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Altermagnets are an emerging third elementary class of magnets. Unlike ferromagnets, their distinct crystal symmetries inhibit magnetization while, unlike antiferromagnets, they promote strong spin polarization in the band structure. The corresponding unconventional mechanism of timereversal symmetry breaking without magnetization in the electronic spectra has been regarded as a primary signature of altermagnetism, but has not been experimentally visualized to date. We directly observe strong time-reversal symmetry breaking in the band structure of altermagnetic RuO$_2$ by detecting magnetic circular dichroism in angle-resolved photoemission spectra. Our experimental results, supported by ab initio calculations, establish the microscopic electronic-structure basis for a family of novel phenomena and functionalities in fields ranging from topological matter to spintronics, that are based on the unconventional time-reversal symmetry breaking in altermagnets.

We use time- and angle-resolved photoemission spectroscopy (tr-ARPES) to investigate ultrafast charge transfer in an epitaxial heterostructure made of monolayer WS$_2$ and graphene. This heterostructure combines the benefits of a direct gap semiconductor with strong spin-orbit coupling and strong light-matter interaction with those of a semimetal hosting massless carriers with extremely high mobility and long spin lifetimes. We find that, after photoexcitation at resonance to the A-exciton in WS$_2$, the photoexcited holes rapidly transfer into the graphene layer while the photoexcited electrons remain in the WS$_2$ layer. The resulting charge transfer state is found to have a lifetime of $\sim1$\,ps. We attribute our findings to differences in scattering phase space caused by the relative alignment of WS$_2$ and graphene bands as revealed by high resolution ARPES. In combination with spin-selective excitation using circularly polarized light the investigated WS$_2$/graphene heterostructure might provide a new platform for efficient optical spin injection into graphene., Comment: 28 pages, 14 figures

Our ability to understand and tailor metal-organic interfaces is mandatory to functionalize organic complexes for next generation electronic and spintronic devices. For magnetic data storage applications, metal-carrying organic molecules, so called single molecular magnets (SMM) are of particular interest as they yield the possibility to store information on the molecular scale. In this work, we focus on the adsorption properties of the prototypical SMM Sc3N@C80 grown in a monolayer film on the Ag(111) substrate. We provide clear evidence of a pyramidal distortion of the otherwise planar Sc3N core inside the carbon cage upon the adsorption on the Ag(111) surface. This adsorption induced structural change of the Sc3N@C80 molecule can be correlated to a charge transfer from the substrate into the lowest unoccupied molecular orbital of Sc3N@C80, which significantly alters the charge density of the fullerene core. Our comprehensive characterization of the Sc3N@C80-Ag(111) interface hence reveals an indirect coupling mechanism between the Sc3N core of the fullerene molecule and the noble metal surface mediated via an interfacial charge transfer. Our work shows that such an indirect coupling between the encapsulated metal centers of SMM and metal surfaces can strongly affect the geometric structure of the metallic centers and thereby potentially also alters the magnetic properties of SMMs on surfaces., Comment: Copyright: https://journals.aps.org/authors/transfer-of-copyright-agreement; All copyrights by APS

We have investigated the atomic and electronic structure of the ($\sqrt{3}\times \sqrt{3}$)$R30^{\circ}$ SnAu$_2$/Au(111) surface alloy. Low energy electron diffraction and scanning tunneling microscopy measurements show that the native herringbone reconstruction of bare Au(111) surface remains intact after formation of a long range ordered ($\sqrt{3}\times \sqrt{3}$)$R30^{\circ}$ SnAu$_2$2/Au(111) surface alloy. Angle-resolved photoemission and two-photon photoemission spectroscopy techniques reveal Rashba-type spin-split bands in the occupied valence band with comparable momentum space splitting as observed for the Au(111) surface state, but with a hole-like parabolic dispersion. Our experimental findings are compared with density functional theory (DFT) calculation that fully support our experimental findings. Taking advantage of the good agreement between our DFT calculations and the experimental results, we are able to extract that the occupied Sn-Au hybrid band is of (s, d)-orbital character while the unoccupied Sn-Au hybrid bands are of (p, d)-orbital character. Hence, we can conclude that the Rashba-type spin splitting of the hole-like Sn-Au hybrid surface state is caused by the significant mixing of Au d- to Sn s-states in conjunction with the strong atomic spin-orbit coupling of Au, i.e., of the substrate., Comment: Copyright: https://journals.aps.org/authors/transfer-of-copyright-agreement; All copyrights by APS

The interplay of light and magnetism has been a topic of interest since the original observations of Faraday and Kerr where magnetic materials affect the light polarization. While these effects have historically been exploited to use light as a probe of magnetic materials there is increasing research on using polarized light to alter or manipulate magnetism. For instance deterministic magnetic switching without any applied magnetic fields using laser pulses of the circular polarized light has been observed for specific ferrimagnetic materials. Here we demonstrate, for the first time, optical control of ferromagnetic materials ranging from magnetic thin films to multilayers and even granular films being explored for ultra-high-density magnetic recording. Our finding shows that optical control of magnetic materials is a much more general phenomenon than previously assumed. These results challenge the current theoretical understanding and will have a major impact on data memory and storage industries via the integration of optical control of ferromagnetic bits., Comment: 21 pages, 11 figures

Irradiating a ferromagnetic material with an ultrashort laser pulse leads to demagnetization on a femtosecond timescale. We implement Elliott-Yafet type spin-flip scattering, mediated by electron-electron and electron-phonon collisions, into the framework of a spin-resolved Boltzmann equation. Considering three mutually coupled reservoirs, (i) spin-up electrons, (ii) spin-down electrons and (iii) phonons, we trace non-equilibrium electron distributions during and after laser excitation. We identify the driving force for ultrafast magnetization dynamics as the equilibration of temperatures and chemical potentials between the electronic subsystems. This principle can be used to easily predict the maximum quenching of magnetization upon ultrashort laser irradiation in any material, as we show for the example of 3d-ferromagnetic nickel.

In this article we investigate the surface spin polarization in a 100 nm Co2Cr0.6Fe0.4Al (CCFA) film grown ex situ epitaxially on MgO(100) with a 10 nm Fe buffer layer by means of spin resolved photoemission. We show that a careful in situ preparation of the sample surface leads to values for the room temperature spin polarization up to 45% at the Fermi level. To our knowledge, this is the highest value measured so far at the surface region of a full Heusler alloy at room temperature., Comment: 8 pages, 3 figures; submitted to J. Phys. D: Appl. Phys

We have grown thin films of the Heusler compound Co_2FeSi by RF magnetron sputtering. On (100)-oriented MgO substrates we find fully epitaxial (100)-oriented and L2_1 ordered growth. On Al_2O_3 (11-20) substrates, the film growth is (110)-oriented, and several in-plane epitaxial domains are observed. The temperature dependence of the electrical resistivity shows a power law with an exponent of 7/2 at low temperatures. Investigation of the bulk magnetic properties reveals an extrapolated saturation magnetization of 5.0 mu_B/fu at 0 K. The films on Al_2O_3 show an in-plane uniaxial anisotropy, while the epitaxial films are magnetically isotropic in the plane. Measurements of the X-ray magnetic circular dichroism of the films allowed us to determine element specific magnetic moments. Finally we have measured the spin polarization at the surface region by spin-resolved near-threshold photoemission and found it strongly reduced in contrast to the expected bulk value of 100%. Possible reasons for the reduced magnetization are discussed., Comment: 9 pages, 12 figures

We have studied the possibly half metallic Co2FeSi full Heusler alloy by means of spin- and time-resolved photoemission spectroscopy. For excitation, the second and fourth harmonic of femtosecond Ti:sapphire lasers were used, with photon energies of 3.1 eV and 5.9 eV, respectively. We compare the dependence of the measured surface spin polarization on the particular photoemission mechanism, i.e. 1-photon-photoemission (1PPE) or 2-photon photoemission (2PPE). The observed differences in the spin polarization can be explained by a spin-dependent lifetime effect occurring in the 2-photon absorption process. The difference in escape depth of the two methods in this context suggests that the observed reduction of spin polarization (compared to the bulk) cannot be attributed just to the outermost surface layer but takes place at least 4-6 nm away from the surface., Comment: 7 pages, 3 figures; submitted to Journal of Magnetism and Magnetic Materials

Electron-spin relaxation at different surfaces of p-doped GaAs is investigated by means of spin, time and energy resolved 2-photon photoemission. These results are contrasted with bulk results obtained by time-resolved Faraday rotation measurements as well as calculations of the Bir-Aronov-Pikus spin-flip mechanism. Due to the reduced hole density in the band bending region at the (100) surface the spin-relaxation time increases over two orders of magnitude towards lower energies. At the flat-band (011) surface a constant spin relaxation time in agreement with our measurements and calculations for bulk GaAs is obtained., Comment: 6 pages, 4 figures

The mechanisms for spin relaxation in semiconductors are reviewed, and the mechanism prevalent in p-doped semiconductors, namely spin relaxation due to the electron-hole exchange interaction, is presented in some depth. It is shown that the solution of Boltzmann-type kinetic equations allows one to obtain quantitative results for spin relaxation in semiconductors that go beyond the original Bir-Aronov-Pikus relaxation-rate approximation. Experimental results using surface sensitive two-photon photoemission techniques show that the spin relaxation-time of electrons in p-doped GaAs at a semiconductor/metal surface is several times longer than the corresponding bulk spin relaxation-times. A theoretical explanation of these results in terms of the reduced density of holes in the band-bending region at the surface is presented., Comment: 33 pages, 12 figures; earlier submission replaced by corrected and expanded version; eps figures now included in the text