The electronic structure of topological insulator/magnetic metal (TI/MM) interfaces is of great importance for understanding of exotic spin-dependent phenomena and realization of advanced spin-orbitronic devices. Here, we employ a model system of submonolayer transition metal (TM) deposited on the surface of a topological crystalline insulator (TCI) of Pb_1-xSn_xSe to systematically map out the modification of the surface electronic structure by angle-resolved photoemission spectroscopy (ARPES) as a function of coverage. For the polar (111) Pb_1-xSn_xSe surface, we observe the coexistence of the Dirac topological surface states (TSS) and Rashba-split surface states (RSS) induced by the combined effects of inversion-symmetry breaking, surface band bending and orbital angular momentum effects. In particular, we demonstrate very large Rashba splittings can be obtained and the Rashba parameter (α_R) can be tuned over a remarkably wide range from 0 to 3.5 eV · A, depending on the type and coverage of the TM adatoms. Model-Hamiltonian calculations corroborate the experimental findings and reveal that this coexistence results from the filling of the TSS by the surface doping caused by the TM. In contrast, for the nonpolar (001) surface exhibiting a double Dirac cone topological surface state, the inversion symmetry is preserved and hence no Rashba-split surface states emerge. Instead, surface charge imbalance induces dephasing of the wave functions of the double Dirac cones that diminishes the momentum-space separation between them. These findings shed light on novel phenomena occurring at the topological insulator / transition metal interface, offering a versatile platform for future spintronic and quantum devices.
We investigate the origin of ferromagnetism (FM) and the exceptionally high Curie temperature (TC) in undoped SnO2 films. Ultra-thin SnO2 films were found to exhibit significant FM, while thicker films show a diamagnetic behavior. Structural and chemical analyses reveal a variation in oxygen vacancy concentrations between thin and thick films. Notably, an exceptionally high TC exceeding 800 K is observed for the first time. XPS and XAS analyses reveal the presence of oxygen and tin vacancies, which might play a crucial role in the observed magnetism. Theoretically, it was supposed that oxygen vacancies play a crucial role in the FM of SnO2 films. However, the experimentally observed TC surpasses the predicted 505 K, suggesting additional contributing factors. This suggests that both oxygen and tin defects might contribute to the total magnetic moment. The findings highlight the key role of defect-induced magnetism in SnO2 thin films and provide insights into the fundamental mechanism driving high- TC FM in undoped oxide semiconductors.
Unlike TiO2 and SnO2, room temperature ferromagnetism in pristine ZnO films does not appear to originate from oxygen vacancies. In this study, we investigated thin films of ZnO deposited on R-cut Al2O3 by sputtering. The ZnO films were ferromagnetic, with a very high T C of about 800 K and were quite magnetically homogenous. Our experiments were complemented by quantum-mechanical calculations of both bulk wurtzite-structure ZnO and its (0001) surfaces, with and without Zn vacancies. While the bulk ground state and the bulk-terminated, vacancy-free (0001) surfaces were non-magnetic, a higher concentration of Zn vacancies deep beneath the surface was shown to contribute magnetic moments to the ferromagnetic state of ZnO.
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Here we report on Landau level spectroscopy of an epitaxially grown thin film of the topological insulator Sb2Te3, complemented by ellipsometry and magneto-transport measurements. The observed response suggests that Sb2Te3 is a direct-gap semiconductor with the fundamental band gap located at the \Gamma point, or along the trigonal axis, and its width reaches Eg = 190 meV at low temperatures. Our data also indicate the presence of other low-energy extrema with a higher multiplicity in both the conduction and valence bands. The conclusions based on our experimental data are confronted with and to a great extent corroborated by the electronic band structure calculated using the GW method.
Non-volatile phase-change materials with large optical contrast are essential for future tunable nanophotonics. Antimony trisulfide (Sb2S3) has recently gained popularity in this field due to its low absorption in the visible spectral region. Although several Sb2S3 deposition techniques have been reported in the literature, none of them was optimized with respect to the lowest possible absorption and largest optical contrast upon the phase change. Here, we present a comprehensive multi-parameter optimization of pulsed laser deposition of Sb2S3 towards this end. We correlate the specific deposition and annealing parameters with the resulting optical properties and propose the combination leading to films with extraordinary qualities (Δn = 1.2 at 633 nm). Finally, we identify crystal orientations and vibrational modes associated with the largest change in the refractive index and propose them as useful indicators of the Sb2S3 switching contrast.
Defect control is critical to achieve long carrier lifetimes in semiconductors. SnS is a promising thermoelectric and photovoltaic material, in which native defects play a detrimental role, particularly in photovoltaics. In this study, we investigated the Fe-doping of SnS and the interaction of Fe impurities with native defects in a series of single crystals of Sn1-xFexS up to concentrations of x = 0.05. Although the doped single crystals appear rather disordered, the hole mobility is very high (similar to 8500 cm(2)V(-1)s(-1) at 30 K for Sn0.99Fe0.01S), suggesting that holemediated charge transport in this material is largely insensitive to extrinsic impurities. Charge transport analysis suggests that the incorporation of Fe atoms leads to the healing of the intrinsic defect structure and the exclusion of minority electrons from charge transport, allowing the observation of high hole mobility.
Altermagnetic (AM) materials exhibit non-relativistic, momentum-dependent spin-split states, ushering in new opportunities for spin electronic devices. While the characteristics of spin-splitting have been documented within the framework of the non-relativistic spin group symmetry, there has been limited exploration of the inclusion of relativistic symmetry and its impact on the emergence of a novel spin-splitting in the band structure. This study delves into the intricate relativistic electronic structure of an AM material, alpha-MnTe. Employing temperature-dependent angle-resolved photoelectron spectroscopy across the AM phase transition, we elucidate the emergence of a relativistic valence band splitting concurrent with the establishment of magnetic order. This discovery is validated through disordered local moment calculations, modeling the influence of magnetic order on the electronic structure and confirming the magnetic origin of the observed splitting. The temperature-dependent splitting is ascribed to the advent of relativistic spin-splitting resulting from the strengthening of AM order in alpha-MnTe as the temperature decreases. This sheds light on a previously unexplored facet of this intriguing material.
The interplay between spin-orbit interaction and magnetic order is one of the most active research fields in condensed matter physics and drives the search for materials with novel, and tunable, magnetic and spin properties. Here we report on a variety of unique and unexpected observations in thin multiferroic Ge1-xMnxTe films. The ferrimagnetic order parameter in this ferroelectric semiconductor is found to switch direction under magnetostochastic resonance with current pulses many orders of magnitude lower as for typical spin-orbit torque systems. Upon a switching event, the magnetic order spreads coherently and collectively over macroscopic distances through a correlated spin-glass state. Utilizing these observations, we apply a novel methodology to controllably harness this stochastic magnetization dynamics.
Fast, reversible, and low-power manipulation of the spin texture is crucial for next generation spintronic devices like non-volatile bipolar memories, switchable spin current injectors or spin field effect transistors. Ferroelectric Rashba semiconductors (FERSC) are the ideal class of materials for the realization of such devices. Their ferroelectric character enables an electronic control of the Rashba-type spin texture by means of the reversible and switchable polarization. Yet, only very few materials have been established to belong to this class of multifunctional materials. Here, Pb1-xGexTe is unraveled as a novel FERSC system down to nanoscale. The ferroelectric phase transition and concomitant lattice distortion is demonstrated by temperature dependent X-ray diffraction, and its effect on electronic properties are measured by angle-resolved photoemission spectroscopy. In few nanometer-thick epitaxial heterostructures, a large Rashba spin-splitting is exhibiting a wide tuning range as a function of temperature and Ge content. Our work defines Pb1- xGexTe as a high-potential FERSC system for spintronic applications.
Dataset for publication DOI 10.1038/s41467-023-41718-4 including images, data used for generate that images, the input file, converged potential file used for the calculations on SPR-KKR package 8.6., raw data files.
We investigate the effect of low concentrations of iron on the physical properties of SnS van der Waals crystals grown from the melt. By means of scanning tunneling microscopy (STM) and photoemission spectroscopy we study Fe-induced defects and observe an electron doping effect in the band structure of the native p-type SnS semiconductor. Atomically resolved and bias dependent STM data of characteristic defects are compared to ab initio density functional theory simulations of vacancy (VS and VSn), Fe substitutional (FeSn), and Fe interstitial (Feint) defects. While native SnS is dominated by acceptor-like VSn vacancies, our results show that Fe preferentially occupies donor-like interstitial Feint sites in close proximity to VSn defects along the high-symmetry c-axis of SnS. The formation of such well-defined coupled (VSn, Feint) defect pairs leads to local compensation of the acceptor-like character of VSn, which is in line with a reduction of p-type carrier concentrations observed in our Hall transport measurements.
We have studied ultrafast dynamics of thin films of LaCoO$_3$ and La$_{0.5}$Sr$_{0.5}$CoO$_3$ with femtosecond pump-probe ellipsometry in the energy range of 1.6-3.4 eV. We have observed a large pump-induced transfer of spectral weight in LaCoO$_3$ that corresponds to an insulator-to-metal transition. The photo-induced metallic state initially relaxes via a fast process with a decay constant of about 200 fs. Both LaCoO$_3$ and La$_{0.5}$Sr$_{0.5}$CoO$_3$ exhibit a significant secondary transient structure in the 1-30 ps range. Results of measurements on films with different thicknesses demonstrate that it corresponds to a propagation of an acoustic strain pulse. On timescales longer than 100 ps, heat diffusion to the substrate takes place that can be modelled with a bi-exponential decay.
Equiatomic and chemically ordered FeRh and MnRh compounds feature a first-order metamagnetic phase transition between antiferromagnetic and ferromagnetic order in the vicinity of room temperature, exhibiting interconnected structural, magnetic, and electronic order parameters. We show that these two alloys can be combined to form hybrid metamagnets in the form of sputter-deposited superlattices and alloys on single-crystalline MgO substrates. Despite being structurally different, the magnetic behavior of the alloys with substantial Mn content resembles that of the FeRh/MnRh superlattices in the ultrathin individual layer limit. For FeRh/MnRh superlattices, dissimilar lattice distortions of the constituent FeRh and MnRh layers at the antiferromagnetic-ferromagnetic transition cause double-step transitions during cooling, while the magnetization during the heating branch shows a smooth, continuous trend. For Fe50-xMnxRh50 alloy films, the substitution of Mn at the Fe sites introduces an effective tensile in-plane strain and magnetic frustration in the highly ordered epitaxial films, largely influencing the phase transition temperature TM (by more than 150 K). In addition, Mn acts as a surfactant, enabling the growth of continuous thin films at higher temperatures. Thus, the introduction of hybrid FeRh-MnRh systems with adjustable parameters provides a pathway for the realization of tunable spintronic devices based on magnetic phase transitions.
We prepared La0.3Sr0.7CoO3_delta thin films by pulsed laser deposition on (LaAlO3)0.3(Sr2TaAlO6)0.7 substrates with and without a protective LaAlO3 capping layer and investigated their structural and magnetic properties. We observed that, in the uncapped films, the Curie temperature strongly decreased after annealing in helium at-mosphere, and it significantly decreased even in samples stored for several weeks at room temperature. The decrease of the Currie temperature is caused by an increase of the concentration of oxygen vacancies, delta. How-ever, we show that already a 3 nm thin LaAlO3 capping layer can essentially conserve delta at room temperature, and it considerably slows down the formation of oxygen vacancies at elevated temperatures.
The impact of Gd addition on the structural and magnetic properties of L10-FePt alloy thin films, which were sputter-deposited on MgO(001) substrates at 800°C, was investigated. A rapid deterioration of L10 chemical ordering along with a strong amorphization effect is observed with addition of Gd. At more than 20 at. % Gd, additional crystalline phases occur. Due to the diminishing L10 chemical order, the perpendicular magnetic anisotropy (PMA) gets strongly reduced from about 3 down to 1 MJ/m3 with addition of 14 at. % Gd. For higher Gd concentrations, the easy axis of magnetization turns fully in-plane due to dominating magnetic shape anisotropy. Furthermore, the saturation magnetization gets reduced with Gd addition due to the antiferromagnetic coupling between the Fe and Gd magnetic moments. Also, the Curie temperature can be lowered. Interestingly, with addition of Gd, a change in film morphology takes place, changing from an isolated island structure to a more continuous film morphology, which is of particular interest for samples with low Gd concentration as these films exhibit still strong PMA but rather low coercive fields.
The spherical polyvinylpyrrolidone (PVP) stabilized red Se NPs (PVP-Se NPs) with a mean size of similar to 45 nm were prepared via upgraded one-step wet chemical reduction by L-cysteine, which considerably shortened the synthesis procedure. Their morphological features were characterized by high-resolution scanning transmission electron microscopy, UV-VIS spectroscopy, and small-angle X-ray scattering method. The toxicological properties of PVP-Se NPs were analyzed by colorimetric cell viability assay based on the reduction of a yellow tetrazolium salt (XTT) in mitochondria, a further assay based on the measurement of lactate dehydrogenase (LDH) release from damaged cell membrane, and finally by cell proliferation assay. The antifungal effect of PVP-Se NPs alone, or in a mixture of commercial fungicide containing 2% of boric acid, 2% alkylbenzyldimethylammonium chloride, and similar to 0.9% ethanolamine in distilled water was tested on the brown-rot fungus Serpula lacrymans The fungus belongs to important basidiomycetes causing economically significant decay of wood, mainly in houses and particularly cold soil cellars. The average mass loss tests performed on spruce wood blocks after four months of inoculation with S. lacrymans showed an enhanced antifungal effect of the mixture of PVP-Se NPs with a commercial fungicide than a PVP-Se NPs or commercial fungicide alone, which proved their synergistic effect on inhibiting fungi growth. Finally, scanning electron microscopy analysis of outer and inner parts of wood blocks treated with our novel mixture was performed.
We have grown La0.3Sr0.7CoO3–δ thin films by pulsed laser deposition on (LaAlO3)0.3(Sr2TaAlO3)0.7 substrates with and without a protective LaAlO3 capping layer and investigated their structural and magnetic properties. We have observed that, in the uncapped films, the Curie temperature strongly decreased after annealing in helium atmosphere, and it significantly decreased even in samples stored for several weeks at room temperature. The decrease of the Currie temperature is caused by an increase of the concentration of oxygen vacancies, δ. However, we show that already a 3 nm thin LaAlO3 capping layer can essentially conserve δ at room temperature, and it considerably slows down the formation of oxygen vacancies at elevated temperatures.
The interplay between spin-orbit interaction (SOI) and magnetic order is currently one of the most active research fields in condensed matter physics and leading the search for materials with novel and tunable magnetic and spin properties. Here we report on a variety of unexpected and unique observations in thin multiferroic _1-xMn_xTe films. The ferrimagnetic order in this ferroelectric semiconductor is found to reverse with current pulses six orders of magnitude lower as for typical spin-orbit torque systems. Upon a switching event, the magnetic order spreads coherently and collectively over macroscopic distances through a correlated spin-glass state. Lastly, we present a novel methodology to controllably harness this stochastic magnetization dynamics, allowing us to detect spatiotemporal nucleation of topological spin textures we term “skyrmiverres”.