ABSTRACT
The role of defects in two-dimensional semiconductors and how they affect the intrinsic properties of these materials have been a widely researched topic over the past few decades. Optical characterization techniques such as photoluminescence and Raman spectroscopies are important tools to probe the physical properties of semiconductors and the impact of defects. However, confocal optical techniques present a spatial resolution limitation lying in a µm-scale, which can be overcome by the use of near-field optical measurements. Here, we use tip-enhanced photoluminescence and Raman spectroscopies to unveil the nanoscale optical properties of grown MoS2 monolayers, revealing that the impact of doping and strain can be disentangled by the combination of both techniques. A noticeable enhancement of the exciton peak intensity corresponding to trion emission quenching is observed at narrow regions down to a width of 47 nm at grain boundaries related to doping effects. Besides, localized strain fields inside the sample lead to non-uniformities in the intensity and energy position of photoluminescence peaks. Finally, two distinct MoS2 samples present different nano-optical responses at their edges associated with opposite strains. The edge of the first sample shows a photoluminescence intensity enhancement and energy blueshift corresponding to a frequency blueshift for E2g and 2LA Raman modes. In contrast, the other sample displays a photoluminescence energy redshift and frequency red shifts for E2g and 2LA Raman modes at their edges. Our work highlights the potential of combining tip-enhanced photoluminescence and Raman spectroscopies to probe localized strain fields and doping effects related to defects in two-dimensional materials.
ABSTRACT
This paper investigates the impact of graphene on tip-enhanced Raman spectroscopy (TERS) by developing an electromagnetic characterization of the TERS-graphene device system. The study focuses on the interaction between the tip, the gate voltage, and the sample, specifically examining the electromagnetic effects in the system. Employing a finite element method (FEM)-based simulation model, we meticulously dissect the electric field distribution and the Raman amplification when graphene is introduced into the system. Our findings reveal that including graphene results in a marginal reduction in Raman amplification and a negligible variation in the induced charges within the system. To reinforce our simulations, we employ a simplified capacitor model, which corroborates our results, showcasing negligible induced charges and validating the obtained capacitance values. In this manuscript, we also explore the influence of the setup on the electro-optical properties of graphene, revealing a slight variation in conductivity despite strong changes in chemical potential. Overall, this work contributes to understanding TERS's electromagnetic aspects in the presence of graphene.
ABSTRACT
Coherence length (Lc) of the Raman scattering process in graphene as a function of Fermi energy is obtained with spatially coherent tip-enhanced Raman spectroscopy. Lc decreases when the Fermi energy is moved into the neutrality point, consistent with the concept of the Kohn anomaly within a ballistic transport regime. Since the Raman scattering involves electrons and phonons, the observed results can be rationalized either as due to unusually large variation of the longitudinal optical phonon group velocity vg, reaching twice the value for the longitudinal acoustic phonon, or due to changes in the electron energy uncertainty, both properties being important for optical and transport phenomena that might not be observable by any other technique.
ABSTRACT
Raman spectroscopy has been established as a valuable tool to study and characterize two-dimensional (2D) systems, but it exhibits two drawbacks: a relatively weak signal response and a limited spatial resolution. Recently, advanced Raman spectroscopy techniques, such as coherent anti-Stokes spectroscopy (CARS), stimulated Raman scattering (SRS) and tip-enhanced Raman spectroscopy (TERS), have been shown to overcome these two limitations. In this article, we review how useful physical information can be retrieved from different 2D materials using these three advanced Raman spectroscopy and imaging techniques, discussing results on graphene, hexagonal boron-nitride, and transition metal di- and mono-chalcogenides, thus providing perspectives for future work in this early-stage field of research, including similar studies on unexplored 2D systems and open questions.
ABSTRACT
Twisted bilayer graphene is created by slightly rotating the two crystal networks in bilayer graphene with respect to each other. For small twist angles, the material undergoes a self-organized lattice reconstruction, leading to the formation of a periodically repeated domain1-3. The resulting superlattice modulates the vibrational3,4 and electronic5,6 structures within the material, leading to changes in the behaviour of electron-phonon coupling7,8 and to the observation of strong correlations and superconductivity9. However, accessing these modulations and understanding the related effects are challenging, because the modulations are too small for experimental techniques to accurately resolve the relevant energy levels and too large for theoretical models to properly describe the localized effects. Here we report hyperspectral optical images, generated by a nano-Raman spectroscope10, of the crystal superlattice in reconstructed (low-angle) twisted bilayer graphene. Observations of the crystallographic structure with visible light are made possible by the nano-Raman technique, which reveals the localization of lattice dynamics, with the presence of strain solitons and topological points1 causing detectable spectral variations. The results are rationalized by an atomistic model that enables evaluation of the local density of the electronic and vibrational states of the superlattice. This evaluation highlights the relevance of solitons and topological points for the vibrational and electronic properties of the structures, particularly for small twist angles. Our results are an important step towards understanding phonon-related effects at atomic and nanometric scales, such as Jahn-Teller effects11 and electronic Cooper pairing12-14, and may help to improve device characterization15 in the context of the rapidly developing field of twistronics16.
