van der Waals Epitaxy of Co10–xZn10–yMnx+y Thin Films: Chemical Composition Engineering and Magnetic Properties

Topologically protected magnetic skyrmions have raised interest for future spintronics applications. One of the main challenges is the synthesis of room temperature skyrmion-hosting materials that are compatible with thin-film technology. We present an approach to produce strain-free epitaxial thin films of Co10–xZn10–yMnx+y using molecular beam epitaxy. Bulk Co10–xZn10–yMnx+y is known to host skyrmions at room temperature for specific composition ratios. Our substrate consists of graphene on oxidized silicon. The van der Waals interactions of the grown material with graphene prevents covalent bonding and corresponding strain. We show how defects in the graphene foster nucleation that results in three different kinds of morphologies: islands, columns, and merged films. Susceptibility measurements suggest a phase transition close to room temperature. We detect up to three spin waves resonances suggesting relatively low magnetic damping. This growth technique opens a new route for the integration of complex alloys and skyrmionic device concepts with silicon electronics.

Synthesis, structural and magnetic characterization of thin films of the chiral magnets CoZnMn and FeGe

Skyrmions are topologically protected nanometer-sized magnetic vortices that have sparked interest for future spintronics applications aiming at high-density, high-speed and low-power consuming magnetic memory devices. One type of skyrmions appears in non-centrosymmetric materials with spin-orbit coupling. Bulk materials such as FeGe and CoZnMn have been in the focus of recent research as they host skyrmion lattices near or above room temperature. The interest in thin-film materials has immensely increased as they promise better control of skyrmions. The main challenges are the synthesis of skyrmion-hosting materials with high critical temperatures and the compatibility with Si-based thin-film technologies. Currently most of the studied thin films do not exhibit the relevant properties. It has been argued that strain and defects related to the lattice mismatch inhibit the skyrmion phase.Here we present novel approaches to synthesize skyrmion-hosting thin films based on FeGe and CoZnMn: 1) the crystallization of an amorphous thin film on a vdW substrate (commercial graphene), 2) van der Waals (vdW) growth on graphene as a substrate to achieve a strain- and defect-free growth of the overlayer.Sputtered FeGe layers were obtained on graphene on oxidized silicon substrates and annealed via rapid thermal (RTA) and flash lamp annealing (FLA). The goal was to use these annealing techniques to guide the material to the temperature/composition window of the cubic phase. For this, we varied the thin film thickness, Fe:Ge ratio, pre-heating and annealing temperature. The thin film temperature during the FLA was studied through heat transfer simulations. The experiments uncovered the long annealing time via RTA with a capping layer leads to 4 types of morphology: islands, discs, individual crystals and crystals on discs. The sub-second annealing via FLA led to the polycrystalline thin film formation. The obtained materials contain hexagonal and cubic FeGe, Fe-rich phases, pure Ge and Fe oxides analysed by Raman spectroscopy and X-ray diffraction. We provide Raman vibrational modes and the symmetry description from first-principles calculations for FeGex with x=1, 1.5 and 2 to fast and locally characterize thin films and microstructures.Molecular beam epitaxy was used to grow CoZnMn thin films of different stoichiometries on graphene on oxidized Si. It has been found in bulk crystals that the critical temperature can be systematically engineered beyond room temperature by tuning the composition. We report on the structural, compositional and magnetic properties of Co10-xZn10-yZnx+y (0

EPFL2021

Ordered nanostructures on silicon substrates

Jelena Vukajlovic Plestina

Silicon is today the main material used in electronics. It is a very advanced and mature technology. It is therefore clear that new technological concepts and materials should be introduced through the integration on the silicon platform. III-V semiconductors, such as GaAs and InAs, are high performance semiconductors, with direct bandgap and high carrier mobility, what makes them very prominent candidates for future electronics and optoelectronics. Lattice, thermal and polarity mismatch have been for decades limiting their integration on Si in the form of thin film technology. The nanowire geometry brings new prospects in this direction by reducing the contact area between mismatched materials,. Now, while growth of defect-free III-V structures on silicon is important, use in applications requires the nanostructures to be placed deterministically following a certain design/order. In this thesis we have studied different mechanisms to obtain ordered nanostructures on a silicon substrate, with the goal of increasing its functionality. The core part of this work was dedicated to the integration of III-V nanowires on Si in the formof ordered arrays. We have considered both GaAs and InAs nanowires. This process has several requirements: substrate fabrication and the growth process should be CMOS compatible, nanowires within the arrays should be grown vertically with a yield close to 100% and nanowires should be clones-looking and performing the same. An additional point to consider is that the fabrication process should be compatible with large scale techniques. The substrate requirements for obtaining ordered arrays of Ga-assisted GaAs nanowires on silicon were identified. In particular, we focused on the initial stages of growth, that turned to be key for achieving a high yield in the arrays. We found that the positioning of the Ga droplet within the predefined holes on the substrate determined whether the nanowire would grow perpendicularly to the substrate. Our HRTEMstudies on the titled nanowires show that the initial nanowire seeds seem to nucleate at the corner of the nanoscale holes. Instead, the crystal seeds of vertical nanowires occupy homogeneously the nanoscale holes. Achieving high yield in the growth of GaAs arrays on silicon also allowed us to study their evolution in time. We demonstrated that there is an incubation time for nanowires to start growing. This incubation time is different from NW to NWand leads to a relatively broad length distribution. We proposed a solution and showed how an increase in the supersaturation in the Ga droplet leads to the formation of homogeneous arrays. Growth of InAs nanowires in ordered arrays on silicon was based on the concept of guided growth. We used a SiO2 nanotube templates to promote vertical growth. Due to the directionality of MBE, achieving growth inside a nanotube was especially challenging. Our results provided new insights on the role of different pathways of the In and As4 adatoms during growth. In this part, large scale patterning by phase shift photolithography was demonstrated as an alternative to the conventionally used electron beam lithography. Stain etching method for producing porous silicon was applied on top-bottom fabricated Si micropillars. This led to geometrically driven electrochemical dissolution of silicon trough the center of the microstructure forming microtubes. The optical properties were also studied and used to produce functional 3D LED.

EPFL2017

Spin-valley optoelectronics based on two-dimensional materials

Dmitrii Unuchek

Two-dimensional (2D) materials, in particular graphene and transition metal dichalcogenides (TMDC), have attracted great scientific interest over the last decade, revealing exceptional mechanical, electrical and optical properties. Owing to their layered nature, subnanometer-thick single-layer forms of these crystals can be chemically grown or mechanically isolated, representing an ultimately scaled-down platform for further miniaturization of electronic devices. Indeed, the large family of 2D materials contains hundreds of members, including metals, semiconductors, insulators, and others, covering the whole spectrum of potential applications. Availability of all necessary building blocks for the construction of all-2D solid-state devices makes this platform ideal for fabrication of ultrathin, transparent and flexible devices. Extensively investigated graphene has demonstrated excellent electrical properties. However, the absence of a bandgap is an obstacle for its interaction with light and therefore limits applications in optics. In this aspect, atomically thin TMDC semiconductors appear to be an alternative, more promising platform, as they possess a direct band gap in the visible range in the monolayer form. Despite being only three atoms thick, these semiconductors demonstrate exceptionally large light absorption, efficient light emission, and strong light-matter interaction, attracting justified interest from the optics community. We will focus on their potential applications for optoelectronics in Chapter 4. Even more, broken inversion symmetry and strong spin-orbit coupling in single-layer TMDC crystals reveal a new quantum number, the so-called valley index. Indeed, this unique degree of freedom of charge carriers is known for some materials since the 1970s. However, in the case of 2D semiconductors, spin-valley locking mechanism and valley contrasting optical selection rules open new ways for addressing, manipulation and sensing of this pseudospin, opening the whole new field of valleytronics. Due to the large splitting of the valence band, spin and valley degree of freedom become locked in these atomically thin materials. We employ this unique feature in Chapter 5 for indirect injection of spins into graphene by pumping valley polarized carriers in an adjacent TMDC monolayer. Being gapless, graphene does not allow direct optical injection of spins. Another striking feature of 2D materials is their unique ability to be stacked in vertical heterostructures with strong electrical coupling between layers. The weak van der Waals force, which keeps components together, provides freedom in the assembly process, so that a lattice mismatch or a twist angle becomes unimportant in the first approximation. This provides a novel platform for harvesting complementary properties of the constituent materials, allowing the engineering of new artificial meta-materials as we demonstrate in Chapter 6. Furthermore, synergistic effects in van der Waals heterostructures enable completely new properties and phenomena, which do not exist in the single materials, with twist angle being an important knob for tuning these effects. We observe and exploit such novel phenomena arising in heterostructures of 2D semiconductors in the last chapter of this thesis. On the way to the realization of practical optoelectronic and valleytronic applications, this thesis studies fundamental aspects of rich spin-valley physics of atomically thin semiconductors

EPFL2019