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Terahertz time-domain conductivity measurements in 2 to 100 nm thick iron films resolve the femtosecond time delay between applied electric fields and resulting currents. This current response time decreases from 29 fs for thickest films to 7 fs for the thinnest films. The macroscopic response time is not strictly proportional to the conductivity. This excludes the existence of a single relaxation time universal for all conduction electrons. We must assume a distribution of microscopic momentum relaxation times. The macroscopic response time depends on average and variation of this distribution; the observed deviation between response time and conductivity scaling corresponds to the scaling of the variation. The variation of microscopic relaxation times depends on film thickness because electrons with different relaxation times are affected differently by the confinement since they have different mean free paths., Comment: 9 pages, 6 figures

Electrically manipulating the quantum properties of nano-objects, such as atoms or molecules, is typically done using scanning tunnelling microscopes and lateral junctions. The resulting nanotransport path is well established in these model devices. Societal applications require transposing this knowledge to nano-objects embedded within vertical solid-state junctions, which can advantageously harness spintronics to address these quantum properties thanks to ferromagnetic electrodes and high-quality interfaces. The challenge here is to ascertain the device's effective, buried nanotransport path, and to electrically involve these nano-objects in this path by shrinking the device area from the macro- to the nano-scale while maintaining high structural/chemical quality across the heterostructure. We've developed a low-tech, resist- and solvent-free technological process that can craft nanopillar devices from entire in-situ grown heterostructures, and use it to study magnetotransport between two Fe and Co ferromagnetic electrodes across a functional magnetic CoPc molecular layer. We observe how spin-flip transport across CoPc molecular spin chains promotes a specific magnetoresistance effect, and alters the nanojunction's magnetism through spintronic anisotropy. In the process, we identify three magnetic units along the effective nanotransport path thanks to a macrospin model of magnetotransport. Our work elegantly connects the until now loosely associated concepts of spin-flip spectroscopy, magnetic exchange bias and magnetotransport due to molecular spin chains, within a solid-state device. We notably measure a 5.9meV energy threshold for magnetic decoupling between the Fe layer's buried atoms and those in contact with the CoPc layer forming the so-called 'spinterface'. This provides a first insight into the experimental energetics of this promising low-power information encoding unit.

To mitigate climate change, our global society is harnessing direct (solar irradiation) and indirect (wind/water flow) sources of renewable electrical power generation. Emerging direct sources include current-producing thermal gradients in thermoelectric materials, while quantum physics-driven processes to convert quantum information into energy have been demonstrated at very low temperatures. The magnetic state of matter, assembled by ordering the electron's quantum spin property, represents a sizeable source of built-in energy. We propose to create a direct source of electrical power at room temperature (RT) by utilizing magnetic energy to harvest thermal fluctuations on paramagnetic (PM) centers. Our spin engine rectifies current fluctuations across the PM centers' spin states according to the electron spin by utilizing so-called 'spinterfaces' with high spin polarization. As a rare experimental event, we demonstrate how this path can generate 0.1nW at room temperature across a 20 micron-wide spintronic device called the magnetic tunnel junction, assembled using commonplace Co, C and MgO materials. The presence of this path in our experiment, which also generates very high spintronic performance, is confirmed by analytical and ab-initio calculations. Device downscaling, and the ability for other materials systems than the spinterface to select a transport spin channel at RT widens opportunities for routine device reproduction. The challenging control over PM centers within the tunnel barrier's nanotransport path may be addressed using oxide- and organic-based nanojunctions. At present densities in MRAM products, this spin engine could lead to 'always-on' areal power densities well beyond that generated by solar irradiation on earth. Further developing this concept can fundamentally alter our energy-driven society's global economic, social and geopolitical constructs.

The organic spinterface describes the spin-polarized properties that develop, due to charge transfer, at the interface between a ferromagnetic metal (FM) and the molecules of an organic semiconductor. Yet, if the latter is also magnetic (e.g. molecular spin chains), the interfacial magnetic coupling can generate complexity within magnetotransport experiments. Also, assembling this interface may degrade the properties of its constituents (e.g. spin crossover or non-sublimable molecules). To circumvent these issues, one can separate the molecular and FM films using a less reactive nonmagnetic metal (NM). Spin-resolved photoemission spectroscopy measurements on the prototypical system Co(001)//Cu/Mnphthalocyanine (MnPc) reveal that the Cu/MnPc spinterface atop ferromagnetic Co is highly spin-polarized at room temperature, up to Cu spacer thicknesses of at least 10 monolayers. Ab-initio theory describes a spin polarization of the topmost Cu layer after molecular hybridization that can be accompanied by magnetic hardening effects. This spinterface's unexpected robustness paves the way for 1) integrating electronically fragile molecules within organic spinterfaces, and 2) manipulating molecular spin chains using the well-documented spin transfer torque properties of the FM/NM bilayer., Comment: 16 pages. Submitted

The quantum mechanical tunnelling process conserves the quantum properties of the particle considered. As applied to solid-state tunnelling (SST), this physical law was verified, within the field of spintronics, regarding the electron spin in early experiments across Ge tunnel barriers, and in the 90s across Al2O3 barriers. The conservation of the quantum parameter of orbital occupancy, as grouped into electronic symmetries, was observed in the '00s across MgO barriers, followed by SrTiO3 (STO). Barrier defects, such as oxygen vacancies, partly conserve this electronic symmetry. In the solid-state, an additional subtlety is the sign of the charge carrier: are holes or electrons involved in transport? We demonstrate that SST across MgO magnetic tunnel junctions (MTJs) with a large resistance-area (RA) product involves holes by examining how shifting the MTJ's Fermi level alters the ensuing barrier heights defined by the barrier's oxygen vacancies. In the process, we consolidate the description of tunnel barrier heights induced by specific oxygen-vacancy induced localized states. Our work opens prospects to understand the concurrent observation of high TMR and spin transfer torque across MgO-based nanopillars., Comment: 8 pages including 2 figures

Terahertz electromagnetic radiation is extremely useful for numerous applications such as imaging and spectroscopy. Therefore, it is highly desirable to have an efficient table-top emitter covering the 1-to-30-THz window whilst being driven by a low-cost, low-power femtosecond laser oscillator. So far, all solid-state emitters solely exploit physics related to the electron charge and deliver emission spectra with substantial gaps. Here, we take advantage of the electron spin to realize a conceptually new terahertz source which relies on tailored fundamental spintronic and photonic phenomena in magnetic metal multilayers: ultrafast photo-induced spin currents, the inverse spin-Hall effect and a broadband Fabry-P\'erot resonance. Guided by an analytical model, such spintronic route offers unique possibilities for systematic optimization. We find that a 5.8-nm-thick W/CoFeB/Pt trilayer generates ultrashort pulses fully covering the 1-to-30-THz range. Our novel source outperforms laser-oscillator-driven emitters such as ZnTe(110) crystals in terms of bandwidth, terahertz-field amplitude, flexibility, scalability and cost., Comment: 18 pages, 10 figures

The research field of spintronics has sought, over the past 25 years and through several materials science tracks, a source of highly spin-polarized current at room temperature. Organic spinterfaces, which consist in an interface between a ferromagnetic metal and a molecule, represent the most promising track as demonstrated for a handful of interface candidates. How general is this effect? We deploy topographical and spectroscopic techniques to show that a strongly spin-polarized interface arises already between ferromagnetic cobalt and mere carbon atoms. Scanning tunneling microscopy and spectroscopy show how a dense semiconducting carbon film with a low band gap of about 0.4 eV is formed atop the metallic interface. Spin-resolved photoemission spectroscopy reveals a high degree of spin polarization at room temperature of carbon-induced interface states at the Fermi energy. From both our previous study of cobalt/phthalocyanine spinterfaces and present x-ray photoemission spectroscopy studies of the cobalt/carbon interface, we infer that these highly spin-polarized interface states arise mainly from sp2-bonded carbon atoms. We thus demonstrate the molecule-agnostic, generic nature of the spinterface formation.

Ultrafast magnetization dynamics induced by femtosecond laser pulses have been measured in ferrimagnetic Co0.8Gd0.2, Co.74Tb.26 and Co.86Tb.14 alloys. Using element sensitivity of X-ray magnetic circular dichroism at the Co L3, Tb M5 and Gd M5 edges we evidence that the demagnetization dynamics is element dependent. We show that a thermalization time as fast as 280 fs is observed for the rare-earth in the alloy, when the laser excited state temperature is below the compensation temperature. It is limited to 500 fs when the laser excited state temperature is below the Curie temperature (Tc). We propose critical spin fluctuations in the vicinity of TC as the mechanism which reduces the demagnetization rates of the 4f electrons in transition-metal rare-earth alloys whereas at any different temperature the limited demagnetization rates could be avoided., Comment: 11 pages, 4 figures

The design of large-scale electronic circuits that are entirely spintronics-driven requires a current source that is highly spin-polarised at and beyond room temperature, cheap to build, efficient at the nanoscale and straightforward to integrate with semiconductors. Yet despite research within several subfields spanning nearly two decades, this key building block is still lacking. We experimentally and theoretically show how the interface between Co and phthalocyanine molecules constitutes a promising candidate. 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 molecules's nitrogen pi orbitals, which substantiates an ab-initio theoretical description of highly spin-polarised charge conduction across the interface due to differing spinterface formation mechanims 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.

The impact of oxygen vacancies on local tunneling properties across rf-sputtered MgO thin films was investigated by optical absorption spectroscopy and conducting atomic force microscopy. Adding O$_2$ to the Ar plasma during MgO growth alters the oxygen defect populations, leading to improved local tunneling characteristics such as a lower density of current hotspots and a lower tunnel current amplitude. We discuss a defect-based potential landscape across ultrathin MgO barriers., Comment: 4 pages, 4 figures

We report on the growth by evaporation under high vacuum of high-quality thin films of Fe(phen)2(NCS)2 (phen=1,10-phenanthroline) that maintain the expected electronic structure down to a thickness of 10 nm and that exhibit a temperature-driven spin transition. We have investigated the current-voltage characteristics of a device based on such films. From the space charge-limited current regime, we deduce a mobility of 6.5x10-6 cm2/V?s that is similar to the low-range mobility measured on the widely studied tris(8-hydroxyquinoline)aluminium organic semiconductor. This work paves the way for multifunctional molecular devices based on spin-crossover complexes.

Using the spectroscopies based upon x-ray absorption, we have studied the structural and magnetic properties of Zn$_{1-x}$Co$_{x}$O films ($x$ = 0.1 and 0.25) produced by reactive magnetron sputtering. These films show ferromagnetism with a Curie temperature $T_{\mathrm{C}}$ above room temperature in bulk magnetization measurements. Our results show that the Co atoms are in a divalent state and in tetrahedral coordination, thus substituting Zn in the wurtzite-type structure of ZnO. However, x-ray magnetic circular dichroism at the Co \textit{L}$_{2,3}$ edges reveals that the Co 3\textit{d} sublattice is paramagnetic at all temperatures down to 2 K, both at the surface and in the bulk of the films. The Co 3\textit{d} magnetic moment at room temperature is considerably smaller than that inferred from bulk magnetisation measurements, suggesting that the Co 3\textit{d} electrons are not directly at the origin of the observed ferromagnetism., Comment: 5 pages, 5 figures