Tip-enhanced Optical Microscopy Research Articles

Inhomogeneous defect distribution of triangular WS2 monolayer revealed by surface-enhanced and tip-enhanced Raman and photoluminescence spectroscopy

Confocal optical microscopy and tip-enhanced optical microscopy are applied to characterize the defect distributions in chemical vapor deposition-grown WS2 monolayer triangles qualitatively and quantitatively. The presence of defects in individual monolayer WS2 triangles is revealed with diffraction-limited spatial resolution in their photoluminescence (PL) images, from which the inhomogeneous defect density distribution is calculated, showing an inverse relationship to the PL intensity. The defect-related surface-enhanced Raman spectroscopy (SERS) effect is investigated by depositing a thin copper phthalocyanine layer (5nm) as the probe molecule on the monolayer WS2 triangles surface. Higher SERS enhancement effects are observed at the defect-rich areas. Furthermore, tip-enhanced optical measurements are performed, which can reveal morphologically defected areas invisible in the confocal optical measurements. Furthermore, the area with high defect density appears brighter than the low-defected area in the tip-enhanced optical measurements, which are different from the observation in the confocal optical measurements. The underlying reasons are attributed to the near-field enhancement of the defect exciton emission induced by the optically excited tip and to an improved coupling efficiency between the tip-generated near-field with the altered dipole moment orientation at the local defect.

In Situ Visualization of Optoelectronic Behavior of Grain Boundaries in Monolayer WSe2 at the Nanoscale

Optoelectronic properties of two-dimensional transition metal dichalcogenides are critically influenced by grain boundaries (GBs). However, optoelectronic behavior of the GBs has not been fully understood in part due to the limited sensitivity and spatial resolution of conventional analytical tools. Herein, we report a detailed investigation of the optoelectronic behavior of GBs in monolayer (1L) WSe2 using a powerful combination of tip-enhanced optical microscopy and electrical-mode atomic force microscopy. Our study reveals that the work function, charge accumulation, and excitonic photoluminescence quenching at the GBs vary significantly with the tilting angle of the merged single crystalline 1L WSe2 flakes. Furthermore, our experimental results are supported by density functional theory calculations of band structure and density of states, which indicate that the variation in optoelectronic behavior is caused by the dislocation structures and midgap states generated in the GBs. The novel insights into optoelectronic understanding of 1L WSe2 gained in this study are directly relevant for applications in high-performance optoelectronic devices.

Laser Scanning-Assisted Tip-Enhanced Optical Microscopy for Robust Optical Nanospectroscopy.

Laser-scanning-assisted tip-enhanced optical microscopy was developed for robust optical nanospectroscopy. The laser-scanning system was utilized to automatically set and keep the center of a tight laser-focusing spot in the proximity of a metallic tip with around 10 nm precision. This enabled us to efficiently and stably induce plasmon-coupled field enhancement at the apex of the metallic probe tip. The laser-scanning technique was also applied to tracking and compensating the thermal drift of the metallic tip in the spot. This technique is usable for long-term tip-enhanced optical spectroscopy without any optical degradation.

Resonant Antenna Probes for Tip-Enhanced Infrared Near-Field Microscopy

We report the development of infrared-resonant antenna probes for tip-enhanced optical microscopy. We employ focused-ion-beam machining to fabricate high-aspect ratio gold cones, which replace the standard tip of a commercial Si-based atomic force microscopy cantilever. Calculations show large field enhancements at the tip apex due to geometrical antenna resonances in the cones, which can be precisely tuned throughout a broad spectral range from visible to terahertz frequencies by adjusting the cone length. Spectroscopic analysis of these probes by electron energy loss spectroscopy, Fourier transform infrared spectroscopy, and Fourier transform infrared near-field spectroscopy corroborates their functionality as resonant antennas and verifies the broad tunability. By employing the novel probes in a scattering-type near-field microscope and imaging a single tobacco mosaic virus (TMV), we experimentally demonstrate high-performance mid-infrared nanoimaging of molecular absorption. Our probes offer excellent perspectives for optical nanoimaging and nanospectroscopy, pushing the detection and resolution limits in many applications, including nanoscale infrared mapping of organic, molecular, and biological materials, nanocomposites, or nanodevices.

Subnanometric stabilization of plasmon-enhanced optical microscopy

We have demonstrated subnanometric stabilization of tip-enhanced optical microscopy under ambient condition. Time-dependent thermal drift of a plasmonic metallic tip was optically sensed at subnanometer scale, and was compensated in real-time. In addition, mechanically induced displacement of the tip, which usually occurs when the amount of tip-applied force varies, was also compensated in situ. The stabilization of tip-enhanced optical microscopy enables us to perform long-time and robust measurement without any degradation of optical signal, resulting in true nanometric optical imaging with high reproducibility and high precision. The technique presented is applicable for AFM-based nanoindentation with subnanometric precision.

Resolving single fluorophores within dense ensembles: contrast limits of tip-enhanced fluorescence microscopy

We investigate the limits of one-photon fluorescence as a contrast mechanism in nanoscale-resolution tip-enhanced optical microscopy. Specifically, we examine the magnitude of tip-induced signal enhancement needed to resolve individual fluorophores within densely-packed ensembles. Modulation of fluorescence signals induced by an oscillating tip followed by demodulation with a lock-in amplifier increases image contrast by nearly two orders of magnitude. A theoretical model of this simple modulation/ demodulation scheme predicts an optimal value for the tip-oscillation amplitude that agrees with experimental measurements. Further, as an important step toward the eventual application of tip-enhanced fluorescence microscopy to the nanoscale structural analysis of biomolecular systems, we show that requisite signal enhancement factors are within the capabilities of commercially available silicon tips.

Simulations of atomic resolution tip-enhanced optical microscopy

Optical techniques can access a wealth of information but traditionally their resolution has been restricted by the diffraction limit. Near-field techniques, which used nanoscale apertures or nanotip electric field enhancement, have succeeded in circumventing Abbe's law. We show that atomic resolution is theoretically achievable for tip enhanced optical microscopy. Using finite element analysis of the electromagnetic field around a small radius metallic scanning probe microscopy tip, we modeled various tip radii and materials, and an aqueous environment as well as ambient air. For a 1 nm gold tip we predict a strong red shift, and surprisingly high values for the enhancement of the intensity of scattered light - over 10(7). For this tip, we predict that 0.2 nm lateral resolution in optical imaging is achievable - good enough to resolve individual atomic bonds. The promise of optical data at these spatial scales offers great potential for nanometrology and nanotechnology applications.

Heating effects in tip-enhanced optical microscopy

Finite element simulations of laser-induced heating in scanning probe microscopy are presented. The electromagnetic field is first simulated for a variety of tip and substrate materials, and for air and aqueous environments. This electromagnetic field, in the end of the tip and substrate under the tip, produces Joule heating. Using this Joule heat source, steady state thermal simulations are performed. As a result of the large enhancement of optical power by the tip-substrate cavity, predicted temperature rises can be over 3 orders of magnitude higher than the values predicted without a tip present, but the optical signal can be enhanced by over 10 orders. Gold tips and substrates are predicted to give the highest optical signal for a given temperature increase.