Femtosecond near-field scanning optical microscopy study of molecular thin films

A near-field scanning optical microscope has been combined with a two-colour time-resolved pump-probe measurement system. It has a noise-equivalent transmittance change of 5.0 × 10⁻⁵ for a probe pulse with an intensity of 30 nW. The system has been used for evaluating molecular thin films that have a domain structure, particularly for observing a gate action of the single domains. The results include key features to understand an origin of the domains and suggest that the film composition is uniform over a distance of several micrometres.     

Demonstrating nanophotonic switching using near-field pump–probe photoluminescence spectroscopy of CuCl quantum cubes

We demonstrated a novel optical switching operation using three CuCl quantum cubes with a size ratio of . Their quantized excitonic energy levels resonate with one another, and the switching mechanism was based on the resonant near‐field energy transfer between the quantum cubes. Using near‐field pump–probe photoluminescence spectroscopy, we succeeded in controlling the near‐field energy transfer and obtained a controlled (i.e. switched) signal in a differential photoluminescence spectrum with and without a pump beam. The internal quantum efficiency of the switching operation was close to 1. These results suggest the possibility of making a nanophotonic switching device smaller than 30 nm.     

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.     

Imaging 'intact' myofibrils with a near-field scanning optical microscope

Fluorescently labelled myofibrils were imaged in physiological salt solution by near-field scanning optical microscopy and shear-force microscopy. These myofibrils were imaged in vitro , naturally adhering to glass while retaining their ability to contract. The Z-line protein structure of the myofibrils was antibody labelled and easily identified in the near-field fluorescence images. The distinctive protein banding structure of the myofibril was also seen clearly in the shear-force images without any labelling requirement. With the microscope in the transmission mode, resolution of the fluorescence images was degraded significantly by excessive specimen thickness (>1 μm), whereas the shear-force images were less affected by specimen thickness and more affected by poor adherence to the substrate. Although the exact mechanism generating contrast in the shear-force images is still unknown, shear-force imaging appears to be a promising new imaging modality.     

Broadband optical near-field microscope for nanoscale absorption spectroscopy of organic materials

The cells and tissues of many marine invertebrates and their associated flora contain fluorescent pigments and proteins, many of which have been utilized commercially and provide marker molecules in other systems for fluorescence imaging technology. However, in the study of marine invertebrates and their symbioses these naturally occurring molecules have been seen to limit or confound fluorescence microscopy analyses. Here we demonstrate the endogenous fluorescence associated with two marine invertebrates (coral and foraminifera) and describe how these qualities can be utilized in fluorescence microanalyses. Understanding and imaging the diversity of fluorescent molecules provide insight into how fluorescence microscopy techniques can now be applied to these complex systems.     

Optical microcantilever consisting of channel waveguide for scanning near-field optical microscopy controlled by atomic force

We develop a novel optical microcantilever for scanning near-field optical microscopy controlled by atomic force mode (SNOM/AFM). The optical microcantilever has the bent channel waveguide, the corner of which acts as aperture with a large tip angle. The resonance frequency of the optical microcantilever is 9 kHz, and the spring constant is estimated to be 0.59 N/m. The optical microcantilever can be operated in contact mode of SNOM/AFM and we obtain the optical resolution of about 200 nm, which is as same size as the diameter of aperture. We confirm that the throughput of optical microcantilever with an aperture of 170 nm diameter would be improved to be more than 10⁻⁵.     

Current-sensing scanning near-field optical microscopy using a metal probe for nanometre-scale observation of electrochromic films

A novel technique for scanning near‐field optical microscopy capable of point‐contact current‐sensing was developed in order to investigate the nanometre‐scale optical and electrical properties of electrochromic materials. An apertureless bent‐metal probe was fabricated in order to detect optical and current signals at a local point on the electrochromic films. The near‐field optical properties could be observed using the local field enhancement effect generated at the edge of the metal probe under p‐polarized laser illumination. With regard to electrical properties, current signal could be detected with the metal probe connected to a high‐sensitive current amplifier. Using the current‐sensing scanning near‐field optical microscopy, the surface topography, optical and current images of coloured WO₃ thin films were observed simultaneously. Furthermore, nanometre‐scale electrochromic modification of local bleaching could be performed using the current‐sensing scanning near‐field optical microscopy. The current‐sensing scanning near‐field optical microscopy has potential use in various fields of nanometre‐scale optoelectronics.     

Tapping-mode tuning-fork near-field scanning optical microscopy of low power semiconductor lasers

The newly developed inverted tapping-mode tuning-fork near-field scanning optical microscopy (TMTF-NSOM) is used to study the local near-field optical properties of strained AlGaInP/Ga_0.4In_0.6P low power visible multiquantum-well laser diodes. In contrast to shear-force mode NSOM, TMTF-NSOM provides the function to acquire the evanescent wave intensity ratio | I (2ω)|/| I (ω)| image, from which the evanescent wave decay coefficient q can be evaluated for a known tapping amplitude. Moreover, we probe the near-field stimulated emission spectrum, which gives the free-space laser light wavelength λ_o and the index of refraction n _r of the laser diode resonant cavity. Once q , λ_o, and n _r are all measured, we can determine the angle of incidence θ_o of the dominant totally internally reflected waves incident on the front mirror facet of the resonator. Determination of such an angle is very important in modelling the stability of the laser diode resonator.     

A scanning near-field optical microscope having scanning electron tunnelling microscope capability using a single metallic probe tip

A new microscope system that has the combined capabilities of a scanning near-field optical microscope (SNOM) and a scanning tunnelling microscope (STM) is described. This is achieved with the use of a single metallic probe tip. The distance between the probe tip and the sample surface is regulated by keeping the tunnelling current constant. In this mode of operation, information about the optical properties of the sample, such as its refractive index distribution and absorption characteristics, can be disassociated from the information describing its surface structure. Details of the surface structure can be studied at resolutions smaller than the illumination wavelength. The performance of the microscope is evaluated by analysing a grating sample that was made by coating a glass substrate with gold. The results are then compared with the corresponding SNOM and STM images of the grating.     

Scanning near-field optical microscopy of a cell membrane in liquid

The applications of scanning near‐field optical microscopy to biological specimens under physiological conditions have so far been very rare since common techniques for a probe–sample distance control are not as well suited for operation in liquid as under ambient conditions. We have shown previously that our own approach for a distance control, based on a short aperture fibre probe and a tuning fork as force sensor in a tapping mode, works well even on soft material in water. By means of an electronic self‐excitation circuit, which compensates for changes of the resonance frequency due to evaporation of liquid, the stability of the force feedback has now been further improved. We present further evidence for the excellent suitability of the tapping‐mode‐like distance control to an operation in liquid, for example, by force‐imaging of double‐stranded DNA. Moreover, we demonstrate that a nuclear envelope in liquid can be imaged with a high optical resolution of ～70 nm without affecting its structural integrity. Thereby, single nuclear pores in the nuclear envelope with a nearest neighbour distance of ～120 nm have been optically resolved for the first time.     

Autocorrelation spectroscopy on single ultrathin layers of CdSe/ZnSe: hints for a non-thermal distribution of excitons in quantum islands

Autocorrelation spectroscopy on the basis of thousands of individual near-field photoluminescence spectra of single ultrathin CdSe layers at low temperatures exhibits a strong positive correlation peak around 18 meV energy with a width of 5 meV. Using simulations and experiments as a function of temperature and laser intensity, we can exclude interpretations along the lines of biexcitons or phonon sidebands. We attribute this feature to the splitting of ground state and an excited state in individual quantum islands. This interpretation implies that the potential minima are rather uniform in size and that the distribution of excitons is nonthermal.     

Detection of an infrared near-field optical signal by attaching an infrared-excitable phosphor to the end of a photocantilever

To improve the signal-to-noise ratio of near-field scanning optical microscopy, we propose attaching an infrared-excitable phosphor (IEP) to a photocantilever. One source of noise is the light scattered from locations on the sample surface other than that of the probe tip. By detecting only the light scattered from the tip, we can obtain a near-field optical signal without noise. We attached an IEP particle to a photocantilever to convert infrared light to visible light and we used 1550-nm infrared illumination, so the light scattered from the sample was only infrared. The silicon photodiode of the photocantilever is 10⁶ times less sensitive to infrared light than to visible light. As a result, only the converted visible light from the IEP particle, i.e. the signal containing the near-field optical information from the tip, was detected. We verified that the photocantilever detected the signal in the evanescent light produced by infrared illumination and that the detected signal was the light converted by the IEP. The experimental results show the feasibility of detecting infrared light and not the background light through the use of the IEP.     

The effects of probe boundary conditions and propagation on nano-Raman spectroscopy

Raman spectra obtained in the near‐field, with collection of the Raman‐shifted light in reflection, show selective enhancement of vibrational modes. We show that the boundary conditions for an electric field near a metal surface affect propagation of the reflected signal and lead to this selection. The enhancement of certain Raman forbidden vibrations is explained by the presence of an electric field gradient near the metal‐apertured fibre probe.     

Photonic nanopatterns of gold nanostructures indicate the excitation of surface plasmon modes of a wavelength of 50–100 nm by scanning near-field optical microscopy

Scanning near‐field optical microscopy images of metal nanostructures taken with the tetrahedral tip (T‐tip) show a distribution of dark and bright spots at distances in the order of 25–50 nm. The images are interpreted as photonic nanopatterns defined as calculated scanning near‐field optical microscopy images using a dipole serving as a light‐emitting scanning near‐field optical microscopy probe. Changing from a positive to a negative value of the dielectric function of a sample leads to the partition of one spot into several spots in the photonic nanopatterns, indicating the excitation of surface plasmons of a wavelength in the order of 50–100 nm in metal nanostructures.     

Study of energy transfer from excited TPD to Alq in organic electroluminescent devices by time-resolved fluorescence spectroscopy using a scanning near-field optical atomic force microscope

We demonstrate the direct measurement of molecular diffusion at organic/organic interfaces of organic electroluminescence devices by use of a scanning near-field optical atomic force microscope. Our preliminary study shows that the degradation of an electroluminescence device is partly caused by crystallization of the organic layers. Because the initial stage of degradation cannot be observed by microscopic methods, nanoscale optical properties of the interface in multilayer systems are currently receiving a great deal of attention. Defects of organic electroluminescence devices were investigated using a scanning near-field optical atomic force microscope. This instrument is capable of measuring both a topographic and a fluorescence image at the same time. The defect area and other areas are clearly observed and time-resolved near-field fluorescence spectra demonstrate emission of the different species. These results suggest that defects occur at the organic solid interface, and that energy transfer occurs from excited TPD, as donor, to Alq, as acceptor.     

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.     

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.