Nano-patterning photosensitive polymers using local field enhancement at the end of apertureless SNOM tips

We show experimentally that local optical field enhancement can occur at the end of an apertureless SNOM tip illuminated by an external light source. Our approach consists in the use of a photosensitive polymer, placed in the tip near‐field, to record intensity distribution in the vicinity of the tip end. The excited nanometre‐size light source permits us to produce nano‐patterns on the polymer surface which are then characterized by atomic force microscopy. Experimental images show the influence, on the field enhancement, of three important experimental parameters: the polarization state of the incident light, the geometry of the external illumination and the radius of curvature of the tip apex. These results are shown to be in good agreement with two‐dimensional numerical calculations based on the finite‐difference time‐domain method. We show preliminary nanometre‐size patterns created by this nano‐source excited at a metallic tip extremity and discuss the potential of this approach for near‐field optical lithography.     

Field enhancement and apertureless near-field optical spectroscopy of single molecules

We report on fluorescence enhancement in near field optical spectroscopy by apertureless microscopy. Our apertureless microscope is designed around a confocal fluorescence microscope associated with an AFM head. First, we show that the confocal microscope alone allows single molecule imaging and single molecule fluorescence analysis. When associated with the AFM head, we demonstrate, for the first time to our knowledge, that single molecule fluorescence is enhanced under the silicon tip. We tentatively attribute this effect to field enhancement under the tip.     

Nanoscale optical imaging of chromosomes with apertureless microscopy.

Near-field optical structure of the centromere region of undyed polytene chromosomes has been observed using an apertureless near-field optical microscope that detects the intensity of light scattered from an atomic force microscope tip under laser illumination. The centromere is of primary importance to the functioning of the chromosome in the cell during cell division. It is also particularly interesting for structural/optical studies since its DNA repeat sequences are highly conserved among organisms and it is possible that they play a part in the centromere self assembly (Clark and Wall 1996).     

Photo-initiated energy transfer in nanostructured complexes observed by near-field optical microscopy

We report an apertureless near‐field optical study on nanostructured objects formed by J‐aggregates adsorbed on silver (Ag) nanoparticles. Near‐field images reveal that the enhanced near‐field from the dressed particle's (DP) resonantly excited plasmon oscillation is efficiently absorbed by the J‐aggregates. The sensitivity of the near‐field images recorded at the harmonics of the probe vibration frequency suggests that the DP is releasing part of the absorbed energy radiatively upon interaction with the probe. The role of the probe in providing this new radiative relaxation channel is further confirmed as fluorescence from the J‐aggregates on the particle is detected on the particle location only. We based the interpretation of our results on the near‐field optical response from a bare Ag particle excited at the plasmon resonance as well as on far‐field emission and transient absorption experiments.     

Total internal reflection fluorescence imaging using an upconverting cover slip for multicolour evanescent excitation

Total internal reflection fluorescence microscopy is well known as a means of studying surface‐bound structures in cell biology. It is usually measured either by coupling a light source to the sample using a prism or with a special objective where light passing through the periphery of the lens illuminates the contact region beyond the critical angle. In this study we present a new and simple approach to total internal reflection fluorescence microscopy where the sample is mounted on a cover slip prepared from a high‐index upconverting glass‐ceramic. Excitation of the cover slip with a low‐cost near‐infrared laser diode generates intense narrow‐band visible emission within the cover slip, some of which is totally internally reflected. This emission gives rise to an evanescent wave at the interface and hence can excite surface‐bound fluorescent species. Depending on the excitation conditions the cover slip can generate violet, green and red emission and hence can excite a wide range of fluorescent labels. Fluorescence emission from the sample can be detected in spectral regions where the direct emission from the cover slip is very weak. The advantages and limitations of the technique are discussed in comparison with conventional total internal reflection fluorescence microscopy measurements and prospects for novel total internal reflection fluorescence microscopy geometries are considered.     

Mesoscopic structures and dynamics of merocyanine J-aggregate studied by time-resolved fluorescence SNOM

Time-resolved fluorescence SNOM is used to probe the mesoscopic structure and dynamics of long-chain merocyanine (C₁₈MC) J-aggregates on glass plates prepared by spin coating, casting, and casting of water-soluble polymer films. A globular structure with an average diameter of ∼ 1 µm and a height of ∼ 50 nm was attributed to the J-aggregate of C₁₈MC in the spin-coating film. In polymer films, the bandwidth of the absorption of J-aggregate is much narrower in polyvinyl alcohol (PVA, ∼ 20 nm) than that in polyvinyl sulphate (PVS, ∼ 60 nm). We have demonstrated that the large bandwidth of the spectrum is due to the inhomogeneous distribution of the J-aggregate. The fluorescence image of the J-aggregate in PVA film was rather uniform, whereas non-uniform distribution of the fluorescence was observed in PVS film. The fluorescence of C₁₈MC J-aggregate in a small domain of PVA film was a single exponential decay with a lifetime as short as 19 ps, which was shorter than that in PVS film with a two-exponential decay (average lifetime of ∼ 25 ps). The fluorescence lifetime of the J-aggregate and its single exponential behaviour are considered to be indicators of the uniform distribution of the J-aggregate. The non-uniform distribution of the J-aggregate in PVS film was interpreted in terms of electrostatic interaction between PVS and merocyanine.     

Far-field emission of a tapered optical fibre tip: a theoretical analysis

The far-field transmission pattern of a tapered optical tip with small aperture (radius ∼ < 40 nm) is modelled by solving Maxwell's equations in the radiation zone with boundary conditions appropriate to the conical geometry. The model is able to reproduce the large differences between the S and P polarizations observed previously in the emission profile of such a tip [ Obermüller and Karrai. Appl. Phys. Lett . (1995) 67 , 3408 ].     

Magnetic characterization of microscopic particles by MO-SNOM

This paper reports on the development of a magneto‐optical scanning near‐field optical microscope and the experimental near‐field study of the domain structure for a model magnetic particle of 16 × 16 µm² of a Co_70.4Fe_4.6Si₁₅B₁₀ amorphous thin film, deposited on a silicon substrate. We present the topographic, optical and magneto‐optical differential susceptibility (MODS) images of the particle. Imaging by using the local MODS reveals the domain structure. These images are also used for positioning the tip in order to acquire local hysteresis loops, with submicrometre spatial resolution.     

Influence of metal roughness on the near-field generated by an aperture/apertureless probe

We study the influence of metal roughness on the near‐field distribution generated by an aperture or an apertureless (scattering) probe. Different experimental parameters are investigated: roughness magnitude, aperture form, distribution of the roughness. Our results show that aluminium roughness has a dramatic impact on the emission characteristics of a near‐field probe and in particular on its polarization sensitivity. Apertureless or scattering probes appear to be less sensitive to roughness and to provide a well confined field even with a somewhat rough probe.     

Cathodoluminescence imaging and spectroscopy by near-field detection

Using near-field techniques, we have developed an experimental set-up for spatially resolved cathodoluminescence (CL) spectroscopy and monochromatic imaging. It combines a scanning near-field optical/force microscope with a scanning electron microscope equipped with a field emission gun. The potentialities of this scanning near-field cathodoluminescence microscope are demonstrated on two kinds of sample: an indented MgO crystal and AlGaN/GaN quantum wells grown on GaN/sapphire. Monochromatic CL imaging allows a clear distinction between the emission of quantum wells and the GaN substrate, and for the MgO crystal, the localization on the slip bands, near the indentation, of luminescent centres emitting at 450 nm.     

Morphology, fluorescence properties, and their photothermal changes of poly(substituted thiophene) films revealed by near-field fluorescence microspectroscopy

The morphology and fluorescence spectrum of poly{3-[2-(N-dodecylcarbamoyloxy)ethyl]thiophene-2,5-diyl} film were examined with spatial resolution of 100 nm using near-field fluorescence microspectroscopy. Fluorescence spectra observed at protruding domains were blue-shifted compared with flat areas, and further blue-shift was observed there more appreciably by long-time irradiation via a near-field scanning optical microscope probe. It is considered that the polymer chains at the protruding domains take disordered conformations, in which conjugated lengths are shorter and further disordering can be induced more easily by irradiation compared with those in the flat areas.     

Thickness measurement of thin dielectric films by evanescent total reflection fluorescence

The electric field of an evanescent wave generates fluorescence in the interface between a dielectric surface and an adjacent, fluorescing, medium of lower refractive index. The difference between the fluorescing signals from covered and noncovered surfaces enables nondestructive measurement of the film thickness to be made in the range 1–15 nm.     

Photoluminescence imaging of phosphor particles using near-field optical microscope with UV light excitation

We have developed fibre probes suitable for 325 nm UV light excitation and a photoluminescence near-field scanning optical microscope (NSOM) and demonstrated the photoluminescence imaging of phosphor BaMgAl₁₀O₁₇:Eu²⁺ (BAM) particles. The probe was fabricated by a two-step-etching method that we developed. The probe had a large taper angle at the top of the probe and a small taper angle at the root. The NSOM image was different from the topographical structure but roughly reflected the corresponding features of the particles. The inhomogeneity of the photoluminescence intensity between BAM particles was observed in the NSOM image. The photoluminescence intensity with various bandpass filters showed differences between the individual particles, which means that they have different spectra.     

Near-field fluorescence imaging of single molecules with a resolution in the range of 10 nm

We demonstrate fluorescence imaging of single molecules, by near-field scanning optical microscopy (NSOM), using the illumination-collection mode of operation, with an aperture probe. Fluorescence images of single dye molecules were obtained with a spatial resolution of 15 nm, which is smaller than the diameter of the aperture (20 nm) of the probe employed. Such super-resolution may be attributable to non-radiative energy transfer from the molecules to the coated metal of the probe since the resolution obtained in the case of conventional NSOM is limited to 30–50 nm due to penetration of light into the metal.     

Three-dimensional imaging in fluorescence by confocal scanning microscopy

The improved resolution and sectioning capability of a confocal microscope make it an ideal instrument for extracting three-dimensional information especially from extended biological specimens. The imaging properties, also with finite detection pinholes are considered and a number of biological applications demonstrated.     

Photoconductive imaging in a photon scanning tunnelling microscope capable of point-contact current sensing using a conductive fibre probe

A photoconductive photon scanning tunnelling microscope was developed to investigate the point-contact photoconductive properties of condensed matter. In order to detect the current and the optical signal at a local point on a surface, we coated the edge of a bent type fibre probe with indium tin oxide. Thus it was possible to measure both photocurrent and optical property with subwavelength resolution. The performance of the novel microscope was evaluated by analysing an organic thin film of copper phthalocyanine (CuPc), which is known to be an efficient photoconductive material. Photocurrent and current–voltage characteristics were observed at the local point on the CuPc thin films. Furthermore, photoconductive images were obtained with topography and near-field optical imaging using this system. The photoconductive PSTM shows potential in various areas of future optics and electronics.     

荧光成像系统对比度分析与成像仿真

目前荧光成像技术在生物医学领域得到越来越广泛的应用。为了缩短产品设计和开发周期,且能更直观地反映系统的成像效果,根据各模块光谱特性曲线,提出了荧光成像链路模型。利用该模型,对荧光成像系统的对比度进行了分析,验证了滤光片光密度(OD)值的合理范围是在5~7之间。最后以荧光显微镜为例,对系统成像过程进行了仿真。结果表明,各模块不匹配也会对系统对比度产生影响,仿真图像能够直观反映出系统的匹配程度和成像效果,并与实际系统测试结果相吻合,证明了该链路模型仿真的可行性和有效性。     

Dynamic etching method for fabricating a variety of tip shapes in the optical fibre probe of a scanning near-field optical microscope

A novel etching method for an optical fibre probe of a scanning near-field optical microscope (SNOM) was developed to fabricate a variety of tip shapes through dynamic movement during etching. By moving the fibre in two-phase fluids of HF solution and organic solvent, the taper length and angle can be varied according to the movement of the position of the meniscus on the optical fibre. This method produces both long (sharp angle) and short (wide angle) tapered tips compared to tips made with stationary etching processes. A bent-type probe for a SNOM/AFM was fabricated by applying this technique and its throughput efficiency was examined. A wide-angle probe with a 50° angle at the tip showed a throughput efficiency of 3.3 × 10⁻⁴ at a resolution of 100 nm.     

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.