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The diversity of 2D materials and their van der Waals (vdW) stacking presents a fertile ground for engineering novel multifunctional materials and quantum states of matter. This permits unique opportunities to tailor the electronic properties of vdW heterostructures by the insertion of only a single 2D material layer. However, such vdW materials engineering at the atomic scale has yet to be investigated for spin-charge interconversion phenomena. Here, we report on the control of these effects at the monolayer level, where drastic increase in intensity and change in sign of THz spintronic emission are demonstrated by inserting a single layer of MoSe$_2$ between PtSe$_2$ and graphene in a fully epitaxial, large area stacked structure. By using a combination of spin and angle resolved photoemission and density functional theory to reveal the electronic and spin structures, we illustrate two different mechanisms relying on charge transfer and electronic hybridization for the formation of Rashba states, which are responsible for spin-charge conversion and hence the THz spintronic emission. These findings open new pathways to design, at the atomic scale, efficient THz spintronic emitters made of 2D materials and other spintronic devices based on spin-charge interconversion phenomena., Comment: 16 pages, 4 figures

Transition metal dichalcogenides (TMD) like MoSe$_2$ exhibit remarkable optical properties such as intense photoluminescence (PL) in the monolayer form. To date, narrow-linewidth PL is only achieved in micrometer-sized exfoliated TMD flakes encapsulated in hexagonal boron nitride (hBN). In this work, we develop a growth strategy to prepare monolayer MoSe$_2$ on hBN flakes by molecular beam epitaxy in the van der Waals regime. It constitutes the first step towards the development of large area single crystalline TMDs encapsulated in hBN for potential integration in electronic or opto-electronic devices. For this purpose, we define a two-step growth strategy to achieve monolayer-thick MoSe$_2$ grains on hBN flakes. The high quality of MoSe$_2$ allows us to detect very narrow PL linewidth down to 5.5 meV at 13 K, comparable to the one of encapsulated exfoliated MoSe$_2$ flakes. Moreover, sizeable PL can be detected at room temperature as well as clear reflectivity signatures of A, B and charged excitons., Comment: 6 pages, 6 figures

Transition Metal Dichalcogenides (TMD) are layered materials obtained by stacking two-dimensional sheets weakly bonded by van der Waals interactions. In bulk TMD, band dispersions are observed in the direction normal to the sheet plane (z-direction) due to the hybridization of out-of-plane orbitals but no kz-dispersion is expected at the single-layer limit. Using angle-resolved photoemission spectroscopy, we precisely address the two-dimensional to three-dimensional crossover of the electronic band structure of epitaxial WSe$_2$ thin films. Increasing number of discrete electronic states appears in given kz-ranges while increasing the number of layers. The continuous bulk dispersion is nearly retrieved for 6-sheet films. These results are reproduced by calculations going from a relatively simple tight-binding model to a sophisticated KKR-Green's function calculation. This two-dimensional system is hence used as a benchmark to compare different theoretical approaches.

Two-dimensional and van der Waals ferromagnets are ideal platform to study low dimensional magnetism and proximity effects in van der Waals heterostructures. Their ultimate two dimensional character offers also the opportunity to easily adjust their magnetic properties using strain or electric fields. Among 2D ferromagnets, the Cr$_{1+x}$Te$_2$ compounds with $x$=0-1 are very promising because their magnetic properties depend on the amount of self-intercalated Cr atoms between pure CrTe$_2$ layers and the Curie temperature (T$_C$) can reach room temperature for certain compositions. Here, we investigate the evolution of the composition, structural and magnetic properties of thin Cr$_{1.33}$Te$_2$ (Cr$_2$Te$_3$) films epitaxially grown on graphene upon annealing. We observe a transition above 450{\deg}C from the Cr$_{1.33}$Te$_2$ phase with perpendicular magnetic anisotropy and a T$_C$ of 180 K to a composition close to Cr$_{1.39}$Te$_2$ with in-plane magnetic anisotropy and a T$_C$ of 240-250 K. This phase remains stable up to 650{\deg}C above which a pure Cr film starts to form. This work demonstrates the complex interplay between intercalated Cr, lattice parameters and magnetic properties in Cr$_{1+x}$Te$_2$ compounds., Comment: 5 pages, 5 figures

With the support of the national program on measurements, standards, and evaluation of quantum technologies MetriQs-France, a part of the French national quantum strategy, the BACQ project is dedicated to application-oriented benchmarks for quantum computing. The consortium gathering THALES, EVIDEN, an Atos business, CEA, CNRS, TERATEC, and LNE aims at establishing performance evaluation criteria of reference, meaningful for industry users.

We present a study by Scanning Tunneling Microscopy, supported by ab initio calculations, of the interaction between graphene and monolayer (semiconducting) PtSe$_2$ as a function of the twist angle ${\theta}$ between the two layers. We analyze the PtSe$_2$ contribution to the hybrid interface states that develop within the bandgap of the semiconductor to probe the interaction. The experimental data indicate that the interlayer coupling increases markedly with the value of ${\theta}$, which is confirmed by ab initio calculations. The moir\'e patterns observed within the gap are consistent with a momentum conservation rule between hybridized states, and the strength of the hybridization can be qualitatively described by a perturbative model., Comment: Article: 12 pages, 3 figures; Supporting Informations: 19 pages, 12 figures

There has been a recent interest in proposing quantum protocols whose security relies on weaker computational assumptions than their classical counterparts. Importantly to our work, it has been recently shown that public-key encryption (PKE) from one-way functions (OWF) is possible if we consider quantum public keys. Notice that we do not expect classical PKE from OWF given the impossibility results of Impagliazzo and Rudich (STOC'89). However, the distribution of quantum public keys is a challenging task. Therefore, the main question that motivates our work is if quantum PKE from OWF is possible if we have classical public keys. Such protocols are impossible if ciphertexts are also classical, given the impossibility result of Austrin et al. (CRYPTO'22) of quantum enhanced key-agreement (KA) with classical communication. In this paper, we focus on black-box separation for PKE with classical public key and quantum ciphertext from OWF under the polynomial compatibility conjecture, first introduced in Austrin et al.. More precisely, we show the separation when the decryption algorithm of the PKE does not query the OWF. We prove our result by extending the techniques of Austrin et al. and we show an attack for KA in an extended classical communication model where the last message in the protocol can be a quantum state.

Epitaxial growth has become a promising route to achieve highly crystalline continuous two-dimensional layers. However, high-quality layer production with expected electrical properties is still challenging due to the defects induced by the coalescence between imperfectly aligned domains. In order to control their intrinsic properties at the device scale, the synthesized materials should be described as a patchwork of coalesced domains. Here, we report multi-scale and multistructural analysis on highly oriented epitaxial WS$_2$ and WSe$_2$ monolayers using scanning transmission electron microscopy (STEM) techniques. Characteristic domain junctions are first identified and classified based on the detailed atomic structure analysis using aberration corrected STEM imaging. Mapping orientation, polar direction and phase at the micrometer scale using four-dimensional STEM enabled to access the density and the distribution of the specific domain junctions. Our results validate a readily applicable process for the study of highly oriented epitaxial transition metal dichalcogenides, providing an overview of synthesized materials from large scale down to atomic scale with multiple structural information., Comment: 22 pages, 6 figures and Supplementary Information

Terahertz (THz) Spintronic emitters based on ferromagnetic/metal junctions have become an important technology for the THz range, offering powerful and ultra-large spectral bandwidths. These developments have driven recent investigations of two-dimensional (2D) materials for new THz spintronic concepts. 2D materials, such as transition metal dichalcogenides (TMDs), are ideal platforms for SCC as they possess strong spin-orbit coupling (SOC) and reduced crystal symmetries. Moreover, SCC and the resulting THz emission can be tuned with the number of layers, electric field or strain. Here, epitaxially grown 1T-PtSe$_2$ and sputtered Ferromagnet (FM) heterostructures are presented as a novel THz emitter where the 1T crystal symmetry and strong SOC favor SCC. High quality of as-grown PtSe$_2$ layers is demonstrated and further FM deposition leaves the PtSe$_2$ unaffected, as evidenced with extensive characterization. Through this atomic growth control, the unique thickness dependent electronic structure of PtSe$_2$ allows the control of the THz emission by SCC. Indeed, we demonstrate the transition from the inverse Rashba-Edelstein effect in one monolayer to the inverse spin Hall effect in multilayers. This band structure flexibility makes PtSe$_2$ an ideal candidate as a THz spintronic 2D material and to explore the underlying mechanisms and engineering of the SCC for THz emission., Comment: 26 pages, 6 figures

Achieving large-scale growth of two-dimensional (2D) ferromagnetic materials with high Curie temperature (TC) and perpendicular magnetic anisotropy (PMA) is highly desirable for the development of ultra-compact magnetic sensors and magnetic memories. In this context, van der Waals (vdW) Cr2Te3 appears as a promising candidate. Bulk Cr2Te3 exhibits strong PMA and a TC of 180 K. Moreover, both PMA and TC might be adjusted in ultrathin films by engineering composition, strain, or applying an electric field. In this work, we demonstrate the molecular beam epitaxy (MBE) growth of vdW heterostructures of five-monolayer quasi-freestanding Cr2Te3 on three classes of 2D materials: graphene (semimetal), WSe2 (semiconductor) and Bi2Te3 (topological insulator). By combining structural and chemical analysis down to the atomic level with ab initio calculations, we confirm the single crystalline character of Cr2Te3 films on the 2D materials with sharp vdW interfaces. They all exhibit PMA and TC close to the bulk Cr2Te3 value of 180 K. Ab initio calculations confirm this PMA and show how its strength depends on strain. Finally, Hall measurements reveal a strong anomalous Hall effect, which changes sign at a given temperature. We theoretically explain this effect by a sign change of the Berry phase close to the Fermi level. This transition temperature depends on the 2D material in proximity, notably as a consequence of charge transfer. MBE-grown Cr2Te3/2D material bilayers constitute model systems for the further development of spintronic devices combining PMA, large spin-orbit coupling and sharp vdW interface., Comment: 18 pages, 13 figures and Supplemental Material

The subset cover problem for $k \geq 1$ hash functions, which can be seen as an extension of the collision problem, was introduced in 2002 by Reyzin and Reyzin to analyse the security of their hash-function based signature scheme HORS. The security of many hash-based signature schemes relies on this problem or a variant of this problem (e.g. HORS, SPHINCS, SPHINCS+, $\dots$). Recently, Yuan, Tibouchi and Abe (2022) introduced a variant to the subset cover problem, called restricted subset cover, and proposed a quantum algorithm for this problem. In this work, we prove that any quantum algorithm needs to make $\Omega\left((k+1)^{-\frac{2^{k}}{2^{k+1}-1}}\cdot N^{\frac{2^{k}-1}{2^{k+1}-1}}\right)$ queries to the underlying hash functions with codomain size $N$ to solve the restricted subset cover problem, which essentially matches the query complexity of the algorithm proposed by Yuan, Tibouchi and Abe. We also analyze the security of the general $(r,k)$-subset cover problem, which is the underlying problem that implies the unforgeability of HORS under a $r$-chosen message attack (for $r \geq 1$). We prove that a generic quantum algorithm needs to make $\Omega\left(N^{k/5}\right)$ queries to the underlying hash functions to find a $(1,k)$-subset cover. We also propose a quantum algorithm that finds a $(r,k)$-subset cover making $O\left(N^{k/(2+2r)}\right)$ queries to the $k$ hash functions.

Multilayers based on quantum materials (complex oxides, topological insulators, transition-metal dichalcogenides, etc) have enabled the design of devices that could revolutionize microelectronics and optoelectronics. However, heterostructures incorporating quantum materials from different families remain scarce, while they would immensely broaden the range of possible applications. Here we demonstrate the large-scale integration of compounds from two highly-multifunctional families: perovskite oxides and transition-metal dichalcogenides (TMDs). We couple BiFeO$_3$, a room-temperature multiferroic oxide, and WSe$_2$, a semiconducting two-dimensional material with potential for photovoltaics and photonics. WSe$_2$ is grown by molecular beam epitaxy and transferred on a centimeter-scale onto BiFeO$_3$ films. Using angle-resolved photoemission spectroscopy, we visualize the electronic structure of 1 to 3 monolayers of WSe$_2$ and evidence a giant energy shift as large as 0.75 eV induced by the ferroelectric polarization direction in the underlying BiFeO$_3$. Such a strong shift opens new perspectives in the efficient manipulation of TMDs properties by proximity effects.

We have analyzed by means of scanning tunneling microscopy and spectroscopy the atomic and electronic structure of monolayers of 1T-VxPt1-xSe2 alloys grown by molecular beam epitaxy on epitaxial graphene substrates. We have focused on the composition range (0.1

Two-dimensional materials (2D) arranged in hybrid van der Waals (vdW) heterostructures provide a route toward the assembly of 2D and conventional III-V semiconductors. Here, we report the structural and electronic properties of single layer WSe2 grown by molecular beam epitaxy on Se-terminated GaAs(111)B. Reflection high-energy electron diffraction images exhibit sharp streaky features indicative of a high-quality WSe2 layer produced via vdW epitaxy. This is confirmed by in-plane x-ray diffraction. The single layer of WSe2 and the absence of interdiffusion at the interface are confirmed by high resolution X-ray photoemission spectroscopy and high-resolution transmission microscopy. Angle-resolved photoemission investigation revealed a well-defined WSe2 band dispersion and a high p-doping coming from the charge transfer between the WSe2 monolayer and the Se-terminated GaAs substrate. By comparing our results with local and hybrid functionals theoretical calculation, we find that the top of the valence band of the experimental heterostructure is close to the calculations for free standing single layer WSe2. Our experiments demonstrate that the proximity of the Se-terminated GaAs substrate can significantly tune the electronic properties of WSe2. The valence band maximum (VBM, located at the K point of the Brillouin zone) presents an upshifts of about 0.56 eV toward the Fermi level with respect to the VBM of WSe2 on graphene layer, which is indicative of high p-type doping and a key feature for applications in nanoelectronics and optoelectronics.

Nearly localized moire flat bands in momentum space, arising at particular twist angles, are the key to achieve correlated effects in transition-metal dichalcogenides. Here, we use angle-resolved photoemission spectroscopy (ARPES) to visualize the presence of a flat band near the Fermi level of van der Waals (vdW) WSe2/MoSe2 heterobilayer grown by molecular beam epitaxy. This flat band is localized near the K point of the Brillouin zone and has a width of several hundred meVs. By combining ARPES measurements with density functional theory (DFT) calculations, we confirm the coexistence of different domains, namely the reference 2H stacking without layer misorientation and regions with arbitrary twist angles. For the 2H-stacked heterobilayer, our ARPES results show strong interlayer hybridization effects, further confirmed by complementary micro- Raman spectroscopy measurements. The spin-splitting of the valence band at K is determined to be 470 meV. The valence band maximum (VBM) position of the heterobilayer is located at the Gamma point. The energy difference between the VBM at Gamma and the K point is of -60 meV, which is a stark difference compared to individual 1L WSe2 and 1L WSe2, showing both a VBM at K.

We present a comparative investigation of the influence of crystallinity and film thickness on the acoustic and thermal properties of 2D layered PtSe2 thin films of varying thickness (0.6-24 nm) by combining a set of experimental techniques, namely, frequency domain thermo-reflectance, low-frequency Raman and pump-probe coherent phonon spectroscopy. We find a 35% reduction in the cross-plane thermal conductivity of polycrystalline films with thickness larger than 12 nm compared to the crystalline films of the same thickness due to phonon grain boundary scattering. Density functional theory calculations are in good agreement with the experiments and further reveal the ballistic nature of cross-plane heat transport in PtSe2 up to a certain thickness (~20 nm). In addition, our experiments revealed strong interlayer interactions in PtSe2, short acoustic phonon lifetimes in the range of picoseconds, out-of-plane elastic constant C33=31.8 GPa and layer-dependent group velocity ranging from 1340 m/s in bilayer PtSe2 to 1873 m/s in 8 layers of PtSe2. The potential of tuning the lattice cross-plane thermal conductivity of layered 2D materials with the level of crystallinity and the real-time observation of coherent phonon dynamics, which have direct implications on the cooling and transport of electrons, open a new playground for research in 2D thermoelectric devices and provide guidelines for thermal management in 2D electronics., Comment: 32 pages

PtSe2 is attracting considerable attention as a high mobility two-dimensional material with envisionned applications in microelectronics, photodetection and spintronics. The growth of high quality PtSe2 on insulating substrates with wafer-scale uniformity is a prerequisite for electronic transport investigations and practical use in devices. Here, we report the growth of highly oriented few-layers PtSe2 on ZnO(0001) by molecular beam epitaxy. The crystalline structure of the films is characterized with electron and X-ray diffraction, atomic force microscopy and transmission electron microscopy. The comparison with PtSe2 layers grown on graphene, sapphire, mica, SiO2 and Pt(111) shows that among insulating substrates, ZnO(0001) yields films of superior structural quality. Hall measurements performed on epitaxial ZnO/PtSe2 with 5 monolayers of PtSe2 show a clear semiconducting behaviour and a high mobility in excess of 200 cm2V 1s-1 at room temperature and up to 447 cm2V-1s-1 at low temperature.

In recent years, two-dimensional van der Waals materials have emerged as an important platform for the observation of long-range ferromagnetic order in atomically thin layers. Although heterostructures of such materials can be conceived to harness and couple a wide range of magneto-optical and magneto-electrical properties, technologically relevant applications require Curie temperatures at or above room-temperature and the ability to grow films over large areas. Here we demonstrate the large-area growth of single-crystal ultrathin films of stoichiometric Fe5GeTe2 on an insulating substrate using molecular beam epitaxy. Magnetic measurements show the persistence of soft ferromagnetism up to room temperature, with a Curie temperature of 293 K, and a weak out-of-plane magnetocrystalline anisotropy. Surface, chemical, and structural characterizations confirm the layer-by-layer growth, 5:1:2 Fe:Ge:Te stoichiometric elementary composition, and single crystalline character of the films.

We report on a novel material, namely two-dimensional (2D) V$_{1-x}$Pt$_x$Se$_2$ alloy, exhibiting simultaneously ferromagnetic order and Rashba spin-orbit coupling. While ferromagnetism is absent in 1T-VSe$_2$ due to the competition with the charge density wave phase, we demonstrate theoretically and experimentally that the substitution of vanadium by platinum in VSe$_2$ (10-50 %) to form an homogeneous 2D alloy restores ferromagnetic order with Curie temperatures of 6 K for 5 monolayers and 25 K for one monolayer of V$_{0.65}$Pt$_{0.35}$Se$_2$. Moreover, the presence of platinum atoms gives rise to Rashba spin-orbit coupling in (V,Pt)Se$_2$ providing an original platform to study the interplay between ferromagnetism and spin-orbit coupling in the 2D limit., Comment: 5 pages, 5 figures

The structure inversion asymmetry at surfaces and interfaces give rise to the Rashba spin-orbit interaction (SOI), that breaks the spin degeneracy of surface or interface states. Hence, when an electric current runs through a surface or interface, this Rashba effect generates an effective magnetic field acting on the electron spin. This provides an additional tool to manipulate the spin state in materials such as Si and Ge that, in their bulk form, possess inversion symmetry (or lack structural inersion asymmetry). The existence of Rashba states could be demonstrated by photoemission spectroscopy at the interface between different metals and Ge(111) and by spin-charge conversion experiments at the Fe/Ge(111) interface even though made of two light elements. In this work, we identify the fingerprint of the Rashba states at the Fe/Ge(111) interface by magnetotransport measurements in the form of a large unidirectional magnetoresistance of up to 0.1 \%. From its temperature dependence, we find that the Rashba energy splitting is larger than in pure Ge(111) subsurface states., Comment: 6 pages, 5 figures

Janus single-layer transition metal dichalcogenides, in which the two chalcogen layers have a different chemical nature, push chemical composition control beyond what is usually achievable with van der Waals heterostructures. Here we report such a novel Janus compound, SPtSe, which is predicted to exhibit strong Rashba spin-orbit coupling. We synthetized it by conversion of a single-layer of PtSe$_2$ on Pt(111) via sulphurization under H$_2$S atmosphere. Our in situ and operando structural analysis with grazing incidence synchrotron X-ray diffraction reveals the process by which the Janus alloy forms. The crystalline long-range order of the as-grown PtSe$_2$ monolayer is first lost due to thermal annealing. A subsequent recrystallization in presence of a source of sulphur yields a highly ordered SPtSe alloy, which is iso-structural to the pristine PtSe$_2$. The chemical composition is resolved, layer-by-layer, using angle-resolved X-ray photoelectron spectroscopy, demonstrating that Se-by-S substitution occurs selectively in the topmost chalcogen layer., Comment: 23 pages, 4 figures and 1 table

Imaging the magnetic configuration of thin-films has been a long-standing area of research. Since a few years, the emergence of two-dimensional ferromagnetic materials calls for innovation in the field of magnetic imaging. As the magnetic moments are extremely small, standard techniques like SQUID, torque magnetometry, magnetic force microscopy and Kerr effect microscopy are challenging and often lead to the detection of parasitic magnetic contributions or spurious effects. In this work, we report a new magnetic microscopy technique based on the combination of magnetic circular dichroism and Seebeck effect in semiconductor/ferromagnet bilayers. We implement this method with perpendicularly magnetized (Co/Pt) multilayers sputtered on Ge (111). We further show that the electrical detection of MCD is more sensitive than the Kerr magnetometry, especially in the ultra-thin film regime, which makes it particularly promising for the study of emergent two-dimensional ferromagnetic materials., Comment: 8 pages, 10 figures

Topological insulators (TIs) hold great promises for new spin-related phenomena and applications thanks to the spin texture of their surface states. However, a versatile platform allowing for the exploitation of these assets is still lacking due to the difficult integration of these materials with the mainstream Si-based technology. Here, we exploit germanium as a substrate for the growth of Bi$_2$Se$_3$, a prototypical TI. We probe the spin properties of the Bi$_2$Se$_3$/Ge pristine interface by investigating the spin-to-charge conversion taking place in the interface states by means of a non-local detection method. The spin population is generated by optical orientation in Ge, and diffuses towards the Bi$_2$Se$_3$ which acts as a spin detector. We compare the spin-to-charge conversion in Bi$_2$Se$_3$/Ge with the one taking place in Pt in the same experimental conditions. Notably, the sign of the spin-to-charge conversion given by the TI detector is reversed compared to the Pt one, while the efficiency is comparable. By exploiting first-principles calculations, we ascribe the sign reversal to the hybridization of the topological surface states of Bi$_2$Se$_3$ with the Ge bands. These results pave the way for the implementation of highly efficient spin detection in TI-based architectures compatible with semiconductor-based platforms., Comment: 5 pages and 5 figures

The search for high-quality transition metal dichalcogenides mono- and multi-layers grown on large areas is still a very active field of investigation nowadays. Here, we use molecular beam epitaxy to grow 15$\times$15 mm large WSe$_2$ on mica in the van der Waals regime. By screening one-step growth conditions, we find that very high temperature ($>$900$^{\circ}$C) and very low deposition rate ($<$0.015 nm/min) are necessary to obtain high quality WSe$_2$ films. The domain size can be larger than 1 $\mu$m and the in-plane rotational misorientation less than $\pm$0.5$^{\circ}$. The WSe$_2$ monolayer is also robust against air exposure, can be easily transferred over 1 cm$^2$ on SiN/SiO$_2$ and exhibits strong photoluminescence signal. Moreover, by combining grazing incidence x-ray diffraction and transmission electron microscopy, we could detect the presence of few misoriented grains. A two-dimensional model based on atomic coincidences between the WSe$_2$ and mica crystals allows us to explain the formation of these misoriented grains and gives suggestion to remove them and further improve the crystalline quality of WSe$_2$., Comment: 20 pages and 6 figures

The Hall effect can be extended by inducing a temperature gradient in lieu of electric field that is known as the Nernst (-Ettingshausen) effect. The recently discovered spin Nernst effect in heavy metals continues to enrich the picture of Nernst effect-related phenomena. However, the collection would not be complete without mentioning the valley degree of freedom benchmarked by the observation of the valley Hall effect. Here we show the experimental evidence of its missing counterpart, the valley Nernst effect. Using millimeter-sized WSe$_{2}$ mono-multi-layers and the ferromagnetic resonance-spin pumping technique, we are able to apply a temperature gradient by off-centering the sample in the radio frequency cavity and address a single valley through spin-valley coupling. The combination of a temperature gradient and the valley polarization leads to the valley Nernst effect in WSe$_{2}$ that we detect electrically at room temperature. The valley Nernst coefficient is in very good agreement with the predicted value., Comment: 8 pages and 5 figures

The magnetic order associated with the degree of freedom of spin in two-dimensional (2D) materials is subjected to intense investigation because of its potential application in 2D spintronics and valley-related magnetic phenomena. We report here a bottom-up strategy using molecular beam epitaxy to grow and dope large-area (cm$^2$) few-layer MoSe$_2$ with Mn as a magnetic dopant. High-quality Mn-doped MoSe$_2$ layers are obtained for Mn content of less than 5 % (atomic). When increasing the Mn content above 5 % we observe a clear transition from layer-by-layer to cluster growth. Magnetic measurements involving a transfer process of the cm$^2$-large doped layers on 100-micron-thick silicon substrate, show plausible proof of high-temperature ferromagnetism of 1 % and 10 % Mn-doped MoSe$_2$. Although we could not point to a correlation between magnetic and electrical properties, we demonstrate that the transfer process described in this report permits to achieve conventional electrical and magnetic measurements on the doped layers transferred on any substrate. Therefore, this study provides a promising route to characterize stable ferromagnetic 2D layers, which is broadening the current start-of-the-art of 2D materials-based applications., Comment: 18 pages and 5 figures

Relating magnetotransport properties to specific spin textures at surfaces or interfaces is an intense field of research nowadays. Here, we investigate the variation of the electrical resistance of Ge(111) grown epitaxially on semi-insulating Si(111) under the application of an external magnetic field. We find a magnetoresistance term which is linear in current density j and magnetic field B, hence odd in j and B, corresponding to a unidirectional magnetoresistance. At 15 K, for I = 10 $\mu$A (or j = 0.33 A/m) and B = 1 T, it represents 0.5 % of the zero field resistance, a much higher value compared to previous reports on unidirectional magnetoresistance. We ascribe the origin of this magnetoresistance to the interplay between the externally applied magnetic field and the current-induced pseudo-magnetic field in the spin-splitted subsurface states of Ge(111). This unidirectional magnetoresistance is independent of the current direction with respect to the Ge crystal axes. It progressively vanishes, either using a negative gate voltage due to carrier activation into the bulk (without spin-splitted bands), or by increasing the temperature due to the Rashba energy splitting of the subsurface states lower than $\sim$58 k$_B$. The highly developed technologies on semiconductor platforms would allow the rapid optimization of devices based on this phenomenon., Comment: 5 pages, 4 figures

Large-area growth of continuous transition metal dichalcogenides (TMDCs) layers is a prerequisite to transfer their exceptional electronic and optical properties into practical devices. It still represents an open issue nowadays. Electric and magnetic doping of TMDC layers to develop basic devices such as p-n junctions or diluted magnetic semiconductors for spintronic applications are also an important field of investigation. Here, we have developed two different techniques to grow MoSe$_2$ mono- and multi-layers on SiO$_2$/Si substrates over large areas. First, we co-deposited Mo and Se atoms on SiO$_2$/Si by molecular beam epitaxy in the van der Waals regime to obtain continuous MoSe$_2$ monolayers over 1 cm$^2$. To grow MoSe$_2$ multilayers, we then used the van der Waals solid phase epitaxy which consists in depositing an amorphous Se/Mo bilayer on top of a co-deposited MoSe$_2$ monolayer which serves as a van der Waals growth template. By annealing, we obtained continuous MoSe$_2$ multilayers over 1 cm$^2$. Moreover, by inserting a thin layer of Mn in the stack, we could demonstrate the incorporation of up to 10 \% of Mn in MoSe$_2$ bilayers., Comment: 32 pages, 13 figures

Topological insulators (TIs) like Bi$_2$Se$_3$ are a class of material with topologically protected surface states in which spin-momentum locking may enable spin-polarized and defect-tolerant transport. In this work, we achieved the epitaxial growth of Bi$_2$Se$_3$ thin films on germanium, which is a key material for microelectronics. Germanium also exhibits interesting properties with respect to the electron spin such as a spin diffusion length of several micrometers at room temperature. By growing Bi$_2$Se$_3$ on germanium, we aim at combining the long spin diffusion length of Ge with the spin-momentum locking at the surface of Bi$_2$Se$_3$. We first performed a thorough structural analysis of Bi$_2$Se$_3$ films using electron and x-ray diffraction as well as atomic force microscopy. Then, magnetotransport measurements at low temperature showed the signature of weak antilocalization as a result of two-dimensional transport in the topologically protected surface states of Bi$_2$Se$_3$. Interestingly, the magnetotransport measurements also point out that the conduction channel can be tuned between the Bi$_2$Se$_3$ film and the Ge layer underneath by means of the bias voltage or the applied magnetic field. This result suggests that the Bi$_2$Se$_3$/Ge junction is a promising candidate for tuning spin-related phenomena at interfaces between TIs and semiconductors., Comment: 18 pages, 8 figures

Gray tin, also known as $\alpha$-Sn, can be turned into a three-dimensional topological insulator (3D-TI) by strain and finite size effects. Such room temperature 3D-TI is peculiarly interesting for spintronics due to the spin-momentum locking along the Dirac cone (linear dispersion) of the surface states. Angle resolved photoemission spectroscopy (ARPES) has been used to investigate the dispersion close to the Fermi level in thin (0\,0\,1)-oriented epitaxially strained films of $\alpha$-Sn, for different film thicknesses as well as for different capping layers (Al, AlO$_x$ and MgO). Indeed a proper capping layer is necessary to be able to use $\alpha$-Sn surface states for spintronics applications. In contrast with free surfaces or surfaces coated with Ag, coating the $\alpha$-Sn surface with Al or AlO$_x$ leads to a drop of the Fermi level below the Dirac point, an important consequence for transport is the presence of bulk states at the Fermi level. $\alpha$-Sn films coated by AlO$_x$ are studied by electrical magnetotransport: despite clear evidence of surface states revealed by Shubnikov-de Haas oscillations, an important part of the magneto-transport properties is governed by "bulk" electronic states attributed to the $\Gamma 8$ band, as suggested by {\it ab-initio} calculations.

Spin-charge interconversion (SCI) phenomena have attracted a growing interest in the field of spintronics as means to detect spin currents or manipulate the magnetization of ferromagnets. The key ingredients to exploit these assets are a large conversion efficiency, the scalability down to the nanometer scale and the integrability with opto-electronic and spintronic devices. Here we show that, when an ultrathin Bi film is epitaxially grown on top of a Ge(111) substrate, quantum size effects arising in nanometric Bi islands drastically boost the SCI efficiency, even at room temperature. Using x-ray diffraction (XRD), scanning tunneling microscopy (STM) and spin- and angle-resolved photoemission (S-ARPES) we obtain a clear picture of the film morphology, crystallography and electronic structure. We then exploit the Rashba-Edelstein effect (REE) and inverse Rashba-Edelstein effect (IREE) to directly quantify the SCI efficiency using optical and electrical spin injection., Comment: 18 pages, 5 figures

Molecular beam epitaxy technique has been used to deposit a single layer and a bilayer of MoSe 2 on sapphire. Extensive characterizations including in-situ and ex-situ measurements show that the layered MoSe 2 grows in a scalable manner on the substrate and reveals characteristics of a stoichiometric 2H-phase. The layered MoSe 2 exhibits polycrystalline features with domains separated by defects and boundaries. Temperature and magnetic field dependent resistivity measurements unveil a carrier hopping character described within two-dimensional variable range hopping mechanism. Moreover, a negative magnetoresistance was observed, stressing a fascinating feature of the charge transport under the application of a magnetic field in the layered MoSe 2 system. This negative magnetoresistance observed at millimeter-scale is similar to that observed recently at room temperature inWS2 flakes at a micrometer scale [Zhang et al., Appl. Phys. Lett. 108, 153114 (2016)]. This scalability highlights the fact that the underlying physical mechanism is intrinsic to these two-dimensional materials and occurs at very short scale., Comment: 15 pages, 6 figures

Non-local carrier injection/detection schemes lie at the very foundation of information manipulation in integrated systems. This paradigm consists in controlling with an external signal the channel where charge carriers flow between a "source" and a well separated "drain". The next generation electronics may operate on the spin of carriers instead of their charge and germanium appears as the best hosting material to develop such a platform for its compatibility with mainstream silicon technology and the long electron spin lifetime at room temperature. Moreover, the energy proximity between the direct and indirect bandgaps allows for optical spin injection and detection within the telecommunication window. In this letter, we demonstrate injection of pure spin currents (\textit{i.e.} with no associated transport of electric charges) in germanium, combined with non-local spin detection blocks at room temperature. Spin injection is performed either electrically through a magnetic tunnel junction (MTJ) or optically, exploiting the ability of lithographed nanostructures to manipulate the distribution of circularly-polarized light in the semiconductor. Pure spin current detection is achieved using either a MTJ or the inverse spin-Hall effect (ISHE) across a platinum stripe. These results broaden the palette of tools available for the realization of opto-spintronic devices., Comment: 14 pages and 5 figures

We present experimental results on the conversion of a spin current into a charge current by spin pumping into the Dirac cone with helical spin polarization of the elemental topological insulator (TI) {\alpha}-Sn[1-3]. By angle-resolved photoelectron spectroscopy (ARPES) we first confirm that the Dirac cone at the surface of {\alpha}-Sn (0 0 1) layers subsists after covering with Ag. Then we show that resonant spin pumping at room temperature from Fe through Ag into {\alpha}-Sn layers induces a lateral charge current that can be ascribed to the Inverse Edelstein Effect[4-5]. Our observation of an Inverse Edelstein Effect length[5-6] much longer than for Rashba interfaces[5-10] demonstrates the potential of the TI for conversion between spin and charge in spintronic devices. By comparing our results with data on the relaxation time of TI free surface states from time-resolved ARPES, we can anticipate the ultimate potential of TI for spin to charge conversion and the conditions to reach it., Comment: 14 pages, 5 figures

Spin injection and detection in Co60Fe40-based all-metallic lateral spin-valves have been studied at both room and low temperatures. The obtained spin signals amplitudes have been compared to that of identical Ni80Fe20-based devices. The replacement of Ni80Fe20 by CoFe allows increasing the spin signal amplitude by up to one order of magnitude, thus reaching 50 m{\Omega} at room temperature. The spin signal dependence with the distance between the ferromagnetic electrodes has been analyzed using both a 1D spin transport model and finite elements method simulations. The enhancement of the spin signal amplitude when using CoFe electrodes can be explained by a higher effective polarization., Comment: 8 pages and 4 figures

We have measured the inverse spin Hall effect (ISHE) in \textit{n}-Ge at room temperature. The spin current in germanium was generated by spin pumping from a CoFeB/MgO magnetic tunnel junction in order to prevent the impedance mismatch issue. A clear electromotive force was measured in Ge at the ferromagnetic resonance of CoFeB. The same study was then carried out on several test samples, in particular we have investigated the influence of the MgO tunnel barrier and sample annealing on the ISHE signal. First, the reference CoFeB/MgO bilayer grown on SiO$_{2}$ exhibits a clear electromotive force due to anisotropic magnetoresistance and anomalous Hall effect which is dominated by an asymmetric contribution with respect to the resonance field. We also found that the MgO tunnel barrier is essential to observe ISHE in Ge and that sample annealing systematically lead to an increase of the signal. We propose a theoretical model based on the presence of localized states at the interface between the MgO tunnel barrier and Ge to account for these observations. Finally, all of our results are fully consistent with the observation of ISHE in heavily doped $n$-Ge and we could estimate the spin Hall angle at room temperature to be $\approx$0.001., Comment: 34 pages, 14 figures

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