Photopatterning of a monomolecular dye film by means of scanning near-field optical microscopy

Patterned bleaching of a photolabile monomolecular dye film by means of scanning near-field optical microscopy (SNOM) is demonstrated. After exposure, the written patterns were verified by SNOM with fluorescence detection. The adsorption of appropriate material to such near-field optically created patterns seems now feasible. The ultimate resolution limit of a monomolecular dye film for patterned bleaching by SNOM is discussed on the basis of a simple model.     

Scanning Near-Field Optical Microscopy and Microspectroscopy of Green Fluorescent Protein in Intact Escherichia coli Bacteria

Scanning near-field optical microscopy (SNOM) yields high-resolution topographic and optical information and constitutes an important new technique for visualizing biological systems. By coupling a spectrograph to a near-field microscope, we have been able to perform microspectroscopic measurements with a spatial resolution greatly exceeding that of the conventional optical microscope. Here we present SNOM images of Escherichia coli bacteria expressing a mutant green fluorescent protein (GFP), an important reporter molecule in cell, developmental, and molecular biology. Near-field emission spectra confirm that the fluorescence detected by SNOM arises from bacterially expressed GFP molecules.     

Scanning near-field optical microscopy-based study of local dynamics of receptor-ligand interactions at the single molecule level

A scanning near-field optical microscope (SNOM)—based modification of the method to study the dynamics of single molecule receptor—ligand interactions exploiting the fluorescence imaging by total internal reflection fluorescence microscopy is introduced. The main advantage of this approach consists in the possibility to study the single molecule interaction dynamics with a subwavelength spatial resolution and a submillisecond time resolution. Additionally, due to the much smaller irradiation area and some other technical features, such a modification enables to enlarge the scope of the receptor—ligand pairs to be investigated and to improve the temporal resolution. We briefly discuss corresponding experimental set up with a special accent on the SNOM operation in liquid and present some preliminary results of related investigations.     

Scanning near-field optical/atomic force microscopy for fluorescence imaging and spectroscopy of biomaterials in air and liquid: Observation of recombinantEscherichia coli with gene coding to green fluorescent protein

We have developed a system of scanning near-field optical/atomic force microscopy (SNOM/AFM) for fluorescence imaging and spectroscopy of biomaterials in air and liquid. SNOM/AFM uses a bent optical fiber simultaneously as a dynamic force AFM cantilever and a SNOM probe. Optical resolution of SNOM images shows about 50 nm in an illumination mode for a standard sample of a patterned chromium layer of 20 nm thickness on a quartz glass plate. The SNOM/AFM system contains a photon counting system and polychrometer/ICCD (intensified charge coupled device) system for observation of the fluorescence image and spectrograph of micro areas, respectively. The gene coding to green fluorescence protein (GFP) was cloned in recombinantEscherichia coli (E. coli). Topography, fluorescence image and spectrograph of recombinantE. coli by SNOM/AFM showed a difference in fluorescence in individualE. coli. Fluorescence activity of GFP can thus be used as a convenient indicator of transformation. SNOM/AFM is also applicable to observe immobilizedE. coli on a glass plate in water with a liquid chamber and may allow the viewing of observation of floating organisms.     

Probing the superfluid velocity with a superconducting tip: the Doppler shift effect

We address the question of probing the supercurrents in superconducting (SC) samples on a local scale by performing scanning tunneling spectroscopy (STS) experiments with a SC tip. In this configuration, we show that the tunneling conductance is highly sensitive to the Doppler shift term in the SC quasiparticle (QP) spectrum of the sample, thus allowing the local study of the superfluid velocity. Intrinsic screening currents, such as those surrounding the vortex cores in a type II SC in a magnetic field, are directly probed. With Nb tips, the STS mapping of the vortices, in single crystal 2H-NbSe(2), reveals both the vortex cores, on the scale of the SC coherence length xi, and the supercurrents, on the scale of the London penetration length lambda. A subtle interplay between the SC pair potential and the supercurrents at the vortex edge is observed. Our results open interesting prospects for the study of screening currents in any superconductor.     

Theoretical Analyses on the Resolution of Collection Mode Scanning Near-Field Optical Microscopy

Numerical simulations have been carried out in the framework of waveguide theory to model collection mode scanning near-field optical microscopy (SNOM). The theoretical model includes the optical fiber end and describes the metal coated aperture on the probe tip. The developed formalism goes beyond the existing Bethe-Bouwkamp theories for electromagnetic transmission of subwavelength apertures. The finite coating and optical fiber end are now taken into account. The new features enable us to simulate the near-field probes that are widely used in the collection mode SNOM. The emphases of the numerical analyses have been mainly on the resolution mechanism of the microscopy. Influence on the resolution from important parameters of the probe tips, such as the size of the apertures and the probe-sample distance, is extensively studied. The resolution dependence has been analyzed in the light of the near-field coupling efficiency of the probe tip. An optimum tip size has been found which is balanced between the significant signal transmission and the resolution of the device.     

25 nm resolution single molecular fluorescence imaging by scanning near-field optical/atomic force microscopy

High-resolution single molecular near-field fluorescence images were observed by scanning near-field optical/atomic force microscopy (SNOM/AFM). We modified the SNOM/AFM for both high-resolution fluorescence imaging and high-resolution topographic imaging. The imaged fluorophore, Alexa 532, is prepared with a poly-methyl-methacrylate (PMMA) film coating. A fluorescence resolution of 25 nm was obtained with a simultaneous topographic image of a flat surface. A sample prepared with a lower PMMA concentration exhibited a rough surface in the micro area. The results for the flat surface indicated that the fluorescence resolution is worst in the rough surface sample, that the maximum fluorescence intensities for the individual fluorophore are similar, and that the decay rate is faster. Thus, we concluded that the morphological effect is an important factor in fluorescence image resolution and the apparent lifetimes of the fluorescence molecules.     

Observation of amplitude and phase in ridge and photonic crystal waveguides operating at 1.55 microm by use of heterodyne scanning near-field optical microscopy

We apply heterodyne scanning near-field optical microscopy (SNOM) to observe with subwavelength resolution the amplitude and phase of optical fields propagating in several microfabricated waveguide devices operating around the 1.55 microm wavelength. Good agreement between the SNOM measurements and predicted optical mode propagation characteristics in standard ridge waveguides demonstrates the validity of the method. In situ observation of the subwavelength-scale distribution and propagation of optical fields in straight and 90 degrees bend photonic crystal waveguides facilitates a more detailed understanding of the optical performance characteristics of these devices and illustrates the usefulness of the technique for investigating nanostructured photonic devices.     

Thermal,spectroscopic and structural characterization of isostructural phase transition in 4-hydroxybenzaldehyde

Polycrystalline samples of 4-hydroxybenzaldehyde (4-HOBAL) were investigated using differential scanning calorimeter (DSC), Raman spectroscopy and X-ray powder diffraction. The DSC data indicated that 4-HOBAL on heating undergoes a polymorphic transformation from polymorph I to polymorph II. The polymorph II formed remains metastable at ambient condition and transforms to polymorph I when annealed at ambient temperature for more than seven days. The structural information of polymorphs I and II obtained using its X-ray powder diffraction patterns indicated that 4-HOBAL undergoes an isostructural phase transition from polymorph I (monoclinic, P2₁/c) to polymorph II (monoclinic, P2₁/c). Raman data suggest that this structural change is associated with some change in its molecular interactions. Thus, in 4-HOBAL the polymorphic phase transformation (II to I) even though energetically favoured is kinetically hindered.     

SNOM应用于光电材料和器件的光学特性的探测和表征

介绍了近场光学及近场探测的原理 ,给出了其用于光电器件研究中的一些结果。近场光学方法具有超衍射分辩的本领和纳米局域光场探测的能力 ,适用于多种光电材料的探测与表征 ,包括 :LD、光纤波导器件、光子晶体器件等。纳米局域光场和倏逝场的探测发现了许多远场探测无法得到的结果 ,为光电器件纳米结构的研究提供了有力证据     

Study of the optically diffused reflectance and thermal-microstructure for the phase transformation of AgNO3

Optical, microstructural, and thermal properties of the investigated silver nitrate samples were characterized by various techniques, such as X-ray analysis, scanning electron microscopy, UV–Vis–NIR absorption and differential scanning calorimetry (DSC). The presence of structural phase transition [orthorhombic structure (phase II) to rhombohedral structure (phase I)] was checked by DSC and X-ray analysis measurements. The thermal energy required for such transformation is found to be 11.6 J/g. The optical band gaps of AgNO₃ are 1.4 and 2.02 eV for phase II and phase I, respectively, at the low-energy region. But at high-energy region, the optical band gaps are 3.41 and 3.43 eV for phase II and phase I, respectively. Characteristic peaks for AgNO₃ corresponding to (2 1 1), (0 0 4) and (3 5 1) for phase II and (0 0 4), (3 1 1) and (0 2 4) for phase I have been observed. The average crystalline size for AgNO₃ samples and the values of dislocation density δ and the strain ε for the planes of two phases II and I are calculated and also the texture coefficient is determined. Such information can considerably aid in understanding the process of phase transformations in AgNO₃.     

“禁戒光”近场光学显微镜原理与系统

扫描近场光学显微术是８０年代后期发展起来的一种分辨率超过衍射极限的新型光学显微镜技术。本文介绍了国外最近出现的“禁戒光”近场光学显微镜系统的工作原理及结构。透射式ＳＮＯＭ中部分光沿着光轴向前传播；部分光沿着大于全内反射临界角的方向传播。前者称为允许光；后者称为禁戒光。应用“禁戒光”近场光学显微镜可同时获得三幅图像，即允许光像、禁戒光像和反映样品表面形貌的剪切力图像。禁戒光图像能够提供很好的对比度和分辨率。     

突破分辨率极限的拉曼光谱学——简介近场光学与近场拉曼光谱

突破分辨率极限的拉曼光谱学——简介近场光学与近场拉曼光谱张树霖（北京大学物理系北京１００８７１）ＴｈｅＲａｍａｎＳｐｅｃｔｒｏｓｃｏｐｙＢｒｏｋｅｎｔｈｅＤｉｆｒａｃｔｉｏｎＬｉｍｉｔａｔｉｏｎ——Ｉｎｔｒｏｄｕｃｔｉｏｎｔｏｔｈｅｎｅａｒ－ｆｉｅｌ...     

AFM and SNOM characterization of carboxylic acid terminated silicon and silicon nitride surfaces

Silicon and silicon nitride surfaces have been successfully terminated with carboxylic acid monolayers and investigated by atomic force microscopy (AFM) and scanning near-field optical microscopy (SNOM). On clean Si surface, AFM showed topographical variations of 0.3-0.4 nm while for the clean Si₃N₄ surface the corrugation was around 3-4 nm. After material deposition, the corrugation increased in both samples with a value in topography of 1-2 nm for Si and 5-6 nm for Si₃N₄. The space distribution of specific chemical species was obtained by taking SNOM reflectivity at several infrared wavelengths corresponding to stretch absorption bands of the material. The SNOM images showed a constant contribution in the local reflectance, suggesting that the two surfaces were uniformly covered.     

Inspection of nano-sized SNOM-tips by optical far-field evaluation

High resolution optical microscopy has many interesting applications in solid state physics, low temperature physics, biology and semiconductor technology. Unfortunately, the lateral resolution of conventional microscopes is limited by the Rayleigh-limit. “Scanning nearfield optical microscopy” (SNOM) seems to be a promising new approach to characterize the properties of materials optically with a high lateral resolution of 50–100 nm. The most important part of such a microscope is the scanning probe (a special glass fiber tip). However, the quality of the optical fiber tip is of decisive importance. Since the production process of pulled and coated glass fiber tips is still highly empirical and error-prone, a technique would be useful to determine the tips’ quality before they are shipped to the user or mounted in the microscope. The tips’ apertures are smaller than λ/2 and therefore they cannot be measured in a non-destructive way by conventional optical microscopy. This paper discusses an easy and fast method for the optical characterization of common glass fiber SNOM tips. The effective aperture of the tip is measured from the far-field distribution of the emitted intensity recorded by a CCD target. A numerical model is introduced to solve this inverse task and a simple optical setup is presented to detect light emitted by the tip at an angle of up to 90° from the optical axis. Experimental investigation, near/far-field calculations and scanning electron microscope investigations show the working principle of this measurement technique for the analysis and evaluation of a typical nanostructured object.     

Influence of the probe--sample interaction on scanning near-field optical microscopic images in the far field

We have studied the influence of probe--sample interaction in a scanning near-field optical microscopy (SNOM) in the far field by using samples with a step structure. For a sample with a step height of $\sim \lambda $/4, the SNOM image contrast between the two sides of the step changes periodically at different scan heights. For a step height of $\sim \lambda $/2, the image contrast remains approximately the same. The probe--sample interaction determines the SNOM image contrast here. The influence of different refractive indices of the sample has been also analysed by using a simple theoretical model.     

Infrared near-field microscopy with the Vanderbilt free electron laser: overview and perspectives

Scanning near-field optical microscopy (SNOM) makes it routinely possible to overcome the fundamental diffraction limit of standard (far-field) microscopy. Recently, aperture-based infrared SNOM performed in the spectroscopic mode, using the Vanderbilt University free electron laser, started delivering spatially-resolved information on the distribution of chemical species and on other laterally-fluctuating properties. The practical examples presented here show the great potential of this new technique both in materials science and in life sciences.     

照明模式SNOM中样品对近场光场分布的影响

在同时考虑样品的形貌及材料光学参量和入射光偏振模式的情况下,利用基于边界元方法编写的二维矢量电磁场计算程序,对工作在照明模式下的扫描近场光学显微镜（Scanning Near-field Optical Microscope,SNOM）的近场矢量电磁场分布进行了数值计算模拟研究.结果表明,在没有表面形貌特征时,探针的光能量透射率随样品材料的折射率和损耗角的增加而增大,而样品表面光斑尺寸受折射率和损耗角的影响很小;对有形貌特征的探针扫描像研究结果表明,SNOM的分辨率随着样品的折射率和损耗角的增加而提高;对SNOM不同的工作模式的扫描成像信号进行的计算结果表明,恒定间距扫描方式比恒定高度扫描方式对样品表面的细节有较强的分辨能力.     

用扫描近场光学显微镜技术研究金膜表面等离体子共振

表面等离体子波(SPW)可与入射光横磁波极化能量耦合并被共振激发,这种现象被称为表面等离体子共振现象(SPR)。主要利用扫描近场光学显微镜(SNOM)技术和表面等离体子共振现象技术相结合,来研究金膜表面等离体子共振。设计并建立了结构独特的新型Kretschmann型表面等离体子共振现象耦合装置,同时又设计了具有厚度梯度的表面等离体子的制备方法。在此基础上,测量了改变入射角条件下的表面等离体子共振曲线,测得该装置的等离体子共振角灵敏度为1°。并且对金膜表面进行表面等离体子共振条件下的扫描近场光学显微成像。实验结果表明,在共振时金膜表面的扫描成像比不共振时清晰,而且增加了很多细节。应用表面等离体子共振现象技术将可以明显提高扫描近场光学显微镜的信噪比、分辨力等性能。     

Internal reflection mode scanning near-field optical microscopy with the tetrahedral tip on metallic samples

An internal reflection mode is introduced for scanning near-field optical microscopy (SNOM) with the tetrahedral tip. A beam of light is coupled into the tip and the light specularly reflected out of the tip is detected as a photosignal for SNOM. An auxiliary STM mode is used to control the distance during the scanning process and to record the topography of the sample simultaneously with the SNOM image. Images were obtained of different metallic samples which show a contrast in the order of 10% of the total reflected photosignal. In images of metallic samples an inverted contrast is consistently obtained compared to images previously obtained of comparable samples in a transmission mode. The contrast shows a pronounced dependence on the polarization of the incident beam with respect to the orientation of the edges of the tip. In the case of gold surfaces, the photosignal as a function of distance between the tip and the surface shows a pronounced peak in the near-field range of 0–20 nm which is tentatively attributed to the excitation of surface plasmons on the gold surface. The pronounced near-field effects and the strong contrast in the near-field images and the resolution well below 50 nm are an indication of a highly efficient coupling of the incident beam to a local excitation of the tip apex which is essential for the function of the tip as a probe for SNOM. Received: 17 May 1999 / Accepted: 18 May 1999 / Published online: 21 October 1999