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Abdelkarim Ouerghi

Publications and source records attributed to Abdelkarim Ouerghi.

At least 19 recordsLinked to original sources

Growth of Highly Conductive PtSe2 Films Controlled by Raman Metrics for High-Frequency Photodetectors and Optoelectronic Mixers at 1.55 μm

Two-dimensional PtSe2 exhibits outstanding intrinsic properties such as high carrier mobility, tunable bandgap, broadband absorption and air stability, making it ideal for (opto)electronic applications. In particular, thick PtSe2 is semimetallic and well suited for ultrafast optoelectronics in the infrared domain. However, achieving PtSe2 films of high crystalline quality with controlled properties on low-cost and insulating substrates remains challenging. Here, highly crystalline semimetallic PtSe2 films are grown by molecular beam epitaxy on sapphire substrates. It is shown how an optimized post-growth annealing remarkably improves the out-of-plane crystallinity and leads to record sheet conductances, up to 1.6 mS. In-depth structural analyses reveal the strong influence of the domain arrangement within the films on their electrical properties. Films that are mainly composed of vertically single crystalline domains exhibit high sheet conductance (1.1 - 1.6 mS), whereas films that contain superimposed twisted domains present low sheet conductance (0.5 - 0.6 mS). Moreover, it is demonstrated that the A1g Raman peak width, in addition to the commonly used Eg peak width, are both effective metrics for evaluating the quality of PtSe2: films with narrower Eg and A1g peaks exhibit higher in-plane and out-of-plane crystalline quality, respectively, as well as higher sheet conductance. Finally, coplanar waveguides integrating a semimetallic PtSe2 channel are fabricated on a 2-inch sapphire substrate to demonstrate optoelectronic devices operating at the 1.55 μm telecom wavelength. This includes photodetectors with a record 60 GHz bandwidth and the first PtSe2-based optoelectronic mixer with a bandwidth above 30 GHz.

cond-mat.mtrl-sci↗

Epitaxial Growth and Electronic Properties of QuasiFreeStanding Rhombohedral WSe2 Bilayers on Cubic W110

Rhombohedral-stacked transition metal dichalcogenides (TMDs) break inversion symmetry between adjacent layers, giving rise to an intrinsic out-of-plane ferroelectric polarization.Controlling the formation of this stacking polytype is therefore essential for harnessing ferroelectric effects in two-dimensional materials. In this work, we demonstrate the epitaxial growth of rhombohedral bilayer tungsten diselenide (3R-WSe2) on a cubic W(110) single crystal by molecular beam epitaxy. We show that selenium passivation of the substrate is key to enable a quasi van der Waals epitaxy effectively suppressing strong interfacial bonding and promoting the growth of quasi free standing bilayer films. The 3R stacking order is confirmed through a combination of Raman spectroscopy and high-resolution angle-resolved photoemission spectroscopy (ARPES), supported by density functional theory (DFT) calculations. ARPES and DFT reveal an indirect-gap electronic structure with the valence-band maximum at the Gamma point, as well as a pronounced spin orbit driven splitting of 520 +- 20 meV at the K point. Analysis of the measured dispersions yields hole effective masses of 0.46 +- 0.04 me and 0.75 +- 0.06 me for the upper and lower valence bands at K point, respectively. These results establish a robust route for synthesizing quasi free standing 3R-WSe2 and provide a platform for exploring the electronic, optical, and ferroelectric functionalities that emerge from inversion symmetry breaking in layered TMDs. Our findings further highlight the potential of cubic substrates for deterministic fabrication of rhombohedral TMD heterostructures and ferroelectric devices at the nanoscale.

cond-mat.mtrl-sci↗

Tunable electronic band structure in WSSe van der Waals Alloys

The electronic structure of semiconducting 2D materials such as transition metal dichalcogenides (TMDs) is known to be tunable by its environment, from simple external fields applied with electrical contacts up to complex van der Waals heterostructure assemblies. However, conventional alloying from reference binary TMD compounds to composition-controlled ternary alloys also offers unexplored opportunities. In this work, we use nano-angle resolved photoemission spectroscopy (nano-ARPES) and density functional theory (DFT) calculations to study the structural and electronic properties of different alloy compositions of bulk WS2(1-x)Se2x. Our results demonstrate the continuous variation of the band structure and the progressive evolution of the valence band splitting at the K points from 420 to 520 meV in bulk WS2(1-x)Se2x. We also carried out scanning tunneling microscopy (STM) measurements and DFT to understand the possible S or Se substitutions variants in WS2(1-x)Se2x alloys, with different local atomic configurations. Our work opens up perspectives for the fine control of the band dispersion in van der Waals materials and demonstrate how the band structure can be tuned in bulk TMDs. The collected information can serve as a reference for future applications.

cond-mat.mtrl-sci↗

Hybridization in van der Waals epitaxy of PtSe2/h-BN and PtSe2/graphene heterostructures

Van der Waals (vdW) heterostructures, which combine bi-dimensional materials of different properties, enable a range of quantum phenomena. Here, we present a comparative study between the electronic properties of mono- and bi-layer of platinum diselenide (PtSe2) grown on hexagonal boron nitride (h-BN) and graphene substrates using molecular beam epitaxy (MBE). Using angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT), the electronic structure of PtSe2/graphene and PtSe2/h-BN vdW heterostructures are investigated in systematic manner. In contrast to PtSe2/h-BN, the electronic structure of PtSe2/graphene reveals the presence of interlayer hybridization between PtSe2 and the graphene, which is evidenced by minigap openings in the π-band of graphene. Furthermore, our measurements show that the valence band maximum (VBM) of monolayer PtSe2 is located at the Γ point with different binding energies of about -0.9 eV and -0.55 eV relative to the Fermi level on h-BN and graphene and substrates, respectively. Our results represent a significant advance in the understanding of electronic hybridization between TMDs and different substrates, and they reaffirm the crucial role of the substrate in any nanoelectronic applications based on van der Waals heterostructures.

cond-mat.mtrl-sci↗

Mexican hat-like valence band dispersion and quantum confinement in rhombohedral ferroelectric alpha-In2Se3

Two-dimensional (2D) ferroelectric (FE) materials offer a large variety of electronic properties depending on chemical composition, number of layers and stacking-order. Among them, alpha-In2Se3 has attracted much attention due to the promise of outstanding electronic properties, attractive quantum physics, in- and out-of-plane ferroelectricity and high photo-response. Precise experimental determination of the electronic structure of rhombohedral (3R) alpha-In2Se3 is needed for a better understanding of potential properties and device applications. Here, combining angle resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) calculations, we demonstrate that 3R alpha-In2Se3 phase exhibits a robust inversion of the valence band parabolicity at the Gamma point forming a bow-shaped dispersion with a depth of 140 +- 10 meV between the valence band maximum (VBM) along the GammaK direction of the Brillouin zone (BZ). Moreover, we unveil an indirect band gap of about 1.25 eV, as well as a highly electron doping of approximatively 5.1012 electrons per cmsquare at the surface. This leads to surface band bending and the formation of a prominent electron accumulation layer. These findings allow a deeper understanding of the rhombohedral alpha-In2Se3 electronic properties underlying the potential of III/VI semiconductors for electronic and photonic technologies.

cond-mat.mtrl-sci↗

Distinguishing different stackings in WSe2 bilayers grown Using Chemical Vapor Deposition

The stacking order of two-dimensional transition metal dichalcogenides (TMDs) is attracting tremendous interest as an essential component of van der Waals heterostructures. A common and fast approach to distinguish between the AAprime (2H) and AB (3R) configurations uses the relative edge orientation of each triangular layer (theta) from optical images. Here, we highlight that this method alone is not sufficient to fully identify the stacking order. Instead we propose a model and methodology to accurately determine the bilayer configuration of WSe2 using second harmonic generation (SHG) and Raman spectroscopy. We demonstrate that the SHG response of the AB phase (theta = 0) deg layers is more intense than the signal from the single layer structure. However, the SHG totally vanishes in the AAprime and ABprime phases (theta = 60 deg) and 0 deg respectively) of homo-bilayer WSe2. Also, several optical features of homo-bilayer WSe2 are found to depend on the details of the stacking order, with the difference being the clearest in the low frequency (LF) Raman frequencies, as confirmed by DFT simulation. This allows unambiguous, high-throughput, nondestructive identification of stacking order in TMDs, which is not robustly addressed in this emerging research area.

cond-mat.mtrl-sci↗

Magnetic evolution of Cr$_2$Te$_3$ epitaxially grown on graphene with post-growth annealing

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°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°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.

cond-mat.mtrl-sci↗

High Strain Engineering of a Suspended WSSe Monolayer Membrane by Indentation and Measured by Tip-enhanced Photoluminescence

Straintronics involves the manipulation and regulation of the electronic characteristics of 2D materials through the use of macro- and nano-scale strain engineering. In this study, we utilized an atomic force microscope (AFM) coupled with an optical system to perform indentation measurements and tip-enhanced photoluminescence (TEPL), allowing us to extract the local optical response of a suspended monolayer membrane of ternary WSSe at various levels of deformation, up to strains of 10%. The photoluminescence signal is modelled considering the deformation, stress distribution and strain dependence of the WSSe band structure. We observe an additional TEPL signal that exhibits significant variation under strain, with 64 meV per percent of elongation. This peak is linked to the highly strained 2D material lying right underneath the tip. We discuss the amplification of the signal and its relation to the excitonic funnelling effect in a more comprehensive model. We will also compare the diffusion caused by Auger recombination against the radiative excitonic decay. We use TEPL to examine and comprehend the local physics of 2D semi-conducting materials subjected to extreme mechanical strain. Chemical vapour deposition-fabricated 2D ternaries possess high strain resistance, comparable to the benchmark MoS2, and a high Young's modulus of 273 GPa.

cond-mat.mes-hall↗

Reconfigurable Multifunctional van der Waals Ferroelectric Devices and Logic Circuits

In this work, we demonstrate the suitability of Reconfigurable Ferroelectric Field-Effect- Transistors (Re-FeFET) for designing non-volatile reconfigurable logic-in-memory circuits with multifunctional capabilities. Modulation of the energy landscape within a homojunction of a 2D tungsten diselenide (WSe$_2$) layer is achieved by independently controlling two split-gate electrodes made of a ferroelectric 2D copper indium thiophosphate (CuInP$_2$S$_6$) layer. Controlling the state encoded in the Program Gate enables switching between p, n and ambipolar FeFET operating modes. The transistors exhibit on-off ratios exceeding 10$^6$ and hysteresis windows of up to 10 V width. The homojunction can change from ohmic-like to diode behavior, with a large rectification ratio of 10$^4$. When programmed in the diode mode, the large built-in p-n junction electric field enables efficient separation of photogenerated carriers, making the device attractive for energy harvesting applications. The implementation of the Re-FeFET for reconfigurable logic functions shows how a circuit can be reconfigured to emulate either polymorphic ferroelectric NAND/AND logic-in-memory or electronic XNOR logic with long retention time exceeding 10$^4$ seconds. We also illustrate how a circuit design made of just two Re-FeFETs exhibits high logic expressivity with reconfigurability at runtime to implement several key non-volatile 2-input logic functions. Moreover, the Re-FeFET circuit demonstrates remarkable compactness, with an up to 80% reduction in transistor count compared to standard CMOS design. The 2D van de Waals Re-FeFET devices therefore exhibit groundbreaking potential for both More-than-Moore and beyond-Moore future of electronics, in particular for an energy-efficient implementation of in-memory computing and machine learning hardware, due to their multifunctionality and design compactness.

cond-mat.mes-hall↗

Quasi van der Waals Epitaxy of Rhombohedral-stacked Bilayer WSe2 on GaP(111) Heterostructure

The growth of bilayers of two-dimensional (2D) materials on conventional 3D semiconductors results in 2D/3D hybrid heterostructures, which can provide additional advantages over more established 3D semiconductors while retaining some specificities of 2D materials. Understanding and exploiting these phenomena hinge on knowing the electronic properties and the hybridization of these structures. Here, we demonstrate that rhombohedral-stacked bilayer (AB stacking) can be obtained by molecular beam epitaxy growth of tungsten diselenide (WSe2) on gallium phosphide (GaP) substrate. We confirm the presence of 3R-stacking of the WSe2 bilayer structure using scanning transmission electron microscopy (STEM) and micro-Raman spectroscopy. Also, we report high-resolution angle-resolved photoemission spectroscopy (ARPES) on our rhombohedral-stacked WSe2 bilayer grown on GaP(111)B substrate. Our ARPES measurements confirm the expected valence band structure of WSe2 with the band maximum located at the gamma point of the Brillouin zone. The epitaxial growth of WSe2 on GaP(111)B heterostructures paves the way for further studies of the fundamental properties of these complex materials, as well as prospects for their implementation in devices to exploit their promising electronic and optical properties.

cond-mat.mes-hall↗

Intrinsic defects and mid-gap states in quasi-one-dimensional Indium Telluride

Recently, intriguing physical properties have been unraveled in anisotropic semiconductors, in which the in-plane electronic band structure anisotropy often originates from the low crystallographic symmetry. The atomic chain is the ultimate limit in material downscaling for electronics, a frontier for establishing an entirely new field of one-dimensional quantum materials. Electronic and structural properties of chain-like InTe are essential for better understanding of device applications such as thermoelectrics. Here, we use scanning tunneling microscopy/spectroscopy (STM/STS) measurements and density functional theory (DFT) calculations to directly image the in-plane structural anisotropy in tetragonal Indium Telluride (InTe). As results, we report the direct observation of one-dimensional In1+ chains in InTe. We demonstrate that InTe exhibits a band gap of about 0.40 +-0.02 eV located at the M point of the Brillouin zone. Additionally, line defects are observed in our sample, were attributed to In1+ chain vacancy along the c-axis, a general feature in many other TlSe-like compounds. Our STS and DFT results prove that the presence of In1+ induces localized gap state, located near the valence band maximum (VBM). This acceptor state is responsible for the high intrinsic p-type doping of InTe that we also confirm using angle-resolved photoemission spectroscopy.

cond-mat.mtrl-sci↗

Quantum Confinement and Electronic Structure at the Surface of van der Waals Ferroelectric α-In$_{2}$Se$_{3}$

Two-dimensional (2D) ferroelectric (FE) materials are promising compounds for next-generation nonvolatile memories, due to their low energy consumption and high endurance. Among them, α-In$_{2}$Se$_{3}$ has drawn particular attention due to its in- and out-of-plane ferroelectricity, whose robustness has been demonstrated down to the monolayer limit. This is a relatively uncommon behavior since most bulk FE materials lose their ferroelectric character at the 2D limit due to depolarization field. Using angle resolved photoemission spectroscopy (ARPES), we unveil another unusual 2D phenomena appearing in 2H α-In$_{2}$Se$_{3}$ single crystals, the occurrence of a highly metallic two-dimensional electron gas (2DEG) at the surface of vacuum-cleaved crystals. This 2DEG exhibits two confined states which correspond to an electron density of approximatively 10$^{13}$ electrons/cm$^{3}$, also confirmed by thermoelectric measurements. Combination of ARPES and density functional theory (DFT) calculations reveals a direct band gap of energy equal to 1.3 +/- 0.1 eV, with the bottom of the conduction band localized at the center of the Brillouin zone, just below the Fermi level. Such strong n-type doping further supports the quantum confinement of electrons and the formation of the 2DEG.

cond-mat.mtrl-sci↗

Hydrogenic Spin-Valley states of the Bromine donor in 2H-MoTe$_2$

In semiconductors, the identification of doping atomic elements allowing to encode a qubit within spin states is of intense interest for quantum technologies. In transition metal dichalcogenides semiconductors, the strong spin-orbit coupling produces locked spin-valley states with expected long coherence time. Here we study the substitutional Bromine Br\textsubscript{Te} dopant in 2H-MoTe$_2$. Electron spin resonance measurements show that this dopant carries a spin with long-lived nanoseconds coherence time. Using scanning tunneling spectroscopy, we find that the hydrogenic wavefunctions associated with the dopant levels have characteristics spatial modulations that result from their hybridization to the \textbf{Q}-valleys of the conduction band. From a Fourier analysis of the conductance maps, we find that the amplitude and phase of the Fourier components change with energy according to the different irreducible representations of the impurity-site point-group symmetry. These results demonstrate that a dopant can inherit the locked spin-valley properties of the semiconductor and so exhibit long spin-coherence time.

cond-mat.mes-hall↗

Epitaxial van der Waals heterostructures of Cr2Te3 on 2D materials

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.

cond-mat.mtrl-sci↗

Unidirectional Rashba Spin Splitting in Single Layer WS$_{2(1-x)}$Se$_{2x}$ alloy

Atomically thin two-dimensional (2D) layered semiconductors such as transition metal dichalcogenides (TMDs) have attracted considerable attention due to their tunable band gap, intriguing spin-valley physics, piezoelectric effects and potential device applications. Here we study the electronic properties of a single layer WS$_{1.4}$Se$_{0.6}$ alloys. The electronic structure of this alloy, explored using angle resolved photoemission spectroscopy, shows a clear valence band structure anisotropy characterized by two paraboloids shifted in one direction of the k-space by a constant in-plane vector. This band splitting is a signature of a unidirectional Rashba spin splitting with a related giant Rashba parameter of 2.8 0.7 eV . The combination of angle resolved photoemission spectroscopy with piezo force microscopy highlights the link between this giant unidirectional Rashba spin splitting and an in-plane polarization present in the alloy. These peculiar anisotropic properties of the WS$_{1.4}$Se$_{0.6}$ alloy can be related to local atomic orders induced during the growth process due the different size and electronegativity between S and Se atoms. This distorted crystal structure combined to the observed macroscopic tensile strain, as evidenced by photoluminescence, displays electric dipoles with a strong in-plane component, as shown by piezoelectric microscopy. The interplay between semiconducting properties, in-plane spontaneous polarization and giant out-of-plane Rashba spin-splitting in this two-dimensional material has potential for a wide range of applications in next-generation electronics, piezotronics and spintronics devices.

cond-mat.mtrl-sci↗

Visualizing giant ferroelectric gating effects in large-scale WSe$_2$/BiFeO$_3$ heterostructures

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.

cond-mat.mtrl-sci↗

Electroluminescence of monolayer WS$_2$ in a scanning tunneling microscope: the effect of bias polarity on the spectral and angular distribution of the emitted light

Inelastic electron tunneling in a scanning tunneling microscope (STM) is used to generate excitons in monolayer tungsten disulfide (WS$_2$). Excitonic electroluminescence is measured both at positive and negative sample bias. Using optical spectroscopy and Fourier-space optical microscopy, we show that the bias polarity of the tunnel junction determines the spectral and angular distribution of the emitted light. At positive sample bias, only emission from excitonic species featuring an in-plane transition dipole moment is detected. Based on the spectral distribution of the emitted light, we infer that the dominant contribution is from charged excitons, i.e., trions. At negative sample bias, additional contributions from lower-energy excitonic species are evidenced in the emission spectra and the angular distribution of the emitted light reveals a mixed character of in-plane and out-of-plane transition dipole moments.

cond-mat.mes-hall↗

Evidence for Highly p-type doping and type II band alignment in large scale monolayer WSe2 /Se-terminated GaAs heterojunction grown by Molecular beam epitaxy

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.

cond-mat.mes-hall↗