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While extensive work has been dedicated to the measurement of the demagnetization time following an ultra-short laser pulse, experimental studies of its underlying microscopic mechanisms are still scarce. In transition metal ferromagnets, one of the main mechanism is the spin-flip of conduction electrons driven by electron-phonon scattering. Here, we present an original experimental method to monitor the electron-phonon mediated spin-flip scattering rate in nickel through the stringent atomic symmetry selection rules of x-ray emission spectroscopy. Increasing the phonon population leads to a waning of the 3d → 2p3/2 decay peak intensity, which reflects an increase of the angular momentum transfer scattering rate attributed to spin-flip. We find a spin relaxation time scale in the order of 50 fs in the 3d-band of nickel at room temperature, while consistantly, no such peak evolution is observed for the diamagnetic counterexample copper, using the same method.

Scientific reports 11(1), 1883 (2021). doi:10.1038/s41598-021-81177-9, How different microscopic mechanisms of ultrafast spin dynamics coexist and interplay is not only relevant for the development of spintronics but also for the thorough description of physical systems out-of-equilibrium. In pure crystalline ferromagnets, one of the main microscopic mechanism of spin relaxation is the electron-phonon (el-ph) driven spin-flip, or Elliott-Yafet, scattering. Unexpectedly, recent experiments with ferro- and ferrimagnetic alloys have shown different dynamics for the different sublattices. These distinct sublattice dynamics are contradictory to the Elliott-Yafet scenario. In order to rationalize this discrepancy, it has been proposed that the intra- and intersublattice exchange interaction energies must be considered in the microscopic demagnetization mechanism, too. Here, using a temperature-dependent x-ray emission spectroscopy (XES) method, we address experimentally the element specific el-ph angular momentum transfer rates, responsible for the spin-flips in the respective (sub)lattices of Fe20Ni80, Fe50Ni50 and pure nickel single crystals. We establish how the deduced rate evolution with the temperature is linked to the exchange coupling constants reported for different alloy stoichiometries and how sublattice exchange energies threshold the related el-ph spin-flip channels. Thus, these results evidence that the Elliott-Yafet spin-flip scattering, thresholded by sublattice exchange energies, is the relevant microscopic process to describe sublattice dynamics in alloys and elemental magnetic systems., Published by Macmillan Publishers Limited, part of Springer Nature, [London]

The electron–phonon scattering is one of the main microscopic mechanisms responsible for the spin-flip in the transient state of ultrafast demagnetization. Here, we present an experimental determination of the temperature-dependent electron–phonon scattering rate in Gd. Using a static x-ray emission spectroscopy method, where the reduction of the decay peak intensities when increasing the temperature is quantified, we measure independently the electron-phonon scattering rate for the 5d and the 4f electrons. We deduce the temperature dependence of scattering for the 5d electrons, while no effect on the phonon population is observed for the 4f electrons. Our results suggest that the ultrafast magnetization dynamics in Gd is triggered by the spin-flip in the 5d electrons. We also evidence the existence of a temperature threshold, above which spin-flip scattering of the 5d electrons takes place. We deduce that during the transient state of ultrafast demagnetization, the exchange energy between 5d electrons has to be overcome before the microscopic electron-phonon scattering process can occur.

We present a scanning tunneling microscopy study of Fe and Co intercalated at the graphene–Ir(111) interface. In the case of Fe, we investigate the morphology of the surface with respect to the annealing temperature, which activates the intercalation, and as a function of coverage. By increasing the coverage we show that it is possible to intercalate multilayers at the interface. Finally, we demonstrate that the successive intercalation of Co and Fe for the same sample leads to distinct adjacent intercalation areas.

We investigate molecule-molecule, as well as molecule-substrate, interactions of phthalocyanine molecules deposited on graphene. In particular, we show how to tune the self-assembly of molecular lattices in two dimensions by intercalation of transition metals between graphene and Ir(111): modifying the surface potential of the graphene layer via intercalation leads to the formation of square, honeycomb, or Kagome lattices. Finally, we demonstrate that such surface induced molecular lattices are stable even at room temperature.

This Feature Article reports on the controlled formation and structure-functionality aspects of vacuum-deposited self-assembled organic and metal-organic networks at metal surfaces using ditopic linear and nonlinear molecular bricks, namely di-carbonitrile polyphenyls. Surface confined supramolecular organization of linear aromatic molecules leads to a fascinating variety of open networks. Moreover, cobalt-directed assembly of the same linear linkers reveals highly regular, open honeycomb networks with tunable pore sizes representing versatile templates for the organization of molecular guests or metal clusters and the control of supramolecular dynamers. In addition, the 2D nanopore organic networks act as arrays of quantum corrals exhibiting confinement of the surface-electronic states of the metallic substrate. A reduction of the linker symmetry leads to the formation of disordered, glassy coordination networks, which represent a structural model for amorphous materials.

We describe scanning tunneling spectroscopy (STS) measurements performed on individual cobalt (Co) atoms deposited onto backgated graphene devices. We find that Co adatoms on graphene can be ionized by either the application of a global backgate voltage or by the application of a local electric field from a scanning tunneling microscope (STM) tip. Large screening clouds are observed to form around Co adatoms ionized in this way, and we observe that some intrinsic graphene defects display a similar behavior. Our results provide new insight into charged impurity scattering in graphene, as well as the possibility of using graphene devices as chemical sensors., Comment: 19 pages, 4 figures

The self-assembly of sexiphenyl-dicarbonitrile molecules on the Ag(111) surface is investigated using low-temperature scanning tunneling microscopy (STM) in ultrahigh vacuum. Several nanoporous networks with varying symmetry and pore size coexist on the surface after submonolayer deposition at room temperature. The different rectangular, rhombic, and kagom shaped phases are commensurate with the Ag(111) substrate and extend over micrometer-sized domains separated by step edges. All phases are chiral and have very similar formation energetics. We attribute this to common construction principles: the approximately flat-lying polyphenyl backbones following high-symmetry directions of the substrate, the epitaxial fit and the nodal motif composed of CN end groups laterally attracted by phenyl hydrogens. Close to saturation coverage, a single dense-packed phase prevails with all molecules aligned parallel within one domain. Our results demonstrate that porous networks of different complexity can evolve by the self-assembly of only one molecular species on a metal surface.

We present a systematic study of metal-organic honeycomb lattices assembled from simple ditopic molecular bricks and Co atoms on Ag(111). This approach enables us to fabricate size- and shape-controlled open nanomeshes with pore dimensions up to 5.7 nm. The networks are thermally robust while extending over microm2 large areas as single domains. They are shape resistant in the presence of further deposited materials and represent templates to organize guest species and realize molecular rotary systems.

Scanning tunneling microscopy (STM) has been used to investigate the nucleation and stability of iron clusters on the Al2O3/Ni3Al (111) surface as a function of coverage and annealing temperature. We show that atomic beam deposition of iron leads to hexagonally ordered cluster arrangements with a distance of 24 angstrom between the clusters evidencing the template effect of the alumina film. The shape of the iron clusters is two-dimensional (2D) at deposition temperatures from 130 K to 160 K and three-dimensional (3D) at 300 K. However, the 2D iron clusters grown between 130 K and 160 K are stable up to 350 K. (c) 2006 Elsevier B.V. All rights reserved.

The lateral variation of the tunnel magnetoresistance (TMR) of a graphene-based vertical heterostructure is studied by spin-polarized scanning tunneling microscopy (SP–STM) using an Fe-coated probe tip. The well-defined heterostructure is obtained by the intercalation of a magnetic Fe monolayer at the graphene/Ir(1 1 1) interface. Its structure is characterized by a moire pattern with a high corrugation. In contrast to the Fe / Ir(1 1 1) surface, graphene/Fe / Ir(1 1 1) exhibits ferromagnetic order with an out-of-plane easy magnetization axis. At the nanometer scale, our experiments reveal that the moire pattern induces a lateral variation of the TMR, which reaches 80%. The measured TMR at valleys of the moire pattern is higher than at hills. We interpret this modulation in terms of a different hybridization between graphene and Fe at valleys and hills due to a different graphene–Fe distance at these sites, which leads to a different transmission of spin-polarized states.

A surface-supported open metal-organic nanomesh featuring a 24 nm(2) cavity size and extending to mum domains was fabricated by Co-directed assembly of para-hexaphenyl-dicarbonitrile linker molecules in two dimensions. The metallosupramolecular lattice is thermally robust and resides fully commensurate on the employed Ag(111) substrate as directly verified by high-resolution scanning tunneling microscopy observations.

Using spin-polarized scanning tunneling microscopy and density functional theory, we have studied the structural and magnetic properties of cobalt-intercalated graphene on Ir(111). The cobalt forms monolayer islands being pseudomorphic with the Ir(111) beneath the graphene. The strong bonding between graphene and cobalt leads to a high corrugation within the Moir\'e pattern which arises due to the lattice mismatch between the graphene and the Co on Ir(111). The intercalation regions exhibit an out-of-plane easy axis with an extremely high switching field, which surpasses the significant values reported for uncovered cobalt islands on Ir(111). Within the Moir\'e unit cell of the intercalation regions, we observe a site-dependent variation of the local effective spin polarization. State-of-the-art first-principles calculations show that the origin of this variation is a site-dependent magnetization of the graphene: At top sites the graphene is coupled ferromagnetically to the cobalt underneath, while it is antiferromagnetically coupled at fcc and hcp sites.

The use of boron nitride (BN) as a substrate for graphene nanodevices has attracted much interest since the recent report that BN greatly improves the mobility of charge carriers in graphene compared to standard SiO(2) substrates. We have explored the local microscopic properties of graphene on a BN substrate using scanning tunneling microscopy. We find that BN substrates result in extraordinarily flat graphene layers that display microscopic Moiré patterns arising from the relative orientation of the graphene and BN lattices. Gate-dependent dI/dV spectra of graphene on BN exhibit spectroscopic features that are sharper than those obtained for graphene on SiO(2). We observe a significant reduction in local microscopic charge inhomogeneity for graphene on BN compared to graphene on SiO(2).

We find the scanning tunneling spectra of backgated graphene monolayers to be significantly altered by many-body excitations. Experimental features in the spectra arising from electron-plasmon interactions show carrier density dependence, distinguishing them from density-independent electron-phonon features. Using a straightforward model, we are able to calculate theoretical tunneling spectra that agree well with our data, providing insight into the effects of many-body interactions on the lifetime of graphene quasiparticles.

This Feature Article reports on the controlled formation and structure-functionality aspects of vacuum-deposited self-assembled organic and metal-organic networks at metal surfaces using ditopic linear and nonlinear molecular bricks, namely di-carbonitrile polyphenyls. Surface confined supramolecular organization of linear aromatic molecules leads to a fascinating variety of open networks. Moreover, cobalt-directed assembly of the same linear linkers reveals highly regular, open honeycomb networks with tunable pore sizes representing versatile templates for the organization of molecular guests or metal clusters and the control of supramolecular dynamers. In addition, the 2D nanopore organic networks act as arrays of quantum corrals exhibiting confinement of the surface-electronic states of the metallic substrate. A reduction of the linker symmetry leads to the formation of disordered, glassy coordination networks, which represent a structural model for amorphous materials.

A detailed structural analysis of the surface supported self-assembly of terphenyl-4,4′′-dicarbonitrile molecules (NC−Ph3−CN) linked by Co adatoms on Ag(111) reveals different surface patterns depending on the constraints applied to the system. Without constraints, i.e., sufficient mobility and absence of space limitations at the surface, extended regular honeycomb nanomeshes are formed. On the basis of high-resolution scanning tunneling microscopy images, an atomistic model is derived showing the crystallographic orientation of the molecules and a commensurate alignment of the honeycomb networks, which exist in two rotational domains on the Ag(111) atomic lattice. For Co deficiency, an additional star-like Co-directed motif has been identified, and fully disordered networks are present if space limitations are imposed. In these cases, nodal motifs exist showing between 3- and 6-fold coordination of Co centers.

Regularly sized Fe and Co nanostructures are created using two-dimensional metal-organic honeycomb lattices as templates. They consist of dicarbonitrile-polyphenyl molecules coordinated to Co centers on Ag(111). Subsequently deposited Fe or Co atoms nucleate clusters at specific sites on top of the metal-organic lattices while leaving their hexagonal pores empty. Choosing the deposition temperature, one can selectively decorate the molecules (120K) or the Co coordination nodes (190K) with Fe. The distance between the Fe and Co clusters and their shape can be adjusted through the lattice constant of the template by varying the number of phenyl rings in the molecules.