction and equal to about m*/m0 = -1.1 was determined. By coupling the ARPES data with high-resolution X-ray photoemission spectroscopy measurements, the Schottky interface barrier height was estimated to be 1.2 eV. These findings allow a deeper understanding of the interlayer interactions and the electronic structure of the GaSe/graphene vdW heterostructure.

We investigated the structural, magnetic, and electronic properties of Bi2Se3 epilayers containing Fe grown on GaAs(111) by molecular beam epitaxy. It is shown that, in the window of growth parameters leading to Bi2Se3 epilayers with optimized quality, Fe atom clustering leads to the formation of FexSey inclusions. These objects have platelet shape and are embedded within Bi2Se3. Monoclinic Fe3Se4 is identified as the main secondary phase through detailed structural measurements. Due to the presence of the hard ferrimagnetic Fe3Se4 inclusions, the system exhibits a very large coercive field at low temperature and room temperature magnetic ordering. Despite this composite structure and the proximity of a magnetic phase, the surface electronic structure of Bi2Se3 is preserved, as shown by the persistence of a gapless Dirac cone at Γ.

Spintronic devices currently rely on magnetization control by external magnetic fields or spin-polarized currents. Developing temperature-driven magnetization control has potential for achieving enhanced device functionalities. Recently, there has been much interest in thermally induced magnetisation switching (TIMS), where the temperature control of intrinsic material properties drives a deterministic switching without applying external fields. TIMS, mainly investigated in rare-earth-transition-metal ferrimagnets, has also been observed in epitaxial Fe/MnAs/GaAs(001), where it stems from a completely different physical mechanism. In Fe/MnAs temperature actually modifies the surface dipolar fields associated with the MnAs magnetic microstructure. This in turn determines the effective magnetic field acting on the Fe overlayer. In this way one can reverse the Fe magnetization direction by performing thermal cycles at ambient temperatures. Here we use element selective magnetization measurements to demonstrate that various magnetic configurations of the Fe/MnAs/GaAs(001) system are stabilized predictably by acting on the thermal cycle parameters and on the presence of a bias field. We show in particular that the maximum temperature reached during the cycle affects the final magnetic configuration. Our findings show that applications are possible for fast magnetization switching, where local temperature changes are induced by laser excitations.

Topological insulators (Bi2Se3) of single-and few-quintuple-layer (few-QLs) films were investigated by Raman spectroscopy and epitaxied on a GaAs substrate. At a measurement temperature of 80 K, we observed the emergence of additional A(2u) and E-u modes (Raman inactive in the bulk crystal) below 9-QLs film thicknesses, assigned to the crystal-symmetry breakdown in ultrathin films. Furthermore, the out-of-plane A(1g) modes changed in width, frequency, and intensity for decreasing numbers of QL, while the in-plane E-g mode split into three Raman lines, not resolved in previous room temperature experiments. The out-of-plane Raman modes showed a strong Raman resonance at 2.4 eV for around 4-QLs film thickness, and the resonant position of the same modes shifted to 2.2 eV for 18-QLs-thick film. The film thickness-dependence of the phonons frequencies cannot solely be explained within models of weak van der Waals interlayer coupling. The results are discussed in terms of stacking-induced changes in inter-and intralayer bonding and/or the presence of long-range Coulombic interlayer interactions in topological insulator Bi2Se3. This work demonstrates that Raman spectroscopy is sensitive to changes in film thickness over the critical range of 9-to 4-QLs, which coincides with the transition between a gapless topological insulator (occurring above 6-QLs) to a conventional gapped insulator (occurring below 4-QLs).

The most advanced X-ray sources (third generation synchrotrons, linear free-electron lasers and high-harmonic generation sources) widen the range of application of X-ray scattering techniques considerably. Beyond flux and brilliance, improvements in polarization tuneability, degree of coherence and selectable time-structure promoted new methods for investigating the electronic and magnetic properties of solids. The soft X-ray range (50-2000 eV) is well suited for studying magneto-optical effects in laterally confined submicron sized objects, either artificially built or self-assembled. First, by tuning the photon energy at a core resonance, one provides the X-ray scattering technique with element selectivity. Second, resonant excitations make the optical constants sensitive to the local magnetization by introducing large off-diagonal elements in the dielectric tensor; since magnetic effects are stronger when the core excitation produces a dipolar transition to final states involving the magnetic orbitals ( 3d for the first row TM; 4 f for RE), the most interesting resonances for X-ray magneto-optics [(2, 3) p → 3 d and (3, 4) d → 4 f] are all located in the soft X-ray region. Finally, the wavelengths corresponding to soft X-rays are very well suited for scattering studies of nanometer- to micrometer-sized magnetic structures. We will present the results of recent soft X-ray resonant scattering experiments, showing that the combination of element selectivity, magnetic sensitivity and structural analysis can help disentangling and understanding the magnetic properties of complex self-assembled periodic systems. Lastly, recent applications of coherent scattering to the X-ray holographic imaging of magnetic domains will be presented.

The molecular beam epitaxy growth of Fe on MnAs/GaAs(001) leads to the formation of a new phase of the FeMnAs compound at the Fe/MnAs interface. We investigated the structural and magnetic properties of this interfacial layer by high angle annular dark field imaging in a scanning transmission electron microscope (HAADF-STEM). We determined that the epitaxial FeMnAs layer presents an unusual orthorhombic structure, with vacancy ordering. We completed our study by ab initio calculations, and we foresee an antiferromagnetic ground state for this structure.

Scattering of 130 nm radiation with 100 fs pulse length was used to monitor the α/β-striped microstructure in MnAs/GaAs(001), after a 390 nm 5 mJcm−2 pump pulse. A strong reduction of the Bragg peak intensity, corresponding to a widening of the β-stripes, takes place with a characteristic time of 15 ps. These results are relevant within the context of using MnAs/GaAs(001) as a template for the growth of ferromagnetic films, whose magnetization direction can be controlled by modifying the template temperature.