A novel fabrication method for fluorescence-based apertureless scanning near-field optical microscope probes

We report a novel method for the fabrication of probes with localized sub-wavelength fluorescing media at their extremities. We present our first results and discuss future plans to extend this technique to the systematic fabrication of fluorescent probes for apertureless scanning near-field optical microscopy.     

A novel fabrication method for fluorescence-based apertureless scanning near-field optical microscope probes

We report a novel method for the fabrication of probes with localized sub-wavelength fluorescing media at their extremities. We present our first results and discuss future plans to extend this technique to the systematic fabrication of fluorescent probes for apertureless scanning near-field optical microscopy.     

Invited review article: a review of techniques for attaching micro- and nanoparticles to a probe's tip for surface force and near-field optical measurements

Cantilevers with single micro- or nanoparticle probes have been widely used for atomic force microscopy surface force measurements and apertureless scanning near-field optical microscopy applications. In this article, I critically review the particle attachment and modification techniques currently available, to help researchers choose the appropriate techniques for specific applications.     

Optoelectronic detector probes for scanning near-field optical microscopy

A brief explanation of the optoelectronic probe concept and a comparison between the implementation of passive waveguide probes and optoelectronic probes in scanning near-field optical microscopy (SNOM) is presented. The first probe realizations using cleaved semiconductor crystals and the work at present in progress using microfabricated Si pyramids are described. These crystals with evaporated metal electrodes forming a slit aperture with subwave-length dimensions work as metal–semiconductor–metal photodetectors. Their optical detection behaviour is investigated by measuring the intensity distribution of a laser focal point. Measurements where the external bias voltage is changed show that it is possible to modify the detection behaviour of the device because of the varying depletion widths. The last part of the article describes a concept where pyramidal probes should function simultaneously as sensors for scanning force microscopy (SFM) to measure topography and as optoelectronic probes for scanning near-field optoelectronic microscopy (SNOEM).     

A single gold particle as a probe for apertureless scanning near-field optical microscopy

We report on the fabrication, characterization and application of a probe consisting of a single gold nanoparticle for apertureless scanning near-field optical microscopy. Particles with diameters of 100 nm have been successfully and reproducibly mounted at the end of sharp glass fibre tips. We present the first optical images taken with such a probe. We have also recorded plasmon resonances of gold particles and discuss schemes for exploiting the wavelength dependence of their scattering cross-section for a novel form of apertureless scanning near-field optical microscopy.     

Fabrication of gold tips by chemical etching in aqua regia

We present a method to produce sharp gold tips for applications in apertureless near-field optical microscopy and spectroscopy. Thin gold wires are tapered by chemical etching in aqua regia, covered by an isooctane protective layer. Tips with apical radii of curvature of <50 nm are obtained with a 40% yield. The tip performances have been checked by shear-force imaging of amyloid fibrils samples and compared to optical fiber probes. The analysis of the tip morphology, carried out by scanning electron microscopy, shows the existence of two different etching processes occurring in bulk and at the liquid-liquid interface. A simple analytical model is presented to describe the dynamics of the tip formation at the liquid-liquid meniscus interface that fits remarkably well the experimental results in terms of tip shape and length.     

Optical near-field harmonic demodulation in apertureless microscopy

Spatial derivatives of the optical fields scattered by a surface can be investigated by apertureless near-field optical microscopy by modulating sinusoidally the probe to sample distance and detecting the optical signal at the first and higher harmonics. Demodulation up to the fifth harmonic order has been accomplished on a sample of close-packed latex spheres by means of the silicon tip of a scanning interference apertureless microscope. The working principles of such microscope are reviewed. The experimental configuration used comprises a tuning-fork-based tapping-mode atomic force microscope for the distance stabilization, and a double-modulation technique for complete separation of the topography tracking from the optical detection. Simple modelling provides first indications for the interpretation of experimental data. The technique described here provides either artefact-free near-field optical imaging, or detailed information on the structure of the near fields scattered by a surface.     

Microarrays of near-field optical probes with adjustable dimensions

We present the fabrication and the characterization of high-density microarrays comprising thousands of near-field optical probes. Two types of microarrays have been prepared by adapting the SNOM methodology: arrays of uncoated fiber nanotips (i.e. apertureless probes) and arrays of apertures with adjustable subwavelength dimensions. Such arrays were fabricated by retaining the coherent structure of monomode optical fiber bundles and therefore keeping their imaging properties. The size of the apertures in a microarray was tuned at the nanometer scale by modifying the fabrication parameters. Far-field characterization of these near-field probe arrays shows completely different behavior depending both on their architecture and on their characteristic size. The angular distribution of the far-field intensity transmitted through the aperture arrays is used to determine the optical size of such diffracting apertures. Aperture radii ranging from 95 to 250 nm were found in good agreement with SEM data. Furthermore, each nanoaperture of the array is optically independent in the far-field regime. Eventually, this study demonstrates potential applications of these imaging arrays as parallel near-field optical probes in both configurations (apertureless and with apertures).     

High-resolution constant-height imaging with apertured silicon cantilever probes

We present high-resolution aperture probes based on non-contact silicon atomic force microscopy (AFM) cantilevers for simultaneous AFM and near-infrared scanning near-field optical microscopy (SNOM). For use in near-field optical microscopy, conventional AFM cantilevers are modified by covering their tip side with an opaque aluminium layer. To fabricate an aperture, this metal layer is opened at the end of the polyhedral probe using focused ion beams (FIB). Here we show that apertures of less than 50 nm can be obtained using this technique, which actually yield a resolution of about 50 nm, corresponding to λ/20 at the wavelength used. To exclude artefacts induced by distance control, we work in constant-height mode. Our attention is particularly focused on the distance dependence of resolution and to the influence of slight cantilever bending on the optical images when scanning at such low scan heights, where first small attractive forces exerted on the cantilever become detectable.     

Invited review article: combining scanning probe microscopy with optical spectroscopy for applications in biology and materials science

This is a comprehensive review of the combination of scanning probe microscopy (SPM) with various optical spectroscopies, with a particular focus on Raman spectroscopy. Efforts to combine SPM with optical spectroscopy will be described, and the technical difficulties encountered will be examined. These efforts have so far focused mainly on the development of tip-enhanced Raman spectroscopy, a powerful technique to detect and image chemical signatures with single molecule sensitivity, which will be reviewed. Beyond tip-enhanced Raman spectroscopy and/or topography measurements, combinations of SPM with optical spectroscopy have a great potential in the characterization of structure and quantitative measurements of physical properties, such as mechanical, optical, or electrical properties, in delicate biological samples and nanomaterials. The different approaches to improve the spatial resolution, the chemical sensitivity, and the accuracy of physical properties measurements will be discussed. Applications of such combinations for the characterization of structure, defects, and physical properties in biology and materials science will be reviewed. Due to the versatility of SPM probes for the manipulation and characterization of small and/or delicate samples, this review will mainly focus on the apertureless techniques based on SPM probes.     

Near-field reflection backscattering apertureless optical microscopy: application to spectroscopy experiments on opaque samples, comparison between lock-in and digital photon counting detection techniques

An apertureless scanning near-field optical microscope (ASNOM) in reflection backscattering configuration is designed to conduct spectroscopic experiments on opaque samples constituted of latex beads. The ASNOM proposed takes advantage of the depth-discrimination properties of confocal microscopes to efficiently extract the near-field optical signal. Given their importance in a spectroscopic experiment, we systematically compare the lock-in and synchronous photon counting detection methods. Some results of Rayleigh's scattering in the near field of the test samples are used to illustrate the possibilities of this technique for reflection backscattering spectroscopy.     

Apertureless scanning near-field magneto-optical microscopy of magnetic multilayers

We imaged magnetic domains in Pt/Co/Pt multilayers using an apertureless scanning near-field optical microscope operating in reflection mode. As the magneto-optical effects are weak for this kind of structure, a polarization modulation technique with a photoelastic modulator was used to reveal the contrast between magnetic domains. In the case of a Pt/Co/Pt trilayer structure, a strong improvement in lateral resolution is observed compared with far-field magneto-optical images and good sensitivity is achieved. In the case of a Pt/[Co/Pt]Pt multilayer structure, stripe domains of 200 nm width could be resolved, in good agreement with images obtained by magnetic force microscopy on the same structure.     

Coaxial probes for scanning near-field microscopy

This paper deals with the development of coaxial aperture tips integrated in a cantilever probe for combined scanning near-field infrared microscopy and scanning force microscopy. A fabrication process is introduced that allows the batch fabrication of hollow metal aperture tips integrated on a silicon cantilever. To achieve the coaxial tip arrangement a metal rod is deposited inside the hollow tip using the focused ion beam technique. Theoretical calculations with a finite integration code were performed to study the transmission characteristics of coaxial tips in comparison with conventional aperture probes. In addition, the influence of the geometrical design parameters of the coaxial probe on its optical behaviour is investigated.     

Coaxial probes for scanning near-field microscopy

This paper deals with the development of coaxial aperture tips integrated in a cantilever probe for combined scanning near-field infrared microscopy and scanning force microscopy. A fabrication process is introduced that allows the batch fabrication of hollow metal aperture tips integrated on a silicon cantilever. To achieve the coaxial tip arrangement a metal rod is deposited inside the hollow tip using the focused ion beam technique. Theoretical calculations with a finite integration code were performed to study the transmission characteristics of coaxial tips in comparison with conventional aperture probes. In addition, the influence of the geometrical design parameters of the coaxial probe on its optical behaviour is investigated.     

Apertureless scanning near-field magneto-optical microscopy of magnetic multilayers

We imaged magnetic domains in Pt/Co/Pt multilayers using an apertureless scanning near-field optical microscope operating in reflection mode. As the magneto-optical effects are weak for this kind of structure, a polarization modulation technique with a photoelastic modulator was used to reveal the contrast between magnetic domains. In the case of a Pt/Co/Pt trilayer structure, a strong improvement in lateral resolution is observed compared with far-field magneto-optical images and good sensitivity is achieved. In the case of a Pt/[Co/Pt]Pt multilayer structure, stripe domains of 200 nm width could be resolved, in good agreement with images obtained by magnetic force microscopy on the same structure.     

SNOM/STM using a tetrahedral tip and a sensitive current-to-voltage converter

Scanning near-field optical microscopes (SNOM) using the tetrahedral-tip (T-tip) with scanning tunnelling microscopy (STM) distance control have been realized in transmission and reflection mode. Both set-ups used ordinary STM current-to-voltage converters allowing measurement of metallic samples. In the transmission mode, a resolution of 10 nm to 1 nm with regard to material contrast can be achieved on binary metal samples. Because of the great near-field optical potential of the T-tip with respect to the optical resolution, it is a challenging task to find out whether these results can be transferred to non-metallic sample systems as well. This paper reports on a newly designed SNOM/STM transmission mode set-up using the tetrahedral-tip. It implements a sensitive current-to-voltage converter to widen the field of measurable sample systems. Beyond this, mechanical and optical measuring conditions are substantially improved compared to previous set-ups. The new set-up provides a basis for the routine investigation of metal nanostructures and adsorbed organic monolayers at resolutions in the 10 nm range.     

Role of multipole moment of the probe in apertureless near-field optical microscopy

The model of apertureless near-field optical microscope is developed taking into account the multipole moment of probe. In the case of samples with small dielectric absorption, the multipole moments are shown to be responsible for the appearance of additional resonances in the spectrum of scattered signal. The influence of multipole moments is especially pronounced in the near-field microscopy with modulation of tip-sample distance. A good agreement of the theoretical results with experimental data in the case of resonant interaction of the probe and sample is demonstrated.     

Background-free imaging of plasmonic structures with cross-polarized apertureless scanning near-field optical microscopy

We present advances in experimental techniques of apertureless scanning near-field optical microscopy (aSNOM). The rational alignment procedure we outline is based upon a phase singularity that occurs while scanning polarizers around the nominal cross-polarized configuration of s-polarized excitation and p-polarized detection. We discuss the theoretical origin of this topological feature of the setup, which is robust against small deviations, such as minor tip misalignment or shape variations. Setting the polarizers to this singular configuration point eliminates all background signal, allowing for reproducible plasmonic eigenmode mapping with optimal signal-to-noise ratio.     

Spectroscopy with scanning near-field optical microscopy using photon tunnelling mode

We have demonstrated Raman spectroscopy using scanning near-field optical microscopy (SNOM). Photon tunnelling mode was employed, in which the sample is illuminated using an attenuated total reflection (ATR) configuration and the evanescent wave perturbed by the sample is picked up by a sharpened optical fibre probe. By this experimental arrangement Raman scattering from the optical fibre probe was greatly reduced, therefore we were able to excite the sample using more intense laser light compared to the illumination mode SNOM. Raman spectra of copper phthalocyanine (CuPc) were obtained in the off-resonance condition and without using surface-enhanced Raman scattering (SERS).     

Spectroscopy with scanning near-field optical microscopy using photon tunnelling mode

We have demonstrated Raman spectroscopy using scanning near-field optical microscopy (SNOM). Photon tunnelling mode was employed, in which the sample is illuminated using an attenuated total reflection (ATR) configuration and the evanescent wave perturbed by the sample is picked up by a sharpened optical fibre probe. By this experimental arrangement Raman scattering from the optical fibre probe was greatly reduced, therefore we were able to excite the sample using more intense laser light compared to the illumination mode SNOM. Raman spectra of copper phthalocyanine (CuPc) were obtained in the off-resonance condition and without using surface-enhanced Raman scattering (SERS).