Atomic-Layer Controlled Transition from Inverse Rashba-Edelstein Effect to Inverse Spin Hall Effect in 2D PtSe2 Probed by THz Spintronic Emission.

2D materials, such as transition metal dichalcogenides, are ideal platforms for spin-to-charge conversion (SCC) as they possess strong spin-orbit coupling (SOC), reduced dimensionality and crystal symmetries as well as tuneable band structure, compared to metallic structures. Moreover, SCC can be tuned with the number of layers, electric field, or strain. Here, SCC in epitaxially grown 2D PtSe2 by THz spintronic emission is studied since its 1T crystal symmetry and strong SOC favor SCC. High quality of as-grown PtSe2 layers is demonstrated, followed by in situ ferromagnet deposition by sputtering that leaves the PtSe2 unaffected, resulting in well-defined clean interfaces as evidenced with extensive characterization. Through this atomic growth control and using THz spintronic emission, the unique thickness-dependent electronic structure of PtSe2 allows the control of SCC. Indeed, the transition from the inverse Rashba-Edelstein effect (IREE) in 1-3 monolayers (ML) to the inverse spin Hall effect (ISHE) in multilayers (>3 ML) of PtSe2 enabling the extraction of the perpendicular spin diffusion length and relative strength of IREE and ISHE is demonstrated. This band structure flexibility makes PtSe2 an ideal candidate to explore the underlying mechanisms and engineering of the SCC as well as for the development of tuneable THz spintronic emitters.

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 a rhombohedral-stacked bilayer (AB stacking) can be obtained by molecular beam epitaxy growth of tungsten diselenide (WSe2) on a 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 a GaP(111)B substrate. Our ARPES measurements confirm the expected valence band structure of WSe2 with the band maximum located at the Γ point of the Brillouin zone. The epitaxial growth of WSe2/GaP(111)B helps to understand the fundamental properties of these 2D/3D heterostructures, toward their implementation in future devices.

Reconfigurable Multifunctional van der Waals Ferroelectric Devices and Logic Circuits.

Emerging reconfigurable devices are fast gaining popularity in the search for next-generation computing hardware, while ferroelectric engineering of the doping state in semiconductor materials has the potential to offer alternatives to traditional von-Neumann architecture. In this work, we combine these concepts and demonstrate the suitability of reconfigurable ferroelectric field-effect transistors (Re-FeFETs) for designing nonvolatile reconfigurable logic-in-memory circuits with multifunctional capabilities. Modulation of the energy landscape within a homojunction of a 2D tungsten diselenide (WSe2) layer is achieved by independently controlling two split-gate electrodes made of a ferroelectric 2D copper indium thiophosphate (CuInP2S6) 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 106 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 104. 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 a long retention time exceeding 104 s. 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 nonvolatile 2-input logic functions. Moreover, the Re-FeFET circuit demonstrates high 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 promising 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.

Quantum Confinement and Electronic Structure at the Surface of van der Waals Ferroelectric α-In2Se3.

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-In2Se3 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 the depolarization field. Using angle resolved photoemission spectroscopy (ARPES), we unveil another unusual 2D phenomenon appearing in 2H α-In2Se3 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 approximately 1013 electrons/cm2, 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.

High p doped and robust band structure in Mg-doped hexagonal boron nitride.

In two dimensional materials, substitutional doping during growth can be used to alter the electronic properties. Here, we report on the stable growth of p-type hexagonal boron nitride (h-BN) using Mg-atoms as substitutional impurities in the h-BN honeycomb lattice. We use micro-Raman spectroscopy, angle-resolved photoemission measurements (nano-ARPES) and Kelvin probe force microscopy (KPFM) to study the electronic properties of Mg-doped h-BN grown by solidification from a ternary Mg-B-N system. Besides the observation of a new Raman line at ∼1347 cm-1 in Mg-doped h-BN, nano-ARPES reveals p-type carrier concentration. Our nano-ARPES experiments demonstrate that the Mg dopants can significantly alter the electronic properties of h-BN by shifting the valence band maximum about 150 meV toward higher binding energies with respect to pristine h-BN. We further show that, Mg doped h-BN exhibits a robust, almost unaltered, band structure compared to pristine h-BN, with no significant deformation. Kelvin probe force microscopy (KPFM) confirms the p-type doping, with a reduced Fermi level difference between pristine and Mg-doped h-BN crystals. Our findings demonstrate that conventional semiconductor doping by Mg as substitutional impurities is a promising route to high-quality p-type doped h-BN films. Such stable p-type doping of large band h-BN is a key feature for 2D materials applications in deep ultra-violet light emitting diodes or wide bandgap optoelectronic devices.

Photoferroelectric All-van-der-Waals Heterostructure for Multimode Neuromorphic Ferroelectric Transistors.

Interface-driven effects in ferroelectric van der Waals (vdW) heterostructures provide fresh opportunities in the search for alternative device architectures toward overcoming the von Neumann bottleneck. However, their implementation is still in its infancy, mostly by electrical control. It is of utmost interest to develop strategies for additional optical and multistate control in the quest for novel neuromorphic architectures. Here, we demonstrate the electrical and optical control of the ferroelectric polarization states of ferroelectric field effect transistors (FeFET). The FeFETs, fully made of ReS2/hBN/CuInP2S6 vdW materials, achieve an on/off ratio exceeding 107, a hysteresis memory window up to 7 V wide, and multiple remanent states with a lifetime exceeding 103 s. Moreover, the ferroelectric polarization of the CuInP2S6 (CIPS) layer can be controlled by photoexciting the vdW heterostructure. We perform wavelength-dependent studies, which allow for identifying two mechanisms at play in the optical control of the polarization: band-to-band photocarrier generation into the 2D semiconductor ReS2 and photovoltaic voltage into the 2D ferroelectric CIPS. Finally, heterosynaptic plasticity is demonstrated by operating our FeFET in three different synaptic modes: electrically stimulated, optically stimulated, and optically assisted synapse. Key synaptic functionalities are emulated including electrical long-term plasticity, optoelectrical plasticity, optical potentiation, and spike rate-dependent plasticity. The simulated artificial neural networks demonstrate an excellent accuracy level of 91% close to ideal-model synapses. These results provide a fresh background for future research on photoferroelectric vdW systems and put ferroelectric vdW heterostructures on the roadmap for the next neuromorphic computing architectures.

Visualizing Giant Ferroelectric Gating Effects in Large-Scale WSe2/BiFeO3 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 BiFeO3, a room-temperature multiferroic oxide, and WSe2, a semiconducting two-dimensional material with potential for photovoltaics and photonics. WSe2 is grown by molecular beam epitaxy and transferred on a centimeter-scale onto BiFeO3 films. Using angle-resolved photoemission spectroscopy, we visualize the electronic structure of 1 to 3 monolayers of WSe2 and evidence a giant energy shift as large as 0.75 eV induced by the ferroelectric polarization direction in the underlying BiFeO3. Such a strong shift opens new perspectives in the efficient manipulation of TMD properties by proximity effects.

Unidirectional Rashba spin splitting in single layer WS2(1-x)Se2xalloy.

Atomically thin two-dimensional (2D) layered semiconductors such as transition metal dichalcogenides 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 WS1.4Se0.6alloys. 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 thek-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 Å. 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 WS1.4Se0.6alloy 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 2D material has potential for a wide range of applications in next-generation electronics, piezotronics and spintronics devices.

Hybridization and localized flat band in the WSe2/MoSe2heterobilayer.

Nearly localized moiré 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 WSe2/MoSe2heterobilayer grown by molecular beam epitaxy. This flat band is localized near the Fermi level and has a width of several hundred meVs. By combining ARPES measurements with density functional theory 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 atKis determined to be 470 meV. The valence band maximum (VBM) position of the heterobilayer is located at the Γ point. The energy difference between the VBM at Γ and theKpoint is of -60 meV, which is a stark difference compared to individual single monolayer WSe2and monolayer WSe2, showing both a VBM atK.

Vanishing Confinement Regime in Terahertz HgTe Nanocrystals Studied under Extreme Conditions of Temperature and Pressure.

While HgTe nanocrystals (NCs) in the mid-infrared region have reached a high level of maturity, their far-infrared counterparts remain far less studied, raising the need for an in-depth investigation of the material before efficient device integration can be considered. Here, we explore the effect of temperature and pressure on the structural, spectroscopic, and transport properties of HgTe NCs displaying an intraband absorption at 10 THz. The temperature leads to a very weak modulation of the spectrum as opposed to what was observed for strongly confined HgTe NCs. HgTe NC films present ambipolar conduction with a clear prevalence of electron conduction as confirmed by transistor and thermoelectric measurements. Under the application of pressure, the material undergoes phase transitions from the zinc blende to cinnabar phase and later to the rock salt phase which we reveal using joint X-ray diffraction and infrared spectroscopy measurements. We discuss how the pressure existence domain of each phase is affected by the particle size.

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 upshift of about 0.56 eV toward the Fermi level with respect to the VBM of the WSe2 on graphene layer, which is indicative of high p-type doping and a key feature for applications in nanoelectronics and optoelectronics.

Strain and Spin-Orbit Coupling Engineering in Twisted WS2/Graphene Heterobilayer.

The strain in hybrid van der Waals heterostructures, made of two distinct two-dimensional van der Waals materials, offers an interesting handle on their corresponding electronic band structure. Such strain can be engineered by changing the relative crystallographic orientation between the constitutive monolayers, notably, the angular misorientation, also known as the "twist angle". By combining angle-resolved photoemission spectroscopy with density functional theory calculations, we investigate here the band structure of the WS2/graphene heterobilayer for various twist angles. Despite the relatively weak coupling between WS2 and graphene, we demonstrate that the resulting strain quantitatively affects many electronic features of the WS2 monolayers, including the spin-orbit coupling strength. In particular, we show that the WS2 spin-orbit splitting of the valence band maximum at K can be tuned from 430 to 460 meV. Our findings open perspectives in controlling the band dispersion of van der Waals materials.

Phase Transition in a Memristive Suspended MoS2 Monolayer Probed by Opto- and Electro-Mechanics.

Semiconducting monolayers of a 2D material are able to concatenate multiple interesting properties into a single component. Here, by combining opto-mechanical and electronic measurements, we demonstrate the presence of a partial 2H-1T' phase transition in a suspended 2D monolayer membrane of MoS2. Electronic transport shows unexpected memristive properties in the MoS2 membrane, in the absence of any external dopants. A strong mechanical softening of the membrane is measured concurrently and may only be related to the 2H-1T' phase transition, which imposes a 3% directional elongation of the topological 1T' phase with respect to the semiconducting 2H. We note that only a few percent 2H-1T' phase switching is sufficient to observe measurable memristive effects. Our experimental results combined with first-principles total energy calculations indicate that sulfur vacancy diffusion plays a key role in the initial nucleation of the phase transition. Our study clearly shows that nanomechanics represents an ultrasensitive technique to probe the crystal phase transition in 2D materials or thin membranes. Finally, a better control of the microscopic mechanisms responsible for the observed memristive effect in MoS2 is important for the implementation of future devices.

Reconfigurable 2D/0D p-n Graphene/HgTe Nanocrystal Heterostructure for Infrared Detection.

Nanocrystals are promising building blocks for the development of low-cost infrared optoelectronics. Gating a nanocrystal film in a phototransistor geometry is commonly proposed as a strategy to tune the signal-to-noise ratio by carefully controlling the carrier density within the semiconductor. However, the performance improvement has so far been quite marginal. With metallic electrodes, the gate dependence of the photocurrent follows the gate-induced change of the dark current. Graphene presents key advantages: (i) infrared transparency that allows back-side illumination, (ii) vertical electric field transparency, and (iii) carrier selectivity under gate bias. Here, we investigate a configuration of 2D/0D infrared photodetectors taking advantage of a high capacitance ionic glass gate, large-scale graphene electrodes, and a HgTe nanocrystals layer of high carrier mobility. The introduction of graphene electrodes combined with ionic glass enables one to reconfigure selectively the HgTe nanocrystals and the graphene electrodes between electron-doped (n) and hole-doped (p) states. We unveil that this functionality enables the design a 2D/0D p-n junction that expands throughout the device, with a built-in electric field that assists charge dissociation. We demonstrate that, in this specific configuration, the signal-to-noise ratio for infrared photodetection can be enhanced by 2 orders of magnitude, and that photovoltaic operation can be achieved. The detectivity now reaches 109 Jones, whereas the device only absorbs 8% of the incident light. Additionally, the time response of the device is fast (<10 µs), which strongly contrasts with the slow response commonly observed for 2D/0D mixed-dimensional heterostructures, where larger photoconduction gains come at the cost of slower response.

Field-Effect Transistor and Photo-Transistor of Narrow-Band-Gap Nanocrystal Arrays Using Ionic Glasses.

The gating of nanocrystal films is currently driven by two approaches: either the use of a dielectric such as SiO2 or the use of electrolyte. SiO2 allows fast bias sweeping over a broad range of temperatures but requires a large operating bias. Electrolytes, thanks to large capacitances, lead to the significant reduction of operating bias but are limited to slow and quasi-room-temperature operation. None of these operating conditions are optimal for narrow-band-gap nanocrystal-based phototransistors, for which the necessary large-capacitance gate has to be combined with low-temperature operation. Here, we explore the use of a LaF3 ionic glass as a high-capacitance gating alternative. We demonstrate for the first time the use of such ionic glasses to gate thin films made of HgTe and PbS nanocrystals. This gating strategy allows operation in the 180 to 300 K range of temperatures with capacitance as high as 1 µF·cm-2. We unveil the unique property of ionic glass gate to enable the unprecedented tunability of both magnitude and dynamics of the photocurrent thanks to high charge-doping capability within an operating temperature window relevant for infrared photodetection. We demonstrate that by carefully choosing the operating gate bias, the signal-to-noise ratio can be improved by a factor of 100 and the time response accelerated by a factor of 6. Moreover, the good transparency of LaF3 substrate allows back-side illumination in the infrared range, which is highly valuable for the design of phototransistors.

Wave-Function Engineering in HgSe/HgTe Colloidal Heterostructures To Enhance Mid-infrared Photoconductive Properties.

The use of intraband transition is an interesting alternative path for the design of optically active complex colloidal materials in the mid-infrared range. However, so far, the performance obtained for photodetection based on intraband transition remains much smaller than the one relying on interband transition in narrow-band-gap materials operating at the same wavelength. New strategies have to be developed to make intraband materials more effective. Here, we propose growing a heterostructure of HgSe/HgTe as a means of achieving enhanced intraband-based photoconduction. We first tackle the synthetic challenge of growing a heterostructure on soft (Hg-based) material. The electronic spectrum of the grown heterostructure is then investigated using a combination of numerical simulation, infrared spectroscopy, transport measurement, and photoemission. We report a type-II band alignment with reduced doping compared with a core-only object and boosted hole conduction. Finally, we probe the photoconductive properties of the heterostructure while resonantly exciting the intraband transition by using a high-power-density quantum cascade laser. Compared to the previous generation of material based on core-only HgSe, the heterostructures have a lower dark current, stronger temperature dependence, faster photoresponse (with a time response below 50 µs), and detectivity increased by a factor of 30.

Intrinsic Properties of Suspended MoS2 on SiO2/Si Pillar Arrays for Nanomechanics and Optics.

Semiconducting two-dimensional (2D) materials, such as transition-metal dichalcogenides (TMDs), are emerging in nanomechanics, optoelectronics, and thermal transport. In each of these fields, perfect control over 2D material properties including strain, doping, and heating is necessary, especially on the nanoscale. Here, we study clean devices consisting of membranes of single-layer MoS2 suspended on pillar arrays. Using Raman and photoluminescence spectroscopy, we have been able to extract, separate, and simulate the different contributions on the nanoscale and to correlate these to the pillar array design. This control has been used to design a periodic MoS2 mechanical membrane with a high reproducibility and to perform optomechanical measurements on arrays of similar resonators with a high-quality factor of 600 at ambient temperature, hence opening the way to multiresonator applications with 2D materials. At the same time, this study constitutes a reference for the future development of well-controlled optical emissions within 2D materials on periodic arrays with reproducible behavior. We measured a strong reduction of the MoS2 band gap induced by the strain generated from the pillars. A transition from direct to indirect band gap was observed in isolated tent structures made of MoS2 and pinched by a pillar. In fully suspended devices, simulations were performed allowing both the extraction of the thermal conductance and doping of the layer. Using the correlation between the influences of strain and doping on the MoS2 Raman spectrum, we have developed a simple, elegant method to extract the local strain in suspended and nonsuspended parts of a membrane. This opens the way to experimenting with tunable coupling between light emission and vibration.

HgSe Self-Doped Nanocrystals as a Platform to Investigate the Effects of Vanishing Confinement.

Self-doped colloidal quantum dots (CQDs) attract a strong interest for the design of a new generation of low-cost infrared (IR) optoelectronic devices because of their tunable intraband absorption feature in the mid-IR region. However, very little remains known about their electronic structure which combines confinement and an inverted band structure, complicating the design of optimized devices. We use a combination of IR spectroscopy and photoemission to determine the absolute energy levels of HgSe CQDs with various sizes and surface chemistries. We demonstrate that the filling of the CQD states ranges from 2 electrons per CQD at small sizes (<5 nm) to more than 18 electrons per CQD at large sizes (≈20 nm). HgSe CQDs are also an interesting platform to observe vanishing confinement in colloidal nanoparticles. We present lines of evidence for a semiconductor-to-metal transition at the CQD level, through temperature-dependent absorption and transport measurements. In contrast with bulk systems, the transition is the result of the vanishing confinement rather than the increase of the doping level.

Charge Dynamics and Optolectronic Properties in HgTe Colloidal Quantum Wells.

We investigate the electronic and transport properties of HgTe 2D colloidal quantum wells. We demonstrate that the material can be made p- or n-type depending on the capping ligands. In addition to the control of majority carrier type, the surface chemistry also strongly affects the photoconductivity of the material. These transport measurements are correlated with the electronic structure determined by high resolution X-ray photoemission. We attribute the change of majority carriers to the strong hybridization of an n-doped HgS layer resulting from capping the HgTe nanoplatelets by S2- ions. We further investigate the gate and temperature dependence of the photoresponse and its dynamics. We show that the photocurrent rise and fall times can be tuned from 100 µs to 1 ms using the gate bias. Finally, we use time-resolved photoemission spectroscopy as a probe of the transport relaxation to determine if the observed dynamics are limited by a fundamental process such as trapping. These pump probe surface photovoltage measurements show an even faster relaxation in the 100-500 ns range, which suggests that the current performances are rather limited by geometrical factors.

Tunable Doping in Hydrogenated Single Layered Molybdenum Disulfide.

Structural defects in the molybdenum disulfide (MoS2) monolayer are widely known for strongly altering its properties. Therefore, a deep understanding of these structural defects and how they affect MoS2 electronic properties is of fundamental importance. Here, we report on the incorporation of atomic hydrogen in monolayered MoS2 to tune its structural defects. We demonstrate that the electronic properties of single layer MoS2 can be tuned from the intrinsic electron (n) to hole (p) doping via controlled exposure to atomic hydrogen at room temperature. Moreover, this hydrogenation process represents a viable technique to completely saturate the sulfur vacancies present in the MoS2 flakes. The successful incorporation of hydrogen in MoS2 leads to the modification of the electronic properties as evidenced by high resolution X-ray photoemission spectroscopy and density functional theory calculations. Micro-Raman spectroscopy and angle resolved photoemission spectroscopy measurements show the high quality of the hydrogenated MoS2 confirming the efficiency of our hydrogenation process. These results demonstrate that the MoS2 hydrogenation could be a significant and efficient way to achieve tunable doping of transition metal dichalcogenides (TMD) materials with non-TMD elements.