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Register a new userOxidation dynamics of ultrathin GaSe probed through Raman spectroscopy
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Gallium selenide (GaSe) is a 2D material with a thickness-dependent gap, strong non-linear optical coefficients and uncommon interband optical selection rules, making it interesting for optoelectronic and spintronic applications. In this work, we monitor the oxidation dynamics of GaSe with thicknesses ranging from 10 to 200 nm using Raman spectroscopy. In ambient temperature and humidity conditions, the intensity of all Raman modes and the luminescence decrease rapidly with moderate exposure to above-gap illumination. Concurrently, several oxidation products appear in the Raman spectra: Ga$_2$Se$_3$, Ga$_2$O$_3$ and amorphous and crystalline selenium. We find that no safe measurement power exists for optical measurements on ultrathin GaSe in ambient conditions. We demonstrate that the simultaneous presence of oxygen, humidity, and above-gap illumination is required to activate this photo-oxidation process, which is attributed to the transfer of photo-generated charge carriers towards aqueous oxygen at the sample surface, generating highly reactive superoxide anions that rapidly degrade the sample and quench the optical response of the material.
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III-VI post-transition metal chalcogenides (InSe and GaSe) are a new class of layered semiconductors, which feature a strong variation of size and type of their band gaps as a function of number of layers (N). Here, we investigate exfoliated layers of InSe and GaSe ranging from bulk crystals down to monolayer, encapsulated in hexagonal boron nitride, using Raman spectroscopy. We present the N-dependence of both intralayer vibrations within each atomic layer, as well as of the interlayer shear and layer breathing modes. A linear chain model can be used to describe the evolution of the peak positions as a function of N, consistent with first principles calculations.
Raman spectroscopy has been used to identify defective bonding in neon and silicon ion irradiated single crystals of 6H-SiC. Observable differences exist in the C-C bonding region corresponding to different defect structures for neon and silicon ion implantations. Raman spectra of ion irradiated SiC show less tensile strain than neutron irradiations, explained by a residual compressive stress caused by the swelling constrained by the undamaged substrate. Evidence of oxidation during high temperature ion implantation is observed as C-O and Si-O Raman signals. Annealing irradiated SiC while acquiring Raman spectra shows rapid recovery of Si-C bonding, but not a complete recovery of the unirradiated structure. Annealing irradiated SiC causes surface oxidation where unirradiated SiC does not oxidise. Comparisons are made to the apparent radiation resistance of diamond and silicon which have similar crystal structures, but are monatomic, leading to the suggestion that chemical defects are responsible for increased radiation damage in SiC.
We grow AlN/4H-SiC and AlN/6H-SiC heterostructures by physical vapor deposition and characterize the heterointerface with nanoscale resolution. Furthermore, we investigate the spatial stress and strain distribution in these heterostructures using confocal Raman spectroscopy. We measure the spectral shifts of various vibrational Raman modes across the heterointerface and along the entire depth of the 4H- and 6H-SiC layers. Using the earlier experimental prediction for the phonon-deformation potential constants, we determine the stress tensor components in SiC as a function of the distance from the AlN/SiC heterointerface. In spite that the lattice parameter of SiC is smaller than that of AlN, the SiC layers are compressively strained at the heterointerface. This counterintuitive behavior is explained by different coefficients of thermal expansion of SiC and AlN when the heterostructures are cooled from growth to room temperature. The compressive stress values are maximum at the heterointerface, approaching one GPa, and relaxes to the equilibrium value on the scale of several tens of microns from the heterointerface.
As the synthesis of graphene on copper became one of the primary preparation methods for both fundamental research and industrial application, Raman spectra of graphene/Cu systems need to be quantitatively understood regarding how their interactions affect the electronic structure of graphene. Using multi-wavelength Raman spectroscopy, we investigated three types of graphene bound on Cu: graphene grown on Cu foils and Cu film/SiO2, and Cu-evaporated exfoliated graphene. 2D peak frequencies of the first two samples were ~17 cm-1 higher than expected for 1.96 eV excitation even when the effect of strain was considered. More notably, the upshift in 2D decreased with increasing excitation energy. Based on control experiments using Cu-evaporated graphene, we revealed that the spectral anomaly was induced by environment-dependent nonlinear dispersion in the electronic bands of graphene and determined the degree of the electronic modification. We also showed that the large upshifts of G and 2D peaks originating from differential thermal expansion of Cu could be significantly reduced by backing Cu films with dielectric substrates of insignificant thermal expansion. The quantitative analysis of electronic coupling between graphene and Cu presented in this study will be highly useful in characterizing as-grown graphene and possibly in other forms.
We present in-situ Raman measurements of laser-induced oxidation in exfoliated single-layer graphene. By using high-power laser irradiation, we can selectively and in a controlled way initiate the oxidation process and investigate its evolution over time. Our results show that the laser-induced oxidation process is divided into two separate stages, namely tensile strain due to heating and subsequent $p$-type doping due to oxygen binding. We discuss the temporal evolution of the $D/G$-mode ratio during oxidation and explain the unexpected steady decrease of the defect-induced $D$ mode at long irradiation times. Our results provide a deeper understanding of the oxidation process in single-layer graphene and demonstrate the possibility of sub-$mu$m patterning of graphene by an optical method.
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