Apertureless Scanning Near-field Optical Microscopy Research Articles

Optical imaging beyond the diffraction limit by SNEM: effects of AFM tip modifications with thiol monolayers on imaging quality.

Tip-enhanced nanoscale optical imaging techniques such as apertureless scanning near-field optical microscopy (a-SNOM) and scanning near-field ellipsometric microscopy (SNEM) applications can suffer from a steady degradation in performance due to adhesion of atmospheric contaminants to the metal coated tip. Here, we demonstrate that a self-assembled monolayer (SAM) of ethanethiol (EtSH) is an effective means of protecting gold-coated atomic force microscopy (AFM) probe tips from accumulation of surface contaminants during prolonged exposure to ambient air. The period over which they yield consistent and reproducible results for scanning near-field ellipsometric microscopy (SNEM) imaging is thus extended. SNEM optical images of a microphase separated polystyrene-block-poly (methylmethacrylate) (PS-b-PMMA) diblock copolymer film, which were captured with bare and SAM-protected gold-coated AFM probes, both immediately after coating and following five days of storage in ambient air, were compared. During this period the intensity of the optical signals from the untreated gold tip fell by 66%, while those from the SAM protected tip fell by 14%. Additionally, gold coated AFM probe tips were modified with various lengths of alkanethiols to measure the change in intensity variation in the optical images with SAM layer thickness. The experimental results were compared to point dipole model calculations. While a SAM of 1-dodecanethiol (DoSH) was found to strongly suppress field enhancement we find that it can be locally removed from the tip apex by deforming the molecules under load, restoring SNEM image contrast.

Sub-100 nm focusing of short wavelength plasmons in homogeneous 2D space.

We present a direct measurement of short-wavelength plasmons focused into a sub-100 nm spot in homogeneous (translation invariant) 2D space. The short-wavelength (SW) surface plasmon polaritons (SPP) are achieved in metal-insulator-insulator (MII) platform consisting of silver, silicon nitride, and air. This platform is homogeneous in two spatial directions and supports SPP at wavelength more than two times shorter than that in free space yet interacts with the outer world through the evanescent tail in air. We use an apertureless (scattering) near-field scanning optical microscope (NSOM) to map directly the amplitude and phase of these SW-SPP and show they can be focused to under 70 nm without structurally assisted confinement such as nanoantennas or nanofocusing. This, along with the use of visible light at 532 nm which is suitable for optical microscopy, can open new directions in direct biological and medical imaging at the sub-100 nm resolution regime.

Laser fabrication of gold nanoparticle clustered tips for use in apertureless near-field scanning optical microscopy.

A laser fabrication method was developed to make gold nanoparticle clustered (GNC) tips for apertureless near-field scanning optical microscopes (ANSOMs) and tip-enhanced Raman spectroscopy (TERS). The near-field Rayleigh and Raman scattering of samples are highly enhanced when a gold nanoparticle cluster is synthesized on the end of the tip. This is due to the lightning rod effect in the sharp tips. The localized electromagnetic field enhancement and the spatial resolution (~30 nm) of the fabricated GNC tip were verified by TERS and ANSOM measurements of carbon nanotubes.

Laser-induced cantilever behaviour in apertureless scanning near-field optical microscopes

The laser-induced deformation of a typical commercial cantilever commonly used for scanning near-field optical microscopes was investigated by means of a software package based on the finite element method. The thermo-mechanical behaviour of such a cantilever whose tip was irradiated by a laser beam was calculated in the temperature regime between room temperature and 850 K. The spatial tip displacement was simulated at timescales <0.1 ms, since feedback-based constant force measurements exhibit reaction times in this range. It could be shown that in addition to former tip-based thermal expansion calculations the cantilever deformation is already significant at moderate temperatures, particularly when a reflective coating is present. The experimental and calculated results suggest that tip scanning in cantilever-based scanning probe microscopes for laser-based surface modification applications should be performed in thermal equilibrium.

Direct Near-Field Observation of Orientation-Dependent Optical Response of Gold Nanorods

The orientation-dependent optical response of short gold nanorods (length less than 100 nm) has been directly observed in the near-field, mapping the in-plane and out-of-plane vector components selectively using interferometric apertureless near-field scanning optical microscope. For the gold nanorods dispersed randomly on oxide-coated silicon wafer, the optical amplitude and phase contrast that are characteristic of the longitudinal and transverse mode dipolar plasmon resonances have been clearly resolved when the long axes of the nanorods are aligned parallel and perpendicular to the electric field of the laser, respectively. The near-field amplitude ratio of the longitudinal to the transverse plasmon mode is much smaller than the corresponding ratio of the scattering cross section, indicating the more efficient coupling of the longitudinal mode to the far-field than the transverse mode. This near-field amplitude ratio increases with the length-to-width aspect ratio of the nanorods, and electromagnetic ...

Spaser spectroscopy with subwavelength spatial resolution

We propose a method for high-sensitivity subwavelength spectromicroscopy based on the usage of a spaser (plasmonic nanolaser) in the form of a scanning probe microscope tip. The high spatial resolution is defined by plasmon localization at the tip, as is the case for apertureless scanning near-field optical microscopy. In contrast to the latter method, we suggest using radiationless plasmon pumping with quantum dots instead of irradiation with an external laser beam. Due to absorption at the transition frequencies of neighboring nano-objects (molecules or clusters), dips appear in the plasmon generation spectrum. The highest sensitivity is achieved near the generation threshold. • A new method for high-sensitivity subwavelength spectromicroscopy is proposed. • The method uses spaser (plasmonic nanolaser) in the form of a scanning probe microscope tip. • The high spatial resolution is defined by plasmon localization at the needle tip. • The highest sensitivity is achieved near the generation threshold.

Optical near-field excitation at commercial scanning probe microscopy tips: a theoretical and experimental investigation

A systematic study of the influence of the excitation angle, the light polarization and the coating thickness of commercial SPM tips on the field enhancement in an apertureless scanning near-field optical microscope is presented. A new method to optimize the alignment of the electric field vector along the major tip axis by measuring the resonance frequency was developed. The simulations were performed with a MNPBEM toolbox based on the Boundary Element Method (BEM). The influence of the coating thickness was investigated for the first time. Coatings below 40 nm showed a drastic influence both on the resonance wavelength and the enhancement. A shift to higher angles of incidence for the maximum enhancement could be observed for greater tip radii.

Inverse extraction of material properties by apertureless scanning near-field optical microscopy using phenomenological model

Apertureless scanning near-field optical microscopy (a-SNOM) enables the surface properties of optically scattering materials to be measured with ultrahigh resolution. However, the detection signal is inevitably contaminated by background signal. The literature contains various configurations capable of directly obtaining a background-free detection signal of a-SNOM, but these methods generally require the use of a complex experimental setup and strict calibration. Accordingly, the present study provides a robust phenomenological model with a genetic algorithm (GA) for inversely extracting material properties without using a background-free signal from a complex experimental setup. Finally, the properties of SiC crystal in different structures are successfully and inversely extracted by only using the first and second orders of modulation signals as multiple objective functions in the curve-fitting GA.

Apertureless scanning near-field optical microscopy of sparsely labeled tobacco mosaic viruses and the intermediate filament desmin

Both fluorescence imaging and atomic force microscopy (AFM) are highly versatile and extensively used in applications ranging from nanotechnology to life sciences. In fluorescence microscopy luminescent dyes serve as position markers. Moreover, they can be used as active reporters of their local vicinity. The dipolar coupling of the tip with the incident light and the fluorophore give rise to a local field and fluorescence enhancement. AFM topographic imaging allows for resolutions down to the atomic scale. It can be operated in vacuum, under ambient conditions and in liquids. This makes it ideal for the investigation of a wide range of different samples. Furthermore an illuminated AFM cantilever tip apex exposes strongly confined non-propagating electromagnetic fields that can serve as a coupling agent for single dye molecules. Thus, combining both techniques by means of apertureless scanning near-field optical microscopy (aSNOM) enables concurrent high resolution topography and fluorescence imaging. Commonly, among the various (apertureless) SNOM approaches metallic or metallized probes are used. Here, we report on our custom-built aSNOM setup, which uses commercially available monolithic silicon AFM cantilevers. The field enhancement confined to the tip apex facilitates an optical resolution down to 20 nm. Furthermore, the use of standard mass-produced AFM cantilevers spares elaborate probe production or modification processes. We investigated tobacco mosaic viruses and the intermediate filament protein desmin. Both are mixed complexes of building blocks, which are fluorescently labeled to a low degree. The simultaneous recording of topography and fluorescence data allows for the exact localization of distinct building blocks within the superordinate structures.

Cold field emission electrode as a local probe of proximal microscopes: Investigation of defects in monocrystalline silicon solar cells

Monocrystalline silicon is still very interesting material for solar cells fabrication due to its quality and external efficiency. Nevertheless during a tailoring of eligible silicon wafers, some inhomogeneities or irregularities emerge and provide defects which give trouble to good operation of solar panels. Generally, there are two classes of defects in silicon wafer: material defects due to imperfections or irregularity in crystal structure (point, line, square or volume defects), and defects induced by wafer processing. To avoid a use of damaged cells, macroscopic and microscopic measurement techniques must be applied. In this paper we present a microscopic method combining electrical noise measurements with scanning probe localization of luminous micro-spots defects. The paper brings experimental results showing local electric and optical investigations of defects in etched monocrystalline silicon solar cells and a use of cold field emission tungsten electrode as a local probe for apertureless scanning near-field optical microscope.

Phase Controlled Homodyne Infrared Near-Field Microscopy and Spectroscopy Reveal Inhomogeneity within and among Individual Boron Nitride Nanotubes

We propose a practical method to obtain near-field infrared absorption spectra in apertureless near-field scanning optical microscopy (aNSOM) through homodyne detection with a specific choice of reference phase. The underlying mechanism of the method is illustrated by theoretical and numeric models to show its ability to obtain absorptive rather than dispersive profiles in near-field infrared vibrational microscopy. The proposed near-field nanospectroscopic method is applied to obtain infrared spectra from regions of individual multiwall boron nitride nanotubes (BNNTs) in spatial regions smaller than the diffraction limit of the light source. The spectra suggest variations in interwall spacing within the individual tubes probed.

Observation of Near-Field Dipolar Interactions Involved in a Metal Nanoparticle Chain Waveguide

We present near-field measurements of transverse plasmonic wave propagation in a chain of gold elliptical nanocylinders fed by a silicon refractive waveguide at optical telecommunication wavelengths. Eigenmode amplitude and phase imaging by apertureless scanning near-field optical microscopy allows us to measure the local out-of-plane electric field components and to reveal the exact nature of the excited localized surface plasmon resonances. Furthermore, the coupling mechanism between subsequent metal nanoparticles along the chain is experimentally analyzed by spatial Fourier transformation on the complex near-field cartography, giving a direct experimental proof of plasmonic Bloch mode propagation along array of localized surface plasmons. Our work demonstrates the possibility to characterize multielement plasmonic nanostructures coupled to a photonic waveguide with a spatial resolution of less than 30 nm. This experimental work constitutes a prerequisite for the development of integrated nanophotonic devices.

Tip-enhanced sub-diffraction fluorescence imaging of nitrogen-vacancy centers in nanodiamonds

This work demonstrates that the gold tip of an atomic force microscope enhances not only the fluorescence of the nitrogen-vacancy centers in nanodiamonds but also improves the optical resolution of the fluorescence image of the particles down to 40 nm in an apertureless near-field scanning optical microscope. With the tip in close contact with 20–30 nm diamonds, the average fluorescence intensity enhancement is 3. By measuring the fluorescence decay lifetime and the saturation intensity, we confirm that the fluorescence enhancement is contributed predominantly by the increase of the radiative decay rate.

Scanning Head for the Apertureless near Field Optical Microscope

The design and characterization of a tip control unit for an apertureless scanning near field optical microscope (ASNOM) is reported. To make the instrument operation easier, the cantilever control parts (piezo excitation of the cantilever vibration for the dynamic mode feedback and the parts necessary for the optical lever scheme of the vibration control) were placed in a separate detachable assembly. To suppress the influence of vibrations of the setup, the assembly was made lightweight. Good optical access to the ASNOM tip from various directions is provided in the system. High long-term mechanical stability of the system (~50 nm lateral drift in 18 hours) as well as low sensitivity to seismic vibrations (~400 pm RMS) is demonstrated. It is shown that external sound is not a main source of noise in the topography image (~200 pm RMS). The light field distribution (with its amplitude and phase) around the ASNOM tip was acquired by scanning the focal spot around the tip, and a high optical quality of the system is demonstrated.

G031094 斜め入射型近接場ラマン分光法によるSiのスペクトル評価([G03-09]材料力学部門,一般セッション : 変形,ひずみ)

In this study, near-field Raman spectroscopy with high special resolution has been developed. This near-field Raman spectroscopy system consists of scanning near-field optical microscopy (SNOM) and polarized micro-Raman spectroscopy with oblique backscattering configuration. By using this system, near-field Raman spectrum of Si was evaluated. However, it was very difficult to detect Raman signal because near-field Raman scattering signal was very weak. To improve the signal, tip-enhanced system was added to developed system. Au coating apertureless SNOM probe has been developed by FIB machining. The curvature radius of this probe tip is less than 50nm. Polarized oblique incident light was irradiated to the probe tip and Raman scattering light was detected. As a result, enhancement of Raman scattering intensity was observed in the transition region from non-contact to contact of probe tip. Therefore, near-field Raman Spectrum of Si was able to be evaluated by near-field Raman spectroscopy with oblique backscattering configuration.

Reciprocity Theory of Apertureless Scanning Near-Field Optical Microscopy with Point-Dipole Probes

Near-field microscopy offers the opportunity to reveal optical contrast at deep subwavelength scales. In scanning near-field optical microscopy (SNOM), the diffraction limit is overcome by a nanoscopic probe in close proximity to the sample. The interaction of the probe with the sample fields necessarily perturbs the bare sample response, and a critical issue is the interpretation of recorded signals. For a few specific SNOM configurations, individual descriptions have been modeled, but a general and intuitive framework is still lacking. Here, we give an exact formulation of the measurable signals in SNOM which is easily applicable to experimental configurations. Our results are in close analogy with the description Tersoff and Hamann have derived for the tunneling currents in scanning tunneling microscopy. For point-like scattering probe tips, such as used in apertureless SNOM, the theory simplifies dramatically to a single scalar relation. We find that the measured signal is directly proportional to the field of the coupled tip-sample system at the position of the tip. For weakly interacting probes, the model thus verifies the empirical findings that the recorded signal is proportional to the unperturbed field of the bare sample. In the more general case, it provides guidance to an intuitive and faithful interpretation of recorded images, facilitating the characterization of tip-related distortions and the evaluation of novel SNOM configurations, both for aperture-based and apertureless SNOM.

Direct mapping of plasmonic coupling between a triangular gold island pair

Local plasmonic coupling between a triangular gold island pair is observed with high spatial resolution (∼10 nm) by an apertureless scanning near-field optical microscope. The measured local field distribution is fully reproduced by three dimensional numerical simulations. Our results show a strong near-field coupling between two adjacent gold triangles, which gives direct evidence to the local field enhancement in plasmonic nanoantenna effect.

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.

Multi-wavelength mid-infrared plasmonic antennas with single nanoscale focal point

We propose and demonstrate a novel photonic-plasmonic antenna capable of confining electromagnetic radiation at several mid-infrared wavelengths to a single sub-wavelength spot. The structure relies on the coupling between the localized surface plasmon resonance of a bow-tie nanoantenna with the photonic modes of surrounding multi-periodic particle arrays. Far-field measurements of the transmission through the central bow-tie demonstrate the presence of Fano-like interference effects resulting from the interaction of the bow-tie antenna with the surrounding nanoparticle arrays. The near-field of the multi-wavelength antenna is imaged using an aperture-less near-field scanning optical microscope. This antenna is relevant for the development of near-field probes for nanoimaging, spectroscopy and biosensing.

Development of a Backscattering Type Ultraviolet Apertureless Near-Field Scanning Optical Microscope

A backscattering type ultraviolet apertureless near-field scanning optical microscope (ANSOM) for the correlated measurement of topographical and optical characteristics of photonic materials with high optical resolution was developed. The near-field Rayleigh scattering image of GaN covered with periodic submicron Cr dots showed that optical resolution around 40 nm was achievable. By measuring the tip scattered photoluminescence of InGaN/GaN multi quantum wells, the applicability of the developed microscope for high resolution fluorescence measurement was also demonstrated.