Spin fluctuation induced Weyl semimetal state in the paramagnetic phase of EuCd2As2.

Weyl fermions as emergent quasiparticles can arise in Weyl semimetals (WSMs) in which the energy bands are nondegenerate, resulting from inversion or time-reversal symmetry breaking. Nevertheless, experimental evidence for magnetically induced WSMs is scarce. Here, using photoemission spectroscopy, we observe that the degeneracy of Bloch bands is already lifted in the paramagnetic phase of EuCd2As2. We attribute this effect to the itinerant electrons experiencing quasi-static and quasi-long-range ferromagnetic fluctuations. Moreover, the spin-nondegenerate band structure harbors a pair of ideal Weyl nodes near the Fermi level. Hence, we show that long-range magnetic order and the spontaneous breaking of time-reversal symmetry are not essential requirements for WSM states in centrosymmetric systems and that WSM states can emerge in a wider range of condensed matter systems than previously thought.

A compact ultrahigh vacuum scanning tunneling microscope with dilution refrigeration.

We have designed and built a scanning tunneling microscope (STM) setup for operation at millikelvin temperatures in an ultrahigh vacuum. A compact cryostat with an integrated dilution refrigerator has been built that allows measurements at a base temperature of 25 mK in the magnetic field up to 7.5 T with low mechanical and electronic noise. The cryostat is not larger than conventional helium bath cryostats (23 and 13 l of nitrogen and helium, respectively) so that the setup does not require a large experimental hall and fits easily into a standard lab space. Mechanical vibrations with running dilution circulation were kept below 1 pm/ Hz by mechanically decoupling the STM from the cryostat and the pumping system. All electronic input lines were low-pass filtered, reducing the electronic temperature to below 100 mK, as deduced from the quasiparticle peaks of superconducting aluminum. The microscope is optically accessible in the parked position, making sample and tip exchange fast and user-friendly. For measurement, the STM is lowered 60 mm down so that the sample ends in the middle of a wet superconducting magnetic coil.

Hysteresis and change of transition temperature in thin films of Fe{[Me2Pyrz]3BH}2, a new sublimable spin-crossover molecule.

Thin films of the spin-crossover (SCO) molecule Fe{[Me2Pyrz]3BH}2 (Fe-pyrz) were sublimed on Si/SiO2 and quartz substrates, and their properties investigated by X-ray absorption and photoemission spectroscopies, optical absorption, atomic force microscopy, and superconducting quantum interference device. Contrary to the previously studied Fe(phen)2(NCS)2, the films are not smooth but granular. The thin films qualitatively retain the typical SCO properties of the powder sample (SCO, thermal hysteresis, soft X-ray induced excited spin-state trapping, and light induced excited spin-state trapping) but present intriguing variations even in micrometer-thick films: the transition temperature decreases when the thickness is decreased, and the hysteresis is affected. We explain this behavior in the light of recent studies focusing on the role of surface energy in the thermodynamics of the spin transition in nano-structures. In the high-spin state at room temperature, the films have a large optical gap (∼5 eV), decreasing at thickness below 50 nm, possibly due to film morphology.

Magnon dispersion in thin magnetic films.

Although the dispersion of magnons has been measured in many bulk materials, few studies deal with the changes in the dispersion when the material is in the form of a thin film, a system that is of interest for applications. Here we review inelastic tunneling spectroscopy studies of magnon dispersion in Mn/Cu3Au(1 0 0) and present new studies on Co and Ni thin films on Cu(1 0 0). The dispersion in Mn and Co films closely follows the dispersion of bulk samples with negligible dependence on thickness. The lifetime of magnons depends slightly on film thickness, and decreases considerably as the magnon energy increases. In Ni/Cu(1 0 0) films the thickness dependence of dispersion is much more pronounced. The measurements indicate a considerable mode softening for thinner films. Magnon lifetimes decrease dramatically near the edge of the Brillouin zone due to a close proximity of the Stoner continuum. The experimental study is supported by first-principles calculations.

First glimpse of the soft x-ray induced excited spin-state trapping effect dynamics on spin cross-over molecules.

The dynamics of the soft x-ray induced excited spin state trapping (SOXIESST) effect of Fe(phen)2(NCS)2 (Fe-phen) powder have been investigated by x-ray absorption spectroscopy (XAS) using the total electron yield method, in a wide temperature range. The low-spin (LS) state is excited into the metastable high-spin (HS) state at a rate that depends on the intensity of the x-ray illumination it receives, and both the temperature and the intensity of the x-ray illumination will affect the maximum HS proportion that is reached. We find that the SOXIESST HS spin state transforms back to the LS state at a rate that is similar to that found for the light induced excited spin state trapping (LIESST) effect. We show that it is possible to use the SOXIESST effect in combination with the LIESST effect to investigate the influence of cooperative behavior on the dynamics of both effects. To investigate the impact of molecular cooperativity, we compare our results on Fe-phen with those obtained for Fe{[Me2Pyrz]3BH}2 (Fe-pyrz) powder, which exhibits a similar thermal transition temperature but with a hysteresis. We find that, while the time constant of the dynamic is identical for both molecules, the SOXIESST effect is less efficient at exciting the HS state in Fe-pyrz than in Fe-phen.

Direct observation of a highly spin-polarized organic spinterface at room temperature.

Organic semiconductors constitute promising candidates toward large-scale electronic circuits that are entirely spintronics-driven. Toward this goal, tunneling magnetoresistance values above 300% at low temperature suggested the presence of highly spin-polarized device interfaces. However, such spinterfaces have not been observed directly, let alone at room temperature. Thanks to experiments and theory on the model spinterface between phthalocyanine molecules and a Co single crystal surface, we clearly evidence a highly efficient spinterface. Spin-polarised direct and inverse photoemission experiments reveal a high degree of spin polarisation at room temperature at this interface. We measured a magnetic moment on the molecule's nitrogen π orbitals, which substantiates an ab-initio theoretical description of highly spin-polarised charge conduction across the interface due to differing spinterface formation mechanisms in each spin channel. We propose, through this example, a recipe to engineer simple organic-inorganic interfaces with remarkable spintronic properties that can endure well above room temperature.

A compact sub-Kelvin ultrahigh vacuum scanning tunneling microscope with high energy resolution and high stability.

We designed a scanning tunneling microscope working at sub-Kelvin temperatures in ultrahigh vacuum (UHV) in order to study the magnetic properties on the nanoscale. An entirely homebuilt three-stage cryostat is used to cool down the microscope head. The first stage is cooled with liquid nitrogen, the second stage with liquid (4)He. The third stage uses a closed-cycle Joule-Thomson refrigerator of a cooling power of 1 mW. A base temperature of 930 mK at the microscope head was achieved using expansion of (4)He, which can be reduced to ≈400 mK when using (3)He. The cryostat has a low liquid helium consumption of only 38 ml/h and standing times of up to 280 h. The fast cooling down of the samples (3 h) guarantees high sample throughput. Test experiments with a superconducting tip show a high energy resolution of 0.3 meV when performing scanning tunneling spectroscopy. The vertical stability of the tunnel junction is well below 1 pm (peak to peak) and the electric noise floor of tunneling current is about 6fA/√Hz. Atomic resolution with a tunneling current of 1 pA and 1 mV was achieved on Au(111). The lateral drift of the microscope at stable temperature is below 20 pm/h. A superconducting spilt-coil magnet allows to apply an out-of-plane magnetic field of up to 3 T at the sample surface. The flux vortices of a Nb(110) sample were clearly resolved in a map of differential conductance at 1.1 K and a magnetic field of 0.21 T. The setup is designed for in situ preparation of tip and samples under UHV condition.

Magnetoelectric coupling at metal surfaces.

Magnetoelectric coupling allows the magnetic state of a material to be changed by an applied electric field. To date, this phenomenon has mainly been observed in insulating materials such as complex multiferroic oxides. Bulk metallic systems do not exhibit magnetoelectric coupling, because applied electric fields are screened by conduction electrons. We demonstrate strong magnetoelectric coupling at the surface of thin iron films using the electric field from a scanning tunnelling microscope, and are able to write, store and read information to areas with sides of a few nanometres. Our work demonstrates that high-density, non-volatile information storage is possible in metals.

Impact on interface spin polarization of molecular bonding to metallic surfaces.

We have studied the repercussion of the molecular adsorption mechanism on the electronic properties of the interface between model nonmagnetic or magnetic metallic surfaces and metallo-organic phthalocyanines molecules (Pcs). Our intertwined x-ray absorption spectroscopy experiments and computational studies reveal that manganese Pc (MnPc) is physisorbed onto a Cu(001) surface and retains the electronic properties of a free molecule. On the other hand, MnPc is chemisorbed onto Co(001), leading to a dominant direct exchange interaction between the Mn molecular site and the Co substrate. By promoting an interfacial spin-polarized conduction state on the molecule, these interactions reveal an important lever to tailor the spintronic properties of hybrid organic-metallic interfaces.

Investigation of non-collinear spin states with scanning tunneling microscopy.

Most ferromagnetic and antiferromagnetic substances show a simple collinear arrangement of the local spins. Under certain circumstances, however, the spin configuration is non-collinear. Scanning tunneling microscopy with its potential atomic resolution is an ideal tool for investigating these complex spin structures. Non-collinearity can be due to topological frustration of the exchange interaction, due to relativistic spin-orbit coupling or can be found in excited states. Examples for all three cases are given, illustrating the capabilities of spin-polarized scanning tunneling microscopy.

Magnetic anisotropy and magnetization dynamics of individual atoms and clusters of Fe and Co on Pt(111).

The recently discovered giant magnetic anisotropy of single magnetic Co atoms raises the hope of magnetic storage in small clusters. We present a joint experimental and theoretical study of the magnetic anisotropy and the spin dynamics of Fe and Co atoms, dimers, and trimers on Pt(111). Giant anisotropies of individual atoms and clusters as well as lifetimes of the excited states were determined with inelastic scanning tunneling spectroscopy. The short lifetimes due to hybridization-induced electron-electron scattering oppose the magnetic stability provided by the magnetic anisotropies.

Spin wave dispersion on the nanometer scale.

Hot electrons injected into antiferromagnetic Mn layers from the tip of a low temperature scanning tunneling microscope have been used to determine the energies, lifetimes, and momenta of antiferromagnetic spin waves on the nanometer scale. The spin waves show a linear dispersion with a velocity of 160+/-10 meV A and lifetimes that scale linearly with energy in agreement with neutron scattering and theory. It is shown that the method is sensitive enough to detect the influence of surface anisotropies on the spin wave dispersion.

Noncollinear surface spin density by surface reconstruction in the alloy NiMn.

At the (001) surface of the alloy Ni(50)Mn(50), a noncollinear spin density is observed in real space by spin-polarized scanning tunneling microscopy. The spin density of individual atoms also varies in both size and direction as a function of bias voltage, indicating a noncollinearity in the energy domain. The noncollinearity is driven by a surface reconstruction which breaks the otherwise high surface symmetry. First-principles electronic-structure calculations support the experimental observations and evidence the interplay of reconstruction and spin-orbit coupling.

Revealing the 120 degrees antiferromagnetic Néel structure in real space: one monolayer Mn on Ag(111).

With spin-polarized scanning tunneling microscopy operating in the constant current mode, the 120 degrees antiferromagnetic Néel structure was found for a monolayer Mn on Ag(111) in both fcc and hcp stacking. The existence of structurally equivalent, but magnetically distinguished, Mn islands was observed. While both the fcc and hcp Mn islands display the frustrated spin structure, the orientations of their magnetic moments differ by 30 degrees possibly due to the spin-orbit coupling.

Mapping the surface spin structure of large unit cells: reconstructed mn films on Fe(001).

Using spin-polarized scanning tunneling microscopy with ring electrodes, the in-plane spin polarization of Mn on Fe(001) was measured. A large (square root 10 x 2 square root 10)R18.4 degrees reconstruction with a noncollinear spin structure was found. By combining maps of the spin polarization for two orthogonal in-plane directions, the vector field of the polarization in the unit cell could be constructed. The complex behavior is explained on the basis of the tendency of Mn to form antiferromagnetically coupled surface dimers.

Magnon excitation with spin-polarized scanning tunneling microscopy.

Using spin-polarized scanning tunneling microscopy, the local excitation of magnons in Fe and Co has been studied. A large cross section for magnon excitation was found for bulk Fe samples while for thin Co films on Cu(111) the cross section linearly scales with film thickness. Recording inelastic tunneling spectra with Fe coated W tips in a magnetic field, the magnonic nature of the excitation was proven. Magnon excitation could be detected without the use of a separating insulating layer opening up the possibility to directly study magnons in magnetic nanostructures via spin-polarized currents.

Step-induced frustration of antiferromagnetic order in Mn on Fe(001).

We studied the spin arrangement in ultrathin antiferromagnetic Mn films in contact with a ferromagnetic Fe(001) substrate using spin-polarized scanning tunneling microscopy. Mn shows a layerwise antiferromagnetic order on Fe(001). In regions where Mn overgrows Fe steps, a frustration of the antiferromagnetic order occurs which is similar to a 180 degrees domain wall. This topologically enforced frustration was studied as a function of Mn thickness. A linear increase of the width of the frustration region with the Mn thickness was found.

Direct observation of the single-domain limit of Fe nanomagnets by spin-polarized scanning tunneling spectroscopy.

We have investigated the magnetic structure of self-organized Fe islands on W(001) by means of spin-polarized scanning tunneling spectroscopy (Sp-STS). Single-domain, simple vortex, and distorted vortex states have been observed. The high resolution magnetic images were used to experimentally determine the single-domain limit. The experimental structures were compared with results of micromagnetic calculations confirming the ground state nature of the experimental configurations. The single-domain limit directly observed with Sp-STS is consistent with theoretical predictions.

Absence of zero-bias anomaly in spin-polarized vacuum tunneling in Co(0001).

In a joint experimental and theoretical study, we investigate the bias-voltage dependence of the tunnel magnetoresistance (TMR) through a vacuum barrier. The TMR observed by spin-polarized scanning tunneling microscopy between an amorphous magnetic tip and a Co(0001) sample is almost independent of the bias voltage at large tip-sample separations. Whereas qualitative understanding is achieved by means of the electronic surface structure of Co, the experimental findings are compared quantitatively with bias-voltage dependent first-principles calculations for ballistic tunneling. At small tip-sample separations, a pronounced minimum in the experimental TMR was found at +200 mV bias.