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Stacking monolayers of transition metal dichalcogenides (TMDs) has led to the discovery of a plethora of new exotic phenomena, resulting from moir\'e pattern formation. Due to the atomic thickness and high surface-to-volume ratio of heterostructures, the interfaces play a crucial role. Fluctuations in the interlayer distance affect interlayer coupling and moir\'e effects. Therefore, to access the intrinsic properties of the TMD stack, it is essential to obtain a clean and uniform interface between the layers. Here, we show that this is achieved by ironing with the tip of an atomic force microscope. This post-stacking procedure dramatically improves the homogeneity of the interfaces, which is reflected in the optical response of the interlayer exciton. We demonstrate that ironing improves the layer coupling, enhancing moir\'e effects and reducing disorder. This is crucial for the investigation of TMD heterostructure physics, which currently suffers from low reproducibility.

This teaching article describes a simple and low-cost methodology for studying electrical transport and constructing basic sensor devices using everyday stationery items, including pencils, paper, and a handheld multimeter. The approach is designed for high school and undergraduate teachers and offers an easy-to-implement, hands-on method for teaching fundamental concepts in physical electronics. The materials and experiments outlined in this article are widely accessible and can be easily replicated in various teaching labs, even with limited budgets.

We present the electrostatic control of photoluminescence of monolayer MoS$_2$ at room temperature via integration of free-standing BaTiO$_3$ (BTO), a ferroelectric perovskite oxide, layers. We show that the use of BTO leads to highly tunable exciton emission of MoS$_2$ in a minimal range of gate voltages, effectively controlling the neutral excitons to charged excitons (trions) conversion. Due to BTO's ferroelectric polarization-induced doping we observe large peak emission shifts as well as a large and tunable A trion binding energy in the range of 40-100 meV. To further investigate the efficacy of electrostatic control, we compared our measurements with those carried out when the BTO is replaced by a hexagonal boron nitride (hBN) dielectric layer of comparable thickness, confirming BTO's superior gating properties and thus lower power consumption. Additionally, we take advantage of the ferroelectric switching of BTO by fabricating devices where the BTO layer is decoupled from the gate electrode with a SiO$_2$ layer. Choosing to isolate the BTO allows us to induce large remanent behavior of MoS$_2$'s excitonic features, observing hysteretic behavior in the peak energy ratio between A exciton and its trion, as well as hysteretic behavior in the doping-related trion energy shift. This study illustrates the rich physics involved in combining free-standing complex oxide layers with two-dimensional materials.

Two-dimensional (2D) materials are widely used in various applications due to their extraordinary properties. In particular, their electrochemical stability, low electrical resistance, and huge specific surface area make them very interesting active materials for supercapacitors. Herein, flexible, biodegradable, and low-cost supercapacitors are introduced in a very simple way based on hand-drawing pencil traces or -rubbing molybdenum disulfide (MoS2), titanium trisulfide (TiS3) and franckeite traces on the paper. Results demonstrate that pencil-drawn paper has higher capacitance performance (~6.39 F/g) among the suggested electrodes. Interestingly, the introduced MoS2/pencil, TiS3/pencil, and franckeite/pencil drawn paper electrodes reveal dramatic improvements with long cyclic life thanks to the occurrence of synergetic effects and higher available active cites within the heterostructures. Moreover, the assembled symmetric solid-state supercapacitors retain their performance even under applied bending, indicating their excellent potential for wearable/flexible applications.

This work presents an automated three-point bending apparatus that can be used to study strain engineering and straintronics in two-dimensional materials. We benchmark the system by reporting reproducible strain tuned micro-reflectance, Raman, and photoluminescence spectra for monolayer molybdenum disulfide (MoS2). These results are in good agreement with reported literature using conventional bending apparatus. We further utilize the system to automate strain investigations of straintronic devices by measuring the piezoresistive effect and the strain effect on photoresponse in an MoS2 electrical device. The details of the construction of the straightforward system are given and we anticipate it can be easily implemented for study of strain engineering and straintronics in a wide variety of 2D material systems.

We study the effect of uniaxial strain on the band structure of ZrSe$_3$, a semiconducting material with a marked in-plane structural anisotropy. By using a modified 3-point bending test apparatus, thin ZrSe$_3$ flakes were subjected to uniaxial strain along different crystalline orientations monitoring the effect of strain on their optical properties through micro-reflectance spectroscopy. The obtained spectra showed excitonic features that blueshift upon uniaxial tension. This shift is strongly dependent on the direction along which the strain is being applied. When the flakes are strained along the b-axis, the exciton peak shifts at ~ 60-95 meV/%, while along the a-axis, the shift only reaches ~ 0-15 meV/%. Ab initio calculations were conducted to study the influence of uniaxial strain, applied along different crystal directions, on the band structure and reflectance spectra of ZrSe$_3$, exhibiting a remarkable agreement with the experimental results.

Two-dimensional materials are attractive for constructing high-performance photonic chip-integrated photodetectors because of their remarkable electronic and optical properties and dangling-bond-free surfaces. However, the reported chip-integrated two-dimensional material photodetectors were mainly implemented with the configuration of metal-semiconductor-metal, suffering from high dark currents and low responsivities at high operation speed. Here, we report a van der Waals PN heterojunction photodetector, composed of p-type black phosphorous and n-type molybdenum telluride, integrated on a silicon nitride waveguide. The built-in electric field of the PN heterojunction significantly suppresses the dark current and improves the responsivity. Under a bias of 1 V pointing from n-type molybdenum telluride to p-type black phosphorous, the dark current is lower than 7 nA, which is more than two orders of magnitude lower than those reported in other waveguide-integrated black phosphorus photodetectors. An intrinsic responsivity up to 577 mA/W is obtained. Remarkably, the van der Waals PN heterojunction is tunable by the electrostatic doping to further engineer its rectification and improve the photodetection, enabling an increased responsivity of 709 mA/W. Besides, the heterojunction photodetector exhibits a response bandwidth of ~1.0 GHz and a uniform photodetection over a wide spectral range, as experimentally measured from 1500 to 1630 nm. The demonstrated chip-integrated van der Waals PN heterojunction photodetector with low dark current, high responsivity and fast response has great potentials to develop high-performance on-chip photodetectors for various photonic integrated circuits based on silicon, lithium niobate, polymer, etc.

Paper offers a low-cost and widely available substrate for electronics. It posses alternative characteristics to silicon, as it shows low density and high-flexibility, together with biodegradability. Solution processable materials, such as hybrid perovskites, also present light and flexible features, together with a huge tunability of the material composition with varying optical properties. In this study, we combine paper substrates with halide-mixed perovskites for the creation of low-cost and easy-to-fabricate perovskite-on-paper photodetectors with a broadband-tunable spectral response. From the bandgap tunability of halide-mixed perovskites we create photodetectors with a cut-off spectral onset that ranges from the NIR to the green, by increasing the bromide content on MAPb(I$_{1-x}$Br$_x$)$_3$ perovskite alloys. The devices show a fast and efficient response. The best performances are observed for the pure I and Br perovskite compositions, with a maximum responsivity of 376 mA/W on the MAPbBr$_3$ device. This study provides an example of the wide range of possibilities that the combination of solution processable materials with paper substrates offer for the development of low-cost, biodegradable and easy-to-fabricate devices., Comment: 3 main text figures, 8 supp info figures

Molybdenum trioxide (MoO$_3$) in-plane anisotropy has increasingly attracted the attention of the scientific community in the last few years. Many of the observed in-plane anisotropic properties stem from the anisotropic refractive index and elastic constants of the material but a comprehensive analysis of these fundamental properties is still lacking. Here we employ Raman and micro-reflectance measurements, using polarized light, to determine the angular dependence of the refractive index of thin MoO$_3$ flakes and we study the directional dependence of the MoO$_3$ Young's modulus using the buckling metrology method. We found that MoO$_3$ displays one of the largest in-plane anisotropic mechanical properties reported for 2D materials so far., Comment: 4 figures in main text. 6 figures in supp. info

Paper holds the promise to replace silicon substrates in applications like internet of things or disposable electronics that require ultra-low-cost electronic components and an environmentally friendly electronic waste management. In the last years, spurred by the abovementioned properties of paper as a substrate and the exceptional electronic, mechanical and optical properties of van der Waals (vdW) materials, many research groups have worked towards the integration of vdW materials-based devices on paper. Recently, a method to deposit a continuous film of densely packed interconnects of vdW materials on paper by simply rubbing the vdW crystals against the rough surface of paper has been presented. This method utilizes the weak interlayer vdW interactions and allows cleaving of the crystals into micro platelets through the abrasion against the paper. Here, we aim to illustrate the general character and the potential of this technique by fabricating films of 39 different vdW materials (including superconductors, semi-metals, semiconductors, and insulators) on standard copier paper. We have thoroughly characterized their optical properties showing their high optical quality: one can easily resolve the absorption band edge of semiconducting vdW materials and even the excitonic features present in some vdW materials with high exciton binding energy. We also measured the electrical resistivity for several vdW materials films on paper finding exceptionally low values, which are in some cases, orders of magnitude lower than those reported for analogous films produced by inkjet printing. We finally demonstrate the fabrication of field-effect devices with vdW materials on paper using the paper substrate as an ionic gate., Comment: 4 figures in main text, 21 figures in Supp. Info

We have implemented three different optical methods to quantitatively assess the thickness of thin GaSe flakes transferred on both transparent substrates, like Gel-Film, or SiO2/Si substrates. We show how their apparent color can be an efficient way to make a quick rough estimation of the thickness of the flakes. This method is more effective for SiO2/Si substrates as the thickness dependent color change is more pronounced on these substrates than on transparent substrates. On the other hand, for transparent substrates, the transmittance of the flakes in the blue region of the visible spectrum can be used to estimate the thickness. We find that the transmittance of flakes in the blue part of the spectrum decreases at a rate of 1.2%/nm. On SiO2/Si, the thickness of the flakes can be accurately determined by fitting optical contrast spectra to a Fresnel law-based model. Finally, we also show how the quantitative analysis of transmission mode optical microscopy images can be a powerful method to quickly probe the environmental degradation of GaSe flakes exposed to aging conditions., Comment: 5 figures

Paper has the potential to dramatically reduce the cost of electronic components. In fact, paper is 10 000 times cheaper than crystalline silicon, motivating the research to integrate electronic materials on paper substrates. Among the different electronic materials, van der Waals materials are attracting the interest of the scientific community working on paper-based electronics because of the combination of high electrical performance and mechanical flexibility. Up to now, different methods have been developed to pattern conducting, semiconducting and insulating van der Waals materials on paper but the integration of superconductors remains elusive. Here, the deposition of NbSe2, an illustrative van der Waals superconductor, on standard copy paper is demonstrated. The deposited NbSe2 films on paper display superconducting properties (e.g. observation of Meissner effect and resistance drop to zero-resistance state when cooled down below its critical temperature) similar to those of bulk NbSe2., Comment: 6 figures in main text, 8 figures in Supp. Info

Strain engineering has arisen as a powerful technique to tune the electronic and optical properties of two-dimensional semiconductors like molybdenum disulfide (MoS2). Although several theoretical works predicted that biaxial strain would be more effective than uniaxial strain to tune the band structure of MoS2, a direct experimental verification is still missing in the literature. Here we implemented a simple experimental setup that allows to apply biaxial strain through the bending of a cruciform polymer substrate. We used the setup to study the effect of biaxial strain on the differential reflectance spectra of 12 single-layer MoS2 flakes finding a redshift of the excitonic features at a rate between -40 meV/% and -110 meV/% of biaxial tension. We also directly compare the effect of biaxial and uniaxial strain on the same single-layer MoS2 finding that the biaxial strain gauge factor is 2.3 times larger than the uniaxial strain one., Comment: 5 figures + 1 table in the main text. 6 figures in the supp. info

Two-dimensional layered trichalcogenide materials have recently attracted the attention of the scientific community because of its robust mechanical, thermal properties and applications in opto and nanoelectronics devices. We report the pressure dependence of out-of plane Ag Raman modes in high quality few-layers titanium trisulfide (TiS3) nanoribbons grown using a direct solid-gas reaction method and infer their cross-plane thermal expansion coefficient.Both mechanical stability and thermal properties of the TiS3 nanoribbons are elucidated using phonon-spectrum analyses. Raman spectroscopic studies at high pressure (up to 34 GPa) using a diamond anvil cell identify four prominent Ag Raman bands; a band at 557 cm-1 softens under compression, and others at 175, 300, and 370 cm-1 show normal hardening. Anomalies in phonon mode frequencies and excessive broadening in line-width of the soft phonon about ~ 13 GPa are attributed to the possible onset of a reversible structural transition. A complete structural phase transition at 43 GPa is inferred from Ag soft mode frequency (557 cm-1) versus pressure extrapolation curve, consistent with recent reported theoretical predictions. Using the experimental mode Gr\"uneisen parameters i of Raman modes, the cross-plane thermal expansion coefficient Cv of the TiS3 nanoribbons at ambient phase is estimated to be1.32110-6K-1. The observed results are expected to be useful in calibration and performance of next generation nano-electronics and optical devices under extreme stress conditions.

Symmetry breaking in two-dimensional layered materials plays a significant role in their macroscopic electrical, optical, magnetic and topological properties, including but not limited to spin-polarization effects, valley-contrasting physics, nonlinear Hall effects, nematic order, ferroelectricity, Bose-Einstein condensation and unconventional superconductivity. Engineering symmetry breaking of two-dimensional layered materials not only offers extraordinary opportunities to tune their physical properties, but also provides unprecedented possibilities to introduce completely new physics and technological innovations in electronics, photonics and optoelectronics. Indeed, over the past 15 years, a wide variety of physical, structural and chemical approaches have been developed to engineer symmetry breaking of two-dimensional layered materials. In this Review, we focus on the recent progresses on engineering the breaking of inversion, rotational, time reversal and spontaneous gauge symmetries in two-dimensional layered materials, and illustrate our perspectives on how these may lead to potential new physics and applications., Comment: 35 pages, 4 figures

The exfoliation of two naturally occurring van der Waals minerals, graphite and molybdenite, arouse an unprecedented level of interest by the scientific community and shaped a whole new field of research: 2D materials research. Several years later, the family of van der Waals materials that can be exfoliated to isolate 2D materials keeps growing, but most of them are synthetic. Interestingly, in nature plenty of naturally occurring van der Waals minerals can be found with a wide range of chemical compositions and crystal structures whose properties are mostly unexplored so far. This Perspective aims to provide an overview of different families of van der Waals minerals to stimulate their exploration in the 2D limit., Comment: Perspective article. 34 pages, 10 figures, 1 table, more than 170 references

Paper based thermoresistive sensors are fabricated by rubbing WS2 powder against a piece of standard copier paper, like the way a pencil is used to write on paper. The abrasion between the layered material and the rough paper surface erodes the material, breaking the weak van der Waals interlayer bonds, yielding a film of interconnected platelets. The resistance of WS2 presents a strong temperature dependence, as expected for a semiconductor material in which charge transport is due to thermally activated carriers. This strong temperature dependence makes the paper supported WS2 devices extremely sensitive to small changes in temperature. This exquisite thermal sensitivity, and their fast response times to sudden temperature changes, is exploited thereby demonstrating the usability of a WS2-on-paper thermal sensor in a respiration monitoring device., Comment: 6 main text figures, 1 table, 6 supp. info. figures

Metal halide perovskites are known to suffer from rapid degradation, limiting their direct applicability. Here, the degradation of phenethylammonium lead iodide (PEA2PbI4) two-dimensional perovskites under ambient conditions is studied using fluorescence, absorbance and fluorescence lifetime measurements. It is demonstrated that a long-term stability of two-dimensional perovskites can be achieved through the encapsulation with hexagonal boron nitride. While un-encapsulated perovskite flakes degrade within hours, the encapsulated perovskites are stable for at least three months. In addition, encapsulation considerably improves the stability under laser irradiation. The environmental stability, combined with the improved durability under illumination, is a critical ingredient for thorough spectroscopic studies of the intrinsic opto-electronic properties of this material platform., Comment: 10 pages, 4 figures, and supporting information

Two-dimensional (2D) materials exhibit a number of improved mechanical, optical, electronic properties compared to their bulk counterparts. The absence of dangling bonds in the cleaved surfaces of these materials allows combining different 2D materials into van der Waals heterostructures to fabricate p-n junctions, photodetectors, 2D-2D ohmic contacts that show unexpected performances. These intriguing results are regularly summarized in comprehensive reviews. A strategy to tailor their properties even further and to observe novel quantum phenomena consists in the fabrication of superlattices whose unit cell is formed either by two dissimilar 2D materials or by a 2D material subjected to a periodical perturbation, each component contributing with different characteristics. Furthermore, in a 2D materials-based superlattice, the interlayer interaction between the layers mediated by van der Waals forces constitutes a key parameter to tune the global properties of the superlattice. The above-mentioned factors reflect the potential to devise countless combinations of van der Waals 2D materials based superlattices. In the present feature article, we explain in detail the state-of-the-art of 2D materials-based superlattices and we describe the different methods to fabricate them, classified as vertical stacking, intercalation with atoms or molecules, moir\'e patterning, strain engineering and lithographic design. We also aim to highlight some of the specific applications for each type of superlattices., Comment: Perspective article. 6 Figures. 133 references

Indium selenide (InSe), as a novel van der Waals layered semiconductor, has attracted a large research interest thanks to its excellent optical and electrical properties in the ultra-thin limit. Here, we discuss four different optical methods to quantitatively identify the thickness of thin InSe flakes on various substrates, such as SiO2/Si or transparent polymeric substrates. In the case of thin InSe deposited on a transparent substrate, the transmittance of the flake in the blue region of the visible spectrum can be used to estimate the thickness. For InSe supported by SiO2/Si, the thickness of the flakes can be estimated either by assessing their apparent colors or accurately analyzed using a Fresnel-law based fitting model of the optical contrast spectra. Finally, we also studied the thickness dependency of the InSe photoluminescence emission energy, which provides an additional tool to estimate the InSe thickness and it works both for InSe deposited on SiO2/Si and on a transparent polymeric substrate., Comment: 4 figures

Considering that two-dimensional (2D) molybdenum trioxide has acquired more attention in the last few years, it is relevant to speed up thickness identification of this material. We provide two fast and non-destructive methods to evaluate the thickness of MoO$_3$ flakes on SiO$_2$/Si substrates. First, by means of quantitative analysis of the apparent color of the flakes in optical microscopy images, one can make a first approximation of the thickness with an uncertainty of $\pm3$ nm. The second method is based on the fit of optical contrast spectra, acquired with micro-reflectance measurements, to a Fresnel law-based model that provides an accurate measurement of the flake thickness with $\pm2$ nm of uncertainty., Comment: 5 Figures

The ultrathin nature and dangling bonds free surface of two-dimensional (2D) semiconductors allow for significant modifications of their band gap through strain engineering. Here, thin InSe photodetector devices are biaxially stretched, finding, a strong band gap tunability upon strain. The applied biaxial strain is controlled through the substrate expansion upon temperature increase and the effective strain transfer from the substrate to the thin InSe is confirmed by Raman spectroscopy. The band gap change upon biaxial strain is determined through photoluminescence measurements, finding a gauge factor of up to ~200 meV/%. We further characterize the effect of biaxial strain on the electrical properties of the InSe devices. In the dark state, a large increase of the current is observed upon applied strain which gives a piezoresistive gauge factor value of ~450-1000, ~5-12 times larger than that of other 2D materials and of state-of-the-art silicon strain gauges. Moreover, the biaxial strain tuning of the InSe band gap also translates in a strain-induced redshift of the spectral response of our InSe photodetectors with {\Delta}Ecut-off ~173 meV at a rate of ~360 meV/% of strain, indicating a strong strain tunability of the spectral bandwidth of the photodetectors., Comment: 5 main text figures, 1 table comparing the strain tunable bandgap for different 2Ds and 11 supporting information figures

Two-dimensional semiconductors are excellent candidates for next-generation electronics and optoelec-tronics thanks to their electrical properties and strong light-matter interaction. To fabricate devices with optimal electrical properties, it is crucial to have both high-quality semiconducting crystals and ideal con-tacts at metal-semiconductor interfaces. Thanks to the mechanical exfoliation of van der Waals crystals, atomically-thin high-quality single-crystals can easily be obtained in a laboratory. However, conventional metal deposition techniques can introduce chemical disorder and metal-induced mid-gap states that induce Fermi level pinning and can degrade the metal-semiconductor interfaces, resulting in poorly performing devices. In this article, we explore the electrical contact characteristics of Au-InSe and graphite-InSe van der Waals contacts, obtained by stacking mechanically exfoliated InSe flakes onto pre-patterned Au or graphite electrodes without the need of lithography or metal deposition. The high quality of the metal-semiconductor interfaces obtained by van der Waals contact allows to fabricate high-quality Schottky di-odes based on the Au-InSe Schottky barrier. Our experimental observation indicates that the contact barrier at the graphite-InSe interface is negligible due to the similar electron affinity of InSe and graphite, while the Au-InSe interfaces are dominated by a large Schottky barrier., Comment: 25 pages, 13 figures, Main text and Supporting Information

Due to the excellent electrical transport properties and optoelectronic performance, thin indium selenide (InSe) has recently attracted attention in the field of 2D semiconducting materials. However, the mechanism behind the photocurrent generation in thin InSe photodetectors remains elusive. Here, we present a set of experiments aimed at explaining the strong scattering in the photoresponsivity values reported in the literature for thin InSe photodetectors. By performing optoelectronic measurements on thin InSe-based photodetectors operated under different environmental conditions we find that the photoresponsivity, the response time and the photocurrent power dependency are strongly correlated in this material. This observation indicates that the photogating effect plays an imporant role for thin InSe flakes, and it is the dominant mechanism in the ultra-high photoresponsivity of pristine InSe devices. In addition, when exposing the pristine InSe photodetectors to the ambient environment we observe a fast and irreversible change in the photoresponse, with a decrease in the photoresponsivity accompanied by an increase of the operating speed. We attribute this photodetector performance change (upon atmospheric exposure) to the decrease in the density of the traps present in InSe, due to the passivation of selenium vacancies by atmospheric oxygen species. This passivation is accompanied by a downward shift of the InSe Fermi level and by a decrease of the Fermi level pinning, which leads to an increase of the Schottky barrier between Au and InSe. Our study reveals the important role of traps induced by defects in tailoring the properties of devices based on 2D materials and offers a controllable route to design and functionalize thin InSe photodetectors to realize devices with either ultrahigh photoresposivity or fast operation speed., Comment: 27 pages, 12 figures, Main text and Supporting Information

We present microfabricated thermal actuators to engineer the biaxial strain in two-dimensional (2D) materials. These actuators are based on microheater circuits patterned onto the surface of a polymer with a high thermal expansion coefficient. By running current through the microheater one can vary the temperature of the polymer and induce a controlled biaxial expansion of its surface. This controlled biaxial expansion can be transduced to biaxial strain to 2D materials, placed onto the polymer surface, which in turn induces a shift of the optical spectrum. Our thermal strain actuators can reach a maximum biaxial strain of 0.64 % and they can be modulated at frequencies up to 8 Hz. The compact geometry of these actuators results in a negligible spatial drift of 0.03 um/deg, which facilitates their integration in optical spectroscopy measurements. We illustrate the potential of this strain engineering platform to fabricate a strain-actuated optical modulator with single-layer MoS2., Comment: 5 main text figures + 5 supp. info. figures

Strain is a powerful tool to modify the optical properties of semiconducting transition metal dichalcogenides like MoS2, MoSe2, WS2 and WSe2. In this work we provide a thorough description of the technical details to perform uniaxial strain measurements on these two-dimensional semiconductors and we provide a straightforward calibration method to determine the amount of applied strain with high accuracy. We then employ reflectance spectroscopy to analyze the strain tunability of the electronic properties of single-, bi- and tri-layer MoS2, MoSe2, WS2 and WSe2. Finally, we quantify the flake-to-flake variability by analyzing 15 different single-layer MoS2 flakes., Comment: 4 main text figures, 5 tables, 18 figures in the supporting information

In two-dimensional materials research, oxidation is usually considered as a common source for the degradation of electronic and optoelectronic devices or even device failure. However, in some cases a controlled oxidation can open the possibility to widely tune the band structure of 2D materials. In particular, we demonstrate the controlled oxidation of titanium trisulfide (TiS$_3$), a layered semiconductor that has attracted much attention recently thanks to its quasi-1D electronic and optoelectronic properties and its direct bandgap of 1.1 eV. Heating TiS$_3$ in air above 300 {\deg}C gradually converts it into TiO$_2$, a semiconductor with a wide bandgap of 3.2 eV with ap-plications in photo-electrochemistry and catalysis. In this work, we investigate the controlled thermal oxidation of individual TiS$_3$ nanoribbons and its influence on the optoelectronic properties of TiS$_3$-based photodetectors. We observe a step-wise change in the cut-off wavelength from its pristine value ~1000 nm to 450 nm after subjecting the TiS$_3$ devices to subsequent thermal treatment cycles. Ab-initio and many-body calculations confirm an increase in the bandgap of titanium oxysulfide (TiO$_{2-x}$S$_x$) when increasing the amount of oxygen and reducing the amount of sulfur., Comment: 7 figures in main text, 9 figures in supp. info

We fabricate large-area atomically thin MoS$_2$ layers through the direct transformation of crystalline molybdenum MoS$_2$ (MoO$_3$) by sulfurization at relatively low temperatures. The obtained MoS2 sheets are polycrystalline (~10-20 nm single-crystal domain size) with areas of up to 300x300 um$^2$ with 2-4 layers in thickness and show a marked p-type behaviour. The synthesized films are characterized by a combination of complementary techniques: Raman spectroscopy, X-ray diffraction, transmission electron microscopy and electronic transport measurements., Comment: 6 figures in main text, 2 figures in supp. info

The exploration of electronic and optoelectronic properties of two-dimensional (2D) materials has become one of the most attractive line of research since the isolation of graphene. Such 'all-surface materials' present a strong sensitivity to environmental conditions and thus characterization of the devices based on these materials usually requires measurement systems operating in high-vacuum. However, conventional optoelectronic probe-station testing systems are are not compatible with high vacuum operation and vacuum-compatible versions are rather expensive. Here, we present a high-vacuum system specifically designed to test electronic and optoelectronic devices based on 2D materials. This system can be implemented with low budget and it is mostly based on the assembly of commercially available standard vacuum and optic components. Despite the simplicity of this system we demonstrate full capabilities to characterize optoelectronic devices in a broad range of wavelengths with fast pumping/venting speed and possibility of modulating the device temperature (room temperature to ~150deg)., Comment: Tables including all the part-numbers to replicate the setup are provided

We fabricate paper-supported semiconducting devices by rubbing a layered molybdenum disulfide (MoS2) crystal onto a piece of paper, similarly to the action of drawing/writing with a pencil on paper. We show that the abrasion between the MoS2 crystal and the paper substrate efficiently exfoliates the crystals, breaking the weak van der Waals interlayer bonds and leading to the deposition of a film of interconnected MoS2 platelets. Employing this simple method, that can be easily extended to other 2D materials, we fabricate MoS2-on-paper broadband photodectectors with spectral sensitivity from the ultraviolet (UV) to the near-infrared (NIR). We also used these paper-based photodetectors to acquire pictures of objects by mounting the photodetectors in a homebuilt single-pixel camera setup., Comment: 6 main text figures + 4 Supp Info figures

We have studied electrical transport as a function of carrier density, temperature and bias in multi-terminal devices consisting of hexagonal boron nitride (h-BN) encapsulated titanium trisulfide (TiS$_3$) sheets. Through the encapsulation with h-BN, we observe metallic behavior and high electron mobilities. Below $\sim$60 K an increase in the resistance, and non-linear transport with plateau-like features in the differential resistance are present, in line with the expected charge density wave (CDW) formation. Importantly, the critical temperature and the threshold field of the CDW phase can be controlled through the back-gate.

Two-dimensional Indium Selenide (InSe) has attracted extensive attention recently due to its record-high charge carrier mobility and photoresponsivity in the fields of electronics and optoelectronics. Nevertheless, the mechanical properties of this material in the ultra-thin regime have not been investigated yet. Here, we present our efforts to determine the Young's modulus of thin InSe (~1-2 layers to ~40 layers) flakes experimentally by using buckling-based methodology. We find that the Young's modulus has a value of 23.1 +- 5.2 GPa, one of the lowest values reported up to date for crystalline two-dimensional materials. This superior flexibility can be very attractive for different applications, such as strain engineering and flexible electronics., Comment: 3 figures, 1 table

The development of systems for the deterministic transfer of two-dimensional (2D) materials have undoubtedly contributed to a great advance in the 2D materials research. In fact, they have made it possible to fabricate van der Waals heterostructures and 2D materials-based devices with complex architectures. Nonetheless, as far as we know, the amount of papers in the literature providing enough details to reproduce these systems by other research groups is very scarce in the literature. Moreover, these systems typically require the use of expensive optical and mechanical components hampering their applicability in research groups with low budget. Here we demonstrate how a deterministic placement system for 2D materials set up with full capabilities can be implemented under 900 Eur which can be easily implemented in low budget labs and educational labs., Comment: 4 Figures in main text, a full step-by-step assembly guide in the supp. info. all part numbers needed to assemble the setup included

The isolation of air-sensitive two-dimensional (2D) materials and the race to achieve a better control of the interfaces in van der Waals heterostructures has pushed the scientific community towards the development of experimental setups that allow to exfoliate and transfer 2D materials under inert atmospheric conditions. These systems are typically based on over pressurized N2 of Ar gloveboxes that require the use of very thick gloves to operate within the chamber or the implementation of several motorized micro-manipulators. Here, we set up a deterministic transfer system for 2D materials within a gloveless anaerobic chamber. Unlike other setups based on over-pressurized gloveboxes, in our system the operator can manipulate the 2D materials within the chamber with bare hands. This experimental setup allows us to exfoliate 2D materials and to deterministically place them at a desired location with accuracy in a controlled O2-free and very low humidity (<2% RH) atmosphere. We illustrate the potential of this system to work with air-sensitive 2D materials by comparing the stability of black phosphorus and perovskite flakes inside and outside the anaerobic chamber., Comment: 6 main text figures, 7 supp. info. figures. 1 main text table with all the part numbers needed to assemble the setup

The successful application of titanium oxide-graphene hybrids in the fields of photocatalysis, photovoltaics and photodetection strongly depends on the interfacial contact between both materials. The need to provide a good coupling between the enabling conductor and the photoactive phase prompted us to directly grow conducting graphenic structures on TiO2 crystals. We here report on the direct synthesis of tailored graphenic structures by using Plasma Assisted Chemical Vapour Deposition that present a clean junction with the prototypical titanium oxide (110) surface. Chemical analysis of the interface indicates chemical bonding between both materials. Photocurrent measurements under UV light illumination manifest that the charge transfer across the interface is efficient. Moreover, the influence of the synthesis atmosphere, gas precursor (C2H2) and diluents (Ar, O2), on the interface and on the structure of the as-grown graphenic material is assessed. The inclusion of O2 promotes vertical growth of partially oxidized carbon nanodots/rods with controllable height and density. The deposition with Ar results in continuous graphenic films with low resistivity (6.8x10-6 ohm x m). The synthesis protocols developed here are suitable to produce tailored carbon-semiconductor structures on a variety of practical substrates as thin films, pillars or nanoparticles., Comment: 24 pages, 8 figures, original research paper

Franckeite is a naturally occurring layered mineral with a structure composed of alternating stacks of SnS2-like and PbS-like layers. Although this superlattice is composed of a sequence of isotropic two-dimensional layers, it exhibits a spontaneous rippling that makes the material structurally anisotropic. We demonstrate that this rippling comes hand in hand with an inhomogeneous in-plane strain profile and anisotropic electrical, vibrational and optical properties. We argue that this symmetry breakdown results from a spatial modulation of the van der Waals interaction between layers due to the SnS2-like and PbS-like lattices incommensurability., Comment: 6 main text figures, Supp. Info. available upon request

We show how the excitonic features of biaxial MoS2 flakes are very sensitive to biaxial strain. We find a lower bound for the gauge factors of the A exciton and B exciton of (-41 +- 2) meV/% and (-45 +- 2) meV/% respectively, which are larger than those found for single-layer MoS2. Interestingly, the interlayer exciton feature also shifts upon biaxial strain but with a gauge factor that is systematically larger than that found for the A exciton, (-48 +- 4) meV/%. We attribute this larger gauge factor for the interlayer exciton to the strain tunable van der Waals interaction due to the Poisson effect (the interlayer distance changes upon biaxial strain)., Comment: 3 figures in the main text, 14 figures in the Supp. Info

When a two-dimensional material, adhered onto a compliant substrate, is subjected to compression it can undertake a buckling instability yielding to a periodic rippling. Interestingly, when black phosphorus flakes are compressed along the zig-zag crystal direction the flake buckles forming ripples with a 40% longer period than that obtained when the compression is applied along the armchair direction. This anisotropic buckling stems from the puckered honeycomb crystal structure of black phosphorus and a quantitative analysis of the ripple period allows us to determine the Youngs's modulus of few-layer black phosphorus along the armchair direction (EbP_AC = 35.1 +- 6.3 GPa) and the zig-zag direction (EbP_ZZ = 93.3 +- 21.8 GPa)., Comment: 4 figures + 1 table in main text, 4 supp. info. figures. Available Open Access at publisher's webpage

Here, we propose a method to determine the thickness of the most common transition metal dichalcogenides (TMDCs) placed on the surface of transparent stamps, used for the deterministic placement of two-dimensional materials, by analyzing the red, green and blue channels of transmission-mode optical microscopy images of the samples. In particular, the blue channel transmittance shows a large and monotonic thickness dependence, making it a very convenient probe of the flake thickness. The method proved to be robust given the small flake-to-flake variation and the insensitivity to doping changes of MoS2. We also tested the method for MoSe2, WS2 and WSe2. These results provide a reference guide to identify the number of layers of this family of materials on transparent substrates only using optical microscopy., Comment: 4 figures in main text, 2 figures in supp. info

We report the isolation of thin flakes of cylindrite, a naturally occurring van der Waals superlattice, by means of mechanical and liquid phase exfoliation. We find that this material is a heavily doped p-type semiconductor with a narrow gap (<0.85 eV) with intrinsic magnetic interactions that are preserved even in the exfoliated nanosheets. Due to its environmental stability and high electrical conductivity, cylindrite can be an interesting alternative to the existing two-dimensional magnetic materials., Comment: 5 figures in main text, 1 supp. info. figure. Available open access at the publisher's web

Semiconducting 2D materials, such as molybdenum disulfide (MoS2) and other members of the transition metal dichalcogenide family, have emerged as promising materials for applications in high performance nanoelectronics that exhibit excellent electrical and optical properties. Highly efficient photocurrent (PC) generation is reported in vertical few layer MoS2 devices contacted with semitransparent metallic electrodes. The light absorption of the device can be improved by fabricating vertical photodevices using few layer flakes, achieving a photoresponse of up to 0.11 A/W and an external quantum efficiency (EQE) of up to 30%. Because of the vertical design, the distance between electrodes can be kept in the range of a few nanometers, thus substantially reducing the collection time of photogenerated carriers and increasing the efficiency of the devices. The wavelength dependent PC, photoresponsivity, and EQE are measured over a photon energy range from 1.24 to 2.58 eV. Compared to previous in plane and vertical devices, these vertical few layer MoS2 photodevices exhibit very short response time, 60 ns, and a cutoff frequency of 5.5 MHz, while maintaining high photoresponsivity., Comment: Main text: 9 pages, 4 figures. Supp. Info: 8 pages, 5 figures

The capability to detect the polarization state of light is crucial in many day-life applications and scientific disciplines. Novel anisotropic two-dimensional materials such as TiS3 combine polarization sensitivity, given by the in-plane optical anisotropy, with excellent electrical properties. Here we demonstrate the fabrication of a monolithic polarization sensitive broadband photodetector based on a mixed-dimensionality TiS3/Si p-n junction. The fabricated devices show broadband responsivity up to 1050 nm, a strong sensitivity to linearly polarized illumination with difference between the two orthogonal polarization states up to 350 % and a good detectivity and fast response time. The discussed devices can be used as building blocks to fabricate more complex polarization sensitive systems such as polarimeters., Comment: 6 main text figures, 1 figure. Includes the supporting information (18 supp. info. figures)

Measuring the mechanical properties of two-dimensional materials is a formidable task. While regular electrical and optical probing techniques are suitable even for atomically thin materials, conventional mechanical tests cannot be directly applied. Therefore, new mechanical testing techniques need to be developed. Up to now, the most widespread approaches require micro-fabrication to create freely suspended membranes, rendering their implementation complex and costly. Here, we revisit a simple yet powerful technique to measure the mechanical properties of thin films. The buckling metrology method, that does not require the fabrication of freely suspended structures, is used to determine the Young's modulus of several transition metal dichalcogenides (MoS2, MoSe2, WS2 and WSe2) with thicknesses ranging from 3 to 10 layers. We critically compare the obtained values for the Young's modulus and their uncertainty, finding that this simple technique provides results, which are in good agreement with those reported using other highly sophisticated testing methods. By comparing the cost, complexity and time required for the different methods reported in the literature, the buckling metrology method presents certain advantages that makes it an interesting mechanical test tool for 2D materials., Comment: Main text: 3 figures, 2 tables. Supp Info: 11 figures, 2 tables. This is an author's version (post peer-review)

Strain engineering, which aims to tune the bandgap of a semiconductor by the application of strain, has emerged as an interesting way to control the electrical and optical properties of two-dimensional (2D) materials. Apart from the changes in the intrinsic properties of 2D materials, the application of strain can be also used to modify the characteristics of devices based on them. In this work, we study flexible and transparent photodetectors based on single-layer MoS2 under the application of biaxial strain. We find that by controlling the level of strain, we can tune the photoresponsivity (by 2-3 orders of magnitude), the response time (from <80 ms to 1.5 s) and the spectral bandwidth (with a gauge factor of 135 meV/% or 58 nm/%) of the device., Comment: 3 main text figures and 12 supporting information figures

Spatially periodic structures with a long range period, referred to as moir\'e pattern, can be obtained in van der Waals bilayers in the presence of a small stacking angle or of lattice mismatch between the monolayers. Theoretical predictions suggest that the resulting spatially periodic variation of the band structure modifies the optical properties of both intra and interlayer excitons of transition metal dichalcogenides heterostructures. Here, we report on the impact of the moir\'e pattern formed in a MoSe$_2$/MoS$_2$ heterobilayer encapsulated in hexagonal boron nitride. The periodic in-plane potential results in a splitting of the MoSe$_2$ exciton and trion in both emission and absorption spectra. The observed energy difference between the split peaks is fully consistent with theoretical predictions., Comment: just accepted in Nano Letters (10.1021/acs.nanolett.8b03266)

Gallium selenide (GaSe) is a novel two-dimensional material, which belongs to the layered III-VIA semiconductors family and attracted interest recently as it displays single-photon emitters at room temperature and strong optical non-linearity. Nonetheless, few-layer GaSe is not stable under ambient conditions and it tends to degrade over time. Here we combine atomic force microscopy, Raman spectroscopy and optoelectronic measurements in photodetectors based on thin GaSe to study its long-term stability. We found that the GaSe flakes exposed to air tend to decompose forming firstly amorphous selenium and Ga2Se3 and subsequently Ga2O3. While the first stage is accompanied by an increase in photocurrent, in the second stage we observe a decrease in photocurrent which leads to the final failure of GaSe photodetectors. Additionally, we found that the encapsulation of the GaSe photodetectors with hexagonal boron nitride (h-BN) can protect the GaSe from degradation and can help to achieve long-term stability of the devices., Comment: 23 pages, 5 figures, supporting information

We study mechanically exfoliated nanosheets of franckeite by quantitative optical microscopy. The analysis of transmission mode and epi-illumination mode optical microscopy images provides a rapid method to estimate the thickness of the exfoliated flakes at first glance. A quantitative analysis of the optical contrast spectra by means of micro-reflectance allows one to determine the refractive index of franckeite in a broad range of the visible spectrum through a fit of the acquired spectra to a Fresnel law based model., Comment: Main text (6 figures) + Supp. Info. (6 figures)