Towards better scanning near-field optical microscopy probes — progress and new developments

Several approaches are described with the aim of producing near-field optical probes with improved properties. Focused ion beam milling allows the fabrication of small apertures in a controlled fashion, resulting in probes with excellent polarization properties and increased transmission. Microfabrication processes are described that allow the production of apertures of 30–50 nm, facilitating the mass-fabrication of apertured tip structures that can be used in a combined force/near-field optical microscope. Finally, possible future developments are outlined.     

Three-dimensional analysis of light propagation through uncoated near-field fibre probes

The near-field emission from uncoated tapered fibre probes is investigated for different probe geometries. The three-dimensional model calculations are based on Maxwell's curl equations and describe the propagation of a 10 fs optical pulse (λ = 805 nm) through tapers of different lengths and different diameters of the taper exit. The numerical evaluation is done with a finite difference time domain code. Two tapers with cone angles of 50°, with taper lengths of 1.5 µm and 1.0 µm and exit diameters of 100 nm and 520 nm, respectively, are considered. We find that without sample the short taper with large exit diameter optimizes both light transmission and spatial resolution. In the presence of a sample with a high dielectric constant, however, the spatial near-field distribution changes drastically for both taper geometries. We find a pronounced increase in spatial resolution, down to about 250 nm inside the medium. This collimation of the near-field distribution arises from interferences between emitted and reflected light from the sample surface and from a collimation effect that the field experiences in the high-index semiconductor material. The combination of high spatial resolution and transmission and collection efficiencies makes such probes interesting for spectroscopic investigations, as demonstrated by recent experiments.     

Brighter near-field optical probes by means of improving the optical destruction threshold

The optical destruction thresholds of conventionally etched and tube-etched near-field optical probes were measured. One of the main advantages of tube-etched tips is their smooth glass surface after taper formation. Presumably for this reason, a destruction limit of over 120 μJ was obtained, almost twice as large as that of the rougher, conventionally etched fibre probes. The use of additional adhesion layers (Ti, Cr, Co and Ni) between the glass surface and the aluminium coating produced, especially for tube-etched tips, a significant increase in the optical destruction threshold. With increasingly thin metal coatings, the use of a protection coating that prevents corrosion during aging is recommended. An additional increase in optical stability was achieved by applying mixed-metal coatings: alternating thin titanium and thick aluminium layers yielded fibre probes with superior properties that achieved average optical destruction thresholds of > 270 μJ. This is an increase in stability of > 400% compared with conventionally fabricated near-field optical tips.     

Single molecule mapping of the optical field distribution of probes for near-field microscopy

The most difficult task in near-field scanning optical microscopy (NSOM) is to make a high quality subwavelength aperture probe. Recently, we have developed high definition NSOM probes by focused ion beam (FIB) milling. These probes have a higher brightness, better polarization characteristics, better aperture definition and a flatter end face than conventional NSOM probes. We have determined the quality of these probes in four independent ways: by FIB imaging and by shear-force microscopy (both providing geometrical information), by far-field optical measurements (yielding throughput and polarization characteristics), and ultimately by single molecule imaging in the near-field. In this paper, we report on a new method using shear-force microscopy to study the size of the aperture and the end face of the probe (with a roughness smaller than 1.5 nm). More importantly, we demonstrate the use of single molecules to measure the full three-dimensional optical near-field distribution of the probe with molecular spatial resolution. The single molecule images exhibit various intensity patterns, varying from circular and elliptical to double arc and ring structures, which depend on the orientation of the molecules with respect to the probe. The optical resolution in the measurements is not determined by the size of the aperture, but by the high optical field gradients at the rims of the aperture. With a 70 nm aperture probe, we obtain fluorescence field patterns with 45 nm FWHM. Clearly, this unprecedented near-field optical resolution constitutes an order of magnitude improvement over far-field methods like confocal microscopy.     

Surface imaging in near-field optical microscopy by using the fluorescence decay rate: a theoretical study

In this paper, we study the fluorescence decay rate of a molecule above a corrugated interface, and particularly the variations of the decay rate as a function of the lateral position of the molecule. As a first step, one has to determine the field diffracted by a corrugated interface when the incident field is the field emitted by a dipole. For this purpose, we have used a perturbative Rayleigh method, and we show that the decay rate variations can be connected to the surface profile via a transfer function. Some numerical calculations of this transfer function and of decay rate variation images are presented for dielectric and metallic samples. The visibility of the theoretical images is up to 20% and, moreover, resolution of the images is good enough to use the fluorescence lifetime of molecules as signal in a life-time scanning near-field optical microscope. The technical problems are discussed briefly.     

Inverse estimation of the tapered probe-sample shear force of scanning near-field optical microscope

In this paper, the conjugate gradient method of minimization with an adjoint equation is successfully applied to solve the inverse problem in estimating the shear force between the tapered probe and sample during the scanning process of scanning near-field optical microscope (SNOM). While knowing the available deflection at the tapered probe tip, the determination of the interaction shear force is regarded as an inverse vibration problem. In the estimating processes, no prior information on the functional form of the unknown quantity is required. The accuracy of the inverse analysis is examined by using the simulated exact and inexact measurements of deflection at the tapered probe tip. Numerical results show that good estimations on the interaction shear force can be obtained for all the test cases considered in this study.     

Design and optimization of tapered structure of near-field fibre probe based on finite-difference time-domain simulation

The finite-difference time-domain method was employed to simulate light propagation in tapered near-field fibre probes with small metal aperture. By conducting large-volume simulations, including tapered metal-cladding waveguide and connected optical fibre waveguide, we illustrated the coupling between these guiding modes as well as the electric field distribution in the vicinity of the aperture. The high collection efficiency of a double-tapered probe was reproduced and was ascribed to the shortening of the cut-off region and the efficient coupling to the guiding mode of the optical fibre. The dependence of the efficiency on the tapered structure parameters was also examined.     

3D simulations of the experimental signal measured in near-field optical microscopy

We present three-dimensional simulations of the image formation process in near-field optical microscopy. Our calculations take into account the different components of a realistic experiment: an extended metal coated tip, a subwavelength sample and its substrate. We investigate all possible detection (transmitted, reflected and collected field) and scanning (constant height, constant gap) modes. Our results emphasize the strong influence of the tip motion on the experimental signal. They also show that it is possible, by controlling the polarization of both the illumination and the detected field, to strongly reduce these artefacts.     

Spatial distribution and polarization dependence of the optical near-field in a silicon microfabricated probe

This paper reports on the spatial distribution and polarization behaviour of the optical near-field at the aperture of a Si micromachined probe. A sub-100 nm aperture at the apex of a SiO₂ tip on a Si cantilever was successfully fabricated by selective etching of the SiO₂ tip in a buffered-HF solution using a thin Cr film as a mask. The aperture, 10–100 nm in size, can be reproducibly fabricated by optimizing the etching time. The optical throughput of several apertures was measured. For a 100 nm aperture, a throughput of 1% was approved. The probe shows a very high optical throughput owing to the geometrical structure of the tip. The spatial distribution of the near-field light is measured and simulated using a finite difference-time domain method. The polarization behaviour of apertures with different shapes was analysed using a photon counting camera system.     

An inverse problem of estimating the heat source in tapered optical fibers for scanning near-field optical microscopy

A conjugate gradient method based on inverse algorithm is applied in this study to estimate the unknown space- and time-dependent heat source in aluminum-coated tapered optical fibers for scanning near-field optical microscopy, by reading the transient temperature data at the measurement positions. No prior information is available on the functional form of the unknown heat source in the present study; thus, it is classified as the function estimation in inverse calculation. The accuracy of the inverse analysis is examined by using the simulated exact and inexact temperature measurements. Results show that an excellent estimation on the heat source and temperature distributions in the tapered optical fiber can be obtained for all the test cases considered in this study.     

Spectroscopic study of the image formation in near-field microscopy, near an evanescent–homogeneous switching

Near-field optical microscopes provide highly resolved images of various samples. However, images are difficult to interpret owing to their sensitivity to illumination conditions. Moreover, by contrast with classical microscopy, the near-field signal combines the contributions of evanescent and propagative modes. In this study, we present results of a spectroscopic study in near-field. Our purpose is to explain how a switching of one diffracted mode from homogeneous to evanescent can modify image formation. The main point is to establish a relation between the evanescence of one diffracted mode and the fringes that are often observed in near-field experimental images. Moreover, on a metallic sample, the possible occurrence of plasmon resonance contributes to image distortion in a mainly different way. We use a Fourier series Rayleigh 3D method to explain image formation.     

On the use of the asymptotic scaled modal analysis for time-harmonic structural analysis and for the prediction of coupling loss factors for similar systems

The paper presents the results of an ongoing research on a scaling procedure aimed at the reduction of the computational cost associated, in a deterministic approach, to the wavelength simulation. The adoption of the energy distribution approach allowed to completely define the way in which a scaled model can represent the mean response of a given original model. This goal is achieved through a reduction in the dimensions not involved in the energy propagation and accordingly in an increase of the original damping loss factors. Here, the coupled systems under observation are those in which the same wave is allowed to travel, exchange and reflect. Specifically the results coming from the classical modal response and the statistical energy analysis are compared with those in output from the scaling procedure. Some highlights with experimental test-case results and comparisons for a plate assembly are also given. The work presents also an investigation about the possibility of estimating the energy influence coefficients through scaled finite element models.