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Fabrice Oehler

Publications and source records attributed to Fabrice Oehler.

18 recordsLinked to original sources

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

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

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

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

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

Hybridization and localized flat band in the WSe2/MoSe2 heterobilayer grown by molecular beam epitaxy

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.

cond-mat.mtrl-sci

Quantitative Assessment of Carrier Density by Cathodoluminescence. I. GaAs thin films and modeling

Doping is a fundamental property of semiconductors and constitutes the basis of modern microelectronic and optoelectronic devices. Their miniaturization requires contactless characterization of doping with nanometer scale resolution. Here, we use low- and room-temperature cathodoluminescence (CL) measurements to analyze p-type and n-type GaAs thin films over a wide range of carrier densities ($2\times 10^{17}$ to $1\times 10^{19}$ cm$^{-3}$). The spectral shift and broadening of CL spectra induced by shallow dopant states and band filling are the signature doping. We fit the whole spectral lineshapes with the generalized Planck's law and refined absorption models to extract the bandgap narrowing (BGN) and the band tail for both doping types, and the electron Fermi level for n doping. This work provides a rigorous method for the quantitative assessment of p-type and n-type carrier density using CL. Taking advantage of the high spatial resolution of CL, it can be used to map the doping in GaAs nanostructures, and it could be extended to other semiconductor materials.

cond-mat.mtrl-sci

Quantitative Assessment of Carrier Density by Cathodoluminescence. II. GaAs nanowires

Precise control of doping in single nanowires (NWs) is essential for the development of NW-based devices. Here, we investigate a series of MBE-grown GaAs NWs with Be (p-type) and Si (n-type) doping using high-resolution cathodoluminescence (CL) mapping at low- and room-temperature. CL spectra are analyzed selectively in different regions of the NWs. Room-temperature luminescence is fitted with the generalized Planck law and an absorption model, and the bandgap and band tail width are extracted. For Be-doped GaAs NWs, the bandgap narrowing provides a quantitative determination of the hole concentration ranging from about $1\times 10^{18}$ to $2\times 10^{19}$~cm$^{-3}$, in good agreement with the targeted doping levels. High-resolution maps of the hole concentration demonstrate the homogeneous doping in the pure zinc-blende segment. For Si-doped GaAs NWs, the electron Fermi level and the full-width at half maximum of low-temperature CL spectra are used to assess the electron concentration to approximately $3\times 10^{17}$ to $6\times 10^{17}$~cm$^{-3}$. These findings confirm the difficulty to obtain highly-doped n-type GaAs NWs, maybe due to doping compensation. Notably, signatures of high concentration (5--9$\times 10^{18}$~cm$^{-3}$) at the very top of NWs are unveiled.

cond-mat.mtrl-sci

Indirect to direct band gap crossover in two-dimensional WS2(1-x)Se2x alloys

In atomically thin transition metal dichalcogenide semiconductors, there is a crossover from indirect to direct bandgap as the thickness drops to one monolayer, which comes with a fast increase of the photoluminescence signal. Here, we show that for different alloy compositions of WS2(1-x)Se2x this trend may be significantly affected by the alloy content and we demonstrate that the sample with the highest Se ratio presents a strongly reduced effect. The highest micro-PL intensity is found for bilayer WS2(1-x)Se2x (x = 0.8) with a decrease of its maximum value by only a factor of 2 when passing from mono- to bi-layer. To better understand this factor and explore the layer-dependent band structure evolution of WS2(1-x)Se2x, we performed a nano-angle resolved photoemission spectroscopy study coupled with first-principles calculations. We find that the high micro-PL value for bilayer WS2(1-x)Se2x (x = 0.8) is due to the overlay of direct and indirect optical transitions. This peculiar high PL intensity in WS2(1-x)Se2x opens the way for spectrally tunable light-emitting devices.

cond-mat.mes-hall

Developing a Purely Visual Based Obstacle Detection using Inverse Perspective Mapping

Our solution is implemented in and for the frame of Duckietown. The goal of Duckietown is to provide a relatively simple platform to explore, tackle and solve many problems linked to autonomous driving. "Duckietown" is simple in the basics, but an infinitely expandable environment. From controlling single driving Duckiebots until complete fleet management, every scenario is possible and can be put into practice. So far, none of the existing modules was capable of reliably detecting obstacles and reacting to them in real time. We faced the general problem of detecting obstacles given images from a monocular RGB camera mounted at the front of our Duckiebot and reacting to them properly without crashing or erroneously stopping the Duckiebot. Both, the detection as well as the reaction have to be implemented and have to run on a Raspberry Pi in real time. Due to the strong hardware limitations, we decided to not use any learning algorithms for the obstacle detection part. As it later transpired, a working "hard coded" software needs thorough analysis and understanding of the given problem. In layman's terms, we simply seek to make Duckietown a safer place.

cs.RO

Interface Dipole and Band Bending in Hybrid p-n Heterojunction MoS2/GaN(0001)

Hybrid heterostructures based on bulk GaN and two-dimensional (2D) materials offer novel paths toward nanoelectronic devices with engineered features. Here, we study the electronic properties of a mixed-dimensional heterostructure composed of intrinsic n-doped MoS2 flakes transferred on p-doped GaN(0001) layers. Based on angle-resolved photoemission spectroscopy (ARPES) and high resolution X-ray photoemission spectroscopy (HR-XPS), we investigate the electronic structure modification induced by the interlayer interactions in MoS2/GaN heterostructure. In particular, a shift of the valence band with respect to the Fermi level for MoS2/GaN heterostructure is observed; which is the signature of a charge transfer from the 2D monolayer MoS2 to GaN. ARPES and HR-XPS revealed an interface dipole associated with local charge transfer from the GaN layer to the MoS2 monolayer. Valence and conduction band offsets between MoS2 and GaN are determined to be 0.77 and -0.51 eV, respectively. Based on the measured work functions and band bendings, we establish the formation of an interface dipole between GaN and MoS2 of 0.2 eV.

cond-mat.mtrl-sci

Non-polar (11-20) InGaN quantum dots with short exciton lifetimes grown by metal-organic vapor phase epitaxy

We report on the optical characterization of non-polar a-plane InGaN quantum dots (QDs) grown by metal-organic vapor phase epitaxy using a short nitrogen anneal treatment at the growth temperature. Spatial and spectral mapping of sub-surface QDs have been achieved by cathodoluminescence at 8 K. Microphotoluminescence studies of the QDs reveal resolution limited sharp peaks with typical linewidth of 1 meV at 4.2 K. Time-resolved photoluminescence studies suggest the excitons in these QDs have a typical lifetime of 538 ps, much shorter than that of the c-plane QDs, which is strong evidence of the significant suppression of the internal electric fields.

cond-mat.mtrl-sci