Search

Continuous solid electrolyte interface (SEI) formation remains the limiting factor of the lifetime of silicon nanoparticles (SiNPs) based negative electrodes. Methods that could provide clear diagnosis of the electrode degradation are of utmost necessity to streamline further developments. We demonstrate that electron energy-loss spectroscopy (EELS) in a scanning transmission electron microscope (STEM) can be used to quickly map SEI components and quantify LixSi alloys from single experiments, with resolutions down to 5 nm. Exploiting the low-loss part of the EEL spectrum allowed us to circumvent the degradation phenomena that have so far crippled the application of this technique on such beam-sensitive compounds. Our results provide unprecedented insight into silicon aging mechanisms in full cell configuration. We observe the morphology of the SEI to be extremely heterogeneous at the particle scale but with clear chemical evolutions with extended cycling coming from both SEI accumulation and a transition from lithium-rich carbonate-like compounds to lithium-poor ones. Thanks to the retrieval of several results from a single dataset, we were able to correlate local discrepancies in lithiation to the initial crystallinity of silicon as well as to the local SEI chemistry and morphology. This study emphasizes how initial heterogeneities in the percolating electronic network and the porosity affect SiNPs aggregates along cycling. These findings pinpoint the crucial role of an optimized formulation in silicon-based thick electrodes., Comment: Nano Letters, American Chemical Society, 2016

We have characterized a film of Ge_0.9Mn_0.1 forming self-organized nanocolumns perpendicular to the Ge substrate with high resolution scanning transmission electron microscopy combined with electron energy loss spectroscopy, and bulk magnetization and positive muon spin rotation and relaxation (muSR) measurements. The Mn-rich nanocolumns form a triangular lattice with no detectable Mn atoms in the matrix. They consist of cores surrounded by shells. The combined analysis of bulk magnetization and muSR data enables us to characterize the electronic and magnetic properties of both the cores and shells. The discovered phase separation of the columns between a core and a shell is probably relevant for other transition-metal doped semiconductors., Comment: 5 pages, 5 figures, and supplemental material

We developed the self-assembly of epitaxial submicrometer-sized face-centered-cubic (fcc) Co(111) dots using pulsed laser deposition. The dots display atomically-fl at facets, from which the ratios of surface and interface energies for fcc Co are deduced. Zero- field magnetic structures are investigated with magnetic force and lorentz microscopies, revealing vortex-based flux-closure patterns. A good agreement is found with micromagnetic simulations.

We report on the elaboration of germanium manganese nanostructured thin films and the measurement of their thermoelectric properties. We investigate the growth of Ge:Mn layers along with a thorough structural characterization of this materials at the nanoscale. The room temperature thermoelectric properties of these layers containing spherical inclusions are discussed regarding their potential as a model of "electron crystal phonon glass material". We show that the thermal conductivity can be decreased by a factor of 30, even if the electronic properties can be conserved as in the bulk. The thermoelectric performance ZT of such material is as high as 0.15 making them a promising thermoelectric p-type material for Ge related application.

In this letter, we first show electrical spin injection in the germanium conduction band at room temperature and modulate the spin signal by applying a gate voltage to the channel. The corresponding signal modulation agrees well with the predictions of spin diffusion models. Then by setting a temperature gradient between germanium and the ferromagnet, we create a thermal spin accumulation in germanium without any tunnel charge current. We show that temperature gradients yield larger spin accumulations than pure electrical spin injection but, due to competing microscopic effects, the thermal spin accumulation in germanium remains surprisingly almost unchanged under the application of a gate voltage to the channel., Comment: 7 pages, 3 figures

Electrical spin injection into semiconductors paves the way for exploring new phenomena in the area of spin physics and new generations of spintronic devices. However the exact role of interface states in spin injection mechanism from a magnetic tunnel junction into a semiconductor is still under debate. In this letter, we demonstrate a clear transition from spin accumulation into interface states to spin injection in the conduction band of $n$-Ge. We observe spin signal amplification at low temperature due to spin accumulation into interface states followed by a clear transition towards spin injection in the conduction band from 200 K up to room temperature. In this regime, the spin signal is reduced down to a value compatible with spin diffusion model. More interestingly, we demonstrate in this regime a significant modulation of the spin signal by spin pumping generated by ferromagnetic resonance and also by applying a back-gate voltage which are clear manifestations of spin current and accumulation in the germanium conduction band., Comment: 5 pages, 4 figures

We use extensive first principle simulations to show the major role played by interfaces in the mechanism of phase separation observed in semiconductor multifunctional materials. We make an analogy with the precipitation sequence observed in over-saturated AlCu alloys, and replace the Guinier-Preston zones in this new context. A new class of materials, the $\alpha$ phases, is proposed to understand the formation of the coherent precipitates observed in the GeMn system. The interplay between formation and interface energies is analyzed for these phases and for the structures usually considered in the literature. The existence of the alpha phases is assessed with both theoretical and experimental arguments.

We investigate in this paper the origin of perpendicular anisotropy in Co (1.6 nm)/Pt (3.0 nm) bilayers grown on alumina and annealed up to 650$^{\circ}$C. Above 350$^{\circ}$C, all layers exhibit perpendicular anisotropy. Then coercive fields increase linearly with annealing temperature following two different rates: 0.05 T/100$^{\circ}$C below 550$^{\circ}$C and 0.8 T/100$^{\circ}$C above. By making careful structural characterizations using x-ray diffraction and transmission electron microscopy, we demonstrate the presence of short range correlation of L1$_{1}$ type below 550$^{\circ}$C whereas above 550$^{\circ}$C, L1$_{0}$ chemical ordering is observed. We conclude that perpendicular anisotropy observed in Co/Pt bilayers grown on alumina and annealed may not only be due to interface anisotropy as usually invoked but also to CoPt alloying and chemical ordering that take place during post-growth annealing., Comment: submitted to Phys. Rev. B

A micromagnetic study of epitaxial micron-sized iron dots is reported through the analysis of Fresnel contrast in Lorentz Microscopy. Their use is reviewed and developed through analysis of various magnetic structures in such dots. Simple Landau configuration is used to investigate various aspects of asymmetric Bloch domain walls. The experimental width of such a complex wall is first derived and its value is discussed with the help of micromagnetic simulations. Combination of these two approaches enables us to define what is really extracted when estimating asymmetric wall width in Lorentz Microscopy. Moreover, quantitative data on the magnetization inside the dot is retrieved using phase retrieval as well as new informations on the degrees of freedom of such walls. Finally, it is shown how the existence and the propagation of a surface vortex can be characterized and monitored. This demonstrates the ability to reach a magnetic sensitivity a priori hidden in Fresnel contrast, based on an original image treatment and backed-up by the evaluation of contrasts obtained from micromagnetic simulations.

The production, observation and manipulation of very small objects is a tour de force, but these objects, which could infiltrate anywhere without being seen, may arouse suspicion. To assess the situation at best, we describe the activity of a nanoscience research institution, some of the methods used there, the spirit of its researchers and their attitude towards risk., Comment: article accept\'e pour publication dans les C.R. Physique. El\'ement d'un dossier 'Nanosciences et nanotechnologies: esp\'erances et inqui\'etudes". D'autres articles de ce dossier, ainsi que la version fran\c{c}aise de cet articles, seront \'egalement soumis \`a HAL

Uniform single layer graphene was grown on single-crystal Ir films a few nanometers thick which were prepared by pulsed laser deposition on sapphire wafers. These graphene layers have a single crystallographic orientation and a very low density of defects, as shown by diffraction, scanning tunnelling microscopy, and Raman spectroscopy. Their structural quality is as high as that of graphene produced on Ir bulk single crystals, i.e. much higher than on metal thin films used so far., Comment: To appear in Appl. Phys. Lett

We report on the structural properties of Ge_(1-x)Mn_x layers grown by molecular beam epitaxy. In these layers, nanocolumns with a high Mn content are embedded in an almost-pure Ge matrix. We have used grazing-incidence X-ray scattering, atomic force and transmission electron microscopy to study the structural properties of the columns. We demonstrate how the elastic deformation of the matrix (as calculated using atomistic simulations) around the columns, as well as the average inter-column distance can account for the shape of the diffusion around Bragg peaks., Comment: 9 pages, 7 figures

Graphene is attractive for spintronics due to its long spin life time and high mobility. So far only thick and polycrystalline slabs have been used as ferromagnetic electrodes. We report the growth of flat, epitaxial ultrathin Co films on graphene. These display perpendicular magnetic anisotropy in the thickness range 0.5-1nm, which is confirmed by theory. PMA, epitaxy and ultrathin thickness bring new perspectives for graphene-based spintronic devices such as the zero-field control of an arbitrary magnetization direction, band matching between electrodes and graphene, and interface effects such as Rashba and electric field control of magnetism.

We investigated with XMCD-PEEM magnetic imaging the magnetization reversal processes of N\'eel caps inside Bloch walls in self-assembled, micron-sized Fe(110) dots with flux-closure magnetic state. In most cases the magnetic-dependent processes are symmetric in field, as expected. However, some dots show pronounced asymmetric behaviors. Micromagnetic simulations suggest that the geometrical features (and their asymmetry) of the dots strongly affect the switching mechanism of the N\'eel caps., Comment: Proceeding for MMM-Intermag 2010 (Washington)

Changing the morphology of the growing surface and the nature of residual impurities in (Ge,Mn) layers - by using different substrates - dramatically changes the morphology of the ferromagnetic Mn-rich inclusions and the magnetotransport properties. We obtained p-type layers with nanocolumns, either parallel or entangled, and n-type layers with spherical clusters. Holes exhibit an anomalous Hall effect, and electrons exhibit a tunneling magnetoresistance, both with a clear dependence on the magnetization of the Mn-rich inclusions; holes exhibit orbital MR, and electrons show only the normal Hall effect, and an additional component of magnetoresistance due to weak localization, all three being independent of the magnetic state of the Mn rich inclusions. Identified mechanisms point to the position of the Fermi level of the Mn-rich material with respect to the valence band of germanium as a crucial parameter in such hybrid layers.

The structure of domain walls delimiting magnetic bubbles in L10 FePd thin layers is described on the basis of Lorentz transmission electron microscopy (LTEM) and multiscale magnetic simulations. Images obtained by high resolution LTEM show the existence of magnetization reversal areas inside domain walls, called vertical Bloch lines (VBLs). Combining these observations and multiscale simulations on various geometries, we can identify the structure of these VBLs, notably the presence or not of magnetic singularities.

We report the use of Lorentz microscopy to observe the domain wall structure during the magnetization process in FePd thin foils. We have focused on the magnetic structure of domain walls of bubble-shaped magnetic domains near saturation. Regions are found along the domain walls where the magnetization abruptly reverses. Multiscale magnetic simulations shown that these regions are vertical Bloch lines (VBL) and the different bubble shapes observed are then related to the inner structure of the VBLs. We were thus able to probe the presence of magnetic singularities as small as Bloch points in the inner magnetization of the domain walls.

Data storage relies on the handling of two states, called bits. The market of mass storage is currently still dominated by magnetic technology, hard disk drives for the broad public and tapes for massive archiving. In these devices each bit is stored in the form of the direction of magnetization of nanosized magnetic domains, i.e. areas of ferromagnetic materials displaying a uniform magnetization. While miniaturization is the conventional way to fuel the continuous increase of device density, disruptive solutions are also sought. To these pertain in recent years many fundamental studies no longer considering the magnetic domains themselves, but the manipulation of the domain walls (DWs) that separate such domains. Concepts of storage and logic based on the propagation of DWs along lithographically-patterned stripes have been patented, while many fundamental aspects of DW propagation deeply related to condensed matter physics are still hotly debated. If one now considers magnetic dots of submicrometer dimensions, the magnetization has a tendency to curl along the outer edges of the nanostructure to close its magnetic flux and thereby reduce its magnetostatic energy. Then both domains and DWs of well-defined geometries arise, whose combined manipulation has been proposed as a multilevel magnetic storage scheme..., Comment: To appear in Elettra Sincrotrone Highlights 2008-2009

Dimensionality cross-over is a classical topic in physics. Surprisingly it has not been searched in micromagnetism, which deals with objects such as domain walls (2D) and vortices (1D). We predict by simulation a second-order transition between these two objects, with the wall length as the Landau parameter. This was conrmed experimentally based on micron-sized ux-closure dots.

Thin film alloys with perpendicular anisotropy were studied using Lorentz Transmission Electron Microscopy (LTEM). This work focuses on the configuration of domain walls and demonstrates the suitability and accuracy of LTEM for the magnetic characterisation of perpendicular magnetic anisotropy materials. Thin films of chemically ordered ($\unit{L1_0}$) FePd alloys were investigated by micro-magnetic modelling and LTEM phase retrieval approach. The different components of magnetization described by the modeling were studied on experimental images and confirmed by LTEM contrast simulation. Furthermore, quantitative measurements of magnetic induction inside the domain walls were made by using an original method to separate the electrical and magnetical contributions to the phase information. Irregularities were also observed along the domain walls which could play a major role during the magnetization processes., Comment: Ultramicroscopy (2009) In press

Off-axis electron holography was used to observe and quantify the magnetic microstructure of a perpendicular magnetic anisotropic (PMA) recording media. Thin foils of PMA materials exhibit an interesting up and down domain configuration. These domains are found to be very stable and were observed at the same time with their stray field, closing magnetic flux in the vacuum. The magnetic moment can thus be determined locally in a volume as small as few tens of cubic nanometers.

Lorentz transmission electron microscopy (LTEM) combined with in-situ magnetizing experiments is a powerful tool for the investigation of the magnetization of the reversal process at the micron scale. We have implemented this tool on a conventional transmission electron microscope (TEM) to study the exchange anisotropy of a polycrystalline Co35Fe65/NiMn bilayer. Semi-quantitative maps of the magnetic induction were obtained at different field values by the differential phase contrast (DPC) technique adapted for a TEM (SIDPC). The hysteresis loop of the bilayer has been calculated from the relative intensity of magnetic maps. The curve shows the appearance of an exchange-bias field reveals with two distinct reversal modes of the magnetization: the first path corresponds to a reversal by wall propagation when the applied field is parallel to the anisotropy direction whereas the second is a reversal by coherent rotation of magnetic moments when the field is applied antiparallel to unidirectional anisotropy direction.

While achieving high Curie temperatures (above room temperature) in diluted magnetic semiconductors remains a challenge in the case of well controlled homogeneous alloys, several systems characterized by a strongly inhomogeneous incorporation of the magnetic component appear as promising. Incorporation of manganese into germanium drastically alters the growth conditions, and in certain conditions of low temperature Molecular Beam Epitaxy it leads to the formation of well organized nanocolumns of a Mn-rich material, with a crystalline structure in epitaxial relationship with the Mn-poor germanium matrix. A strong interaction between the Mn atoms in these nanocolums is demonstrated by x-ray absorption spectroscopy, giving rise to a ferromagnetic character as observed through magnetometry and x-ray magnetic circular dichroism. Most interesting, intense magneto-transport features are observed on the whole structure, which strongly depend on the magnetic configuration of the nanocolumns., Comment: SPIE Optics & Photonics Symposium, San Diego : \'Etats-Unis d'Am\'erique (2008)

While magnetic hysteresis usually considers magnetic domains, the switching of the core of magnetic vortices has recently become an active topic. We considered Bloch domain walls, which are known to display at the surface of thin films flux-closure features called N\'eel caps. We demonstrated the controlled switching of these caps under a magnetic field, occurring via the propagation of a surface vortex. For this we considered flux-closure states in elongated micron-sized dots, so that only the central domain wall can be addressed, while domains remain unaffected., Comment: 4 pages, 3 figures

We report on the structural and magnetic properties of thin Ge(1-x)Mn(x)films grown by molecular beam epitaxy (MBE) on Ge(001) substrates at temperatures (Tg) ranging from 80deg C to 200deg C, with average Mn contents between 1 % and 11 %. Their crystalline structure, morphology and composition have been investigated by transmission electron microscopy (TEM), electron energy loss spectroscopy and x-ray diffraction. In the whole range of growth temperatures and Mn concentrations, we observed the formation of manganese rich nanostructures embedded in a nearly pure germanium matrix. Growth temperature mostly determines the structural properties of Mn-rich nanostructures. For low growth temperatures (below 120deg C), we evidenced a two-dimensional spinodal decomposition resulting in the formation of vertical one-dimensional nanostructures (nanocolumns). Moreover we show in this paper the influence of growth parameters (Tg and Mn content) on this decomposition i.e. on nanocolumns size and density. For temperatures higher than 180deg C, we observed the formation of Ge3Mn5 clusters. For intermediate growth temperatures nanocolumns and nanoclusters coexist. Combining high resolution TEM and superconducting quantum interference device magnetometry, we could evidence at least four different magnetic phases in Ge(1-x)Mn(x) films: (i) paramagnetic diluted Mn atoms in the germanium matrix, (ii) superparamagnetic and ferromagnetic low-Tc nanocolumns (120 K < Tc < 170 K), (iii) high-Tc nanocolumns (Tc> 400 K) and (iv) Ge3Mn5 clusters., Comment: 10 pages 2 colonnes revTex formatted