Defect healing and doping of CVD graphene by thermal sulfurization.

CVD graphene layers are intrinsically polycrystalline; depending on grain size, their structure at the atomic level is scarcely free of defects, which affects the properties of graphene. On the one hand, atomic-scale defects act as scattering centers and lead to a loss of carrier mobility. On the other hand, structural disorder at grain boundaries provides additional resistance in series that affects material conductivity. Graphene chemical functionalization has been demonstrated to be an effective way to improve its conductivity mainly by increasing carrier concentration. The present study reports the healing effects of sulfur doping on the electrical transport properties of single-layer CVD graphene. A post-growth thermal sulfurization process operating at 250 °C is applied on single layers of graphene on Corning-glass and Si/SiO2 substrates. XPS and Raman analyses reveal the covalent attachment of sulfur atoms in graphene carbon lattice without creating new C-sp3 defects. Measurements of transport properties show a significant improvement in hole mobility as revealed by Hall measurements and related material conductivity. Typically, Hall mobility values as high as 2500 cm2 V-1 s-1 and sheet resistance as low as 400 Ohm per square are measured on single-layer sulfurized graphene.

Stability of Nanometer-Thick Layered Gallium Chalcogenides and Improvements via Hydrogen Passivation.

The gallium monochalcogenides family, comprising gallium sulfide (GaS), gallium selenide (GaSe), and gallium telluride (GaTe), is capturing attention for its applications in energy storage and production, catalysis, photonics, and optoelectronics. This interest originates from their properties, which include an optical bandgap larger than those of most common transition metal dichalcogenides, efficient light absorption, and significant carrier mobility. For any application, stability to air exposure is a fundamental requirement. Here, we perform a comparative study of the stability of layered GaS, GaSe, and GaTe nanometer-thick films down to a few layers with the goal of identifying the most suitable Ga chalcogenide for future integration in photonic and optoelectronic devices. Our study unveils a trend of decreasing air stability from sulfide to selenide and finally to telluride. Furthermore, we demonstrate a hydrogen passivation process to prevent the oxidation of GaSe with a higher feasibility and durability than other state-of-the-art passivation methods proposed in the literature.

Layered gallium sulfide optical properties from monolayer to CVD crystalline thin films.

Interest in layered van der Waals semiconductor gallium monosulfide (GaS) is growing rapidly because of its wide band gap value between those of two-dimensional transition metal dichalcogenides and of insulating layered materials such as hexagonal boron nitride. For the design of envisaged optoelectronic, photocatalytic and photonic applications of GaS, the knowledge of its dielectric function is fundamental. Here we present a combined theoretical and experimental investigation of the dielectric function of crystalline 2H-GaS from monolayer to bulk. Spectroscopic imaging ellipsometry with micron resolution measurements are corroborated by first principle calculations of the electronic structure and dielectric function. We further demonstrate and validate the applicability of the established dielectric function to the analysis of the optical response of c-axis oriented GaS layers grown by chemical vapor deposition (CVD). These optical results can guide the design of novel, to our knowledge, optoelectronic and photonic devices based on low-dimensional GaS.

Interlaboratory study on Sb2S3 interplay between structure, dielectric function, and amorphous-to-crystalline phase change for photonics.

Antimony sulfide, Sb2S3, is interesting as the phase-change material for applications requiring high transmission from the visible to telecom wavelengths, with its band gap tunable from 2.2 to 1.6 eV, depending on the amorphous and crystalline phase. Here we present results from an interlaboratory study on the interplay between the structural change and resulting optical contrast during the amorphous-to-crystalline transformation triggered both thermally and optically. By statistical analysis of Raman and ellipsometric spectroscopic data, we have identified two regimes of crystallization, namely 250°C ≤ T < 300°C, resulting in Type-I spherulitic crystallization yielding an optical contrast Δn ∼ 0.4, and 300 ≤ T < 350°C, yielding Type-II crystallization bended spherulitic structure with different dielectric function and optical contrast Δn ∼ 0.2 below 1.5 eV. Based on our findings, applications of on-chip reconfigurable nanophotonic phase modulators and of a reconfigurable high-refractive-index core/phase-change shell nanoantenna are designed and proposed.

Interplay between Thickness, Defects, Optical Properties, and Photoconductivity at the Centimeter Scale in Layered GaS.

From the group-III monochalcogenide (MX, M = Ga, In; X = S, Se, Te) layered semiconductors, gallium monosulfide, GaS, has emerged as a promising material for electronics, optoelectronics, and catalysis applications. In this work, GaS samples of various thicknesses in the range from 38 to 1665 nm have been obtained by mechanical exfoliation to study the interplay between structural, morphological, optical, and photoresponsivity properties as a function of thickness. This interplay has been established by analyzing the structure through Raman spectroscopy and X-ray diffraction, the morphology through scanning electron microscopy and atomic force microscopy, the density and optical properties through spectroscopic ellipsometry, and the photoresponsivity through current-voltage measurements under UV light. This work shows that photoresponsivity increases with increases in GaS thickness, resulting in a UV photoresponsivity of 1.5·10-4 AW-1 stable over several on/off cycles.

Exploring the Thickness-Dependence of the Properties of Layered Gallium Sulfide.

Group III layered monochalcogenide gallium sulfide, GaS, is one of the latest additions to the two-dimensional (2D) materials family, and of particular interest for visible-UV optoelectronic applications due to its wide bandgap energy in the range 2.35-3.05 eV going from bulk to monolayer. Interestingly, when going to the few-layer regime, changes in the electronic structure occur, resulting in a change in the properties of the material. Therefore, a systematic study on the thickness dependence of the different properties of GaS is needed. Here, we analyze mechanically exfoliated GaS layers transferred to glass substrates. Specifically, we report the dependence of the Raman spectra, photoluminescence, optical transmittance, resistivity, and work function on the thickness of GaS. Those findings can be used as guidance in designing devices based on GaS.