Femtosecond near-field scanning optical microscopy

We have developed an instrument for optically measuring carrier dynamics in thin-film materials with approximately 150 nm lateral resolution, approximately 250 fs temporal resolution and high sensitivity. This is accomplished by combining an ultrafast pump-probe laser spectroscopic technique with a near-field scanning optical microscope. A diffraction-limited pump and near-field probe configuration is used, with a novel detection system that allows for either two-colour or degenerate pump and probe photon energies, permitting greater measurement flexibility than that reported in earlier published work. The capabilities of this instrument are proven through near-field degenerate pump-probe studies of carrier dynamics in GaAs/AIGaAs single quantum well samples locally patterned by focused ion beam (FIB) implantation. We find that lateral carrier diffusion across the nanometre-scale FIB pattern plays a significant role in the decay of the excited carriers within approximately 1 microm of the implanted stripes, an effect which could not have been resolved with a far-field system.     

Femtosecond near-field spectroscopy: carrier relaxation and transport in single quantum wires

Quasi-two-colour femtosecond pump and probe spectroscopy and near-field scanning optical microscopy are combined to study the carrier dynamics in single semiconductor nanostructures. In temporally, spectrally and spatially resolved measurements with a time resolution of 200 fs and a spatial resolution of 200 nm, the non-linear change in reflectivity of a single quantum wire is mapped in real space and time. The experiments show that carrier relaxation into a single quantum wire occurs on a 100 fs time scale at room temperature. Evidence is given for a transient unipolar electron transport along the wire axis on a picosecond time and 100 nm length scale.     

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.     

Polarization contrast in reflection near-field optical microscopy with uncoated fibre tips

Using cross-hatched, patterned semiconductor surfaces and round 20-nm-thick gold pads on semiconductor wafers, we investigate the imaging characteristics of a reflection near-field optical microscope with an uncoated fibre tip for different polarization configurations and light wavelengths. It is shown that cross-polarized detection allows one to effectively suppress far-field components in the detected signal and to realize imaging of optical contrast on the sub-wavelength scale. The sensitivity window of our microscope, i.e. the scale on which near-field optical images represent mainly optical contrast, is found to be ≈100 nm for light wavelengths in the visible region. We demonstrate imaging of near-field components of a dipole field and purely dielectric contrast (related to well-width fluctuations in a semiconductor quantum well) with a spatial resolution of ≈100 nm. The results obtained show that such a near-field technique can be used for polarization-sensitive imaging with reasonably high spatial resolution and suggest a number of applications for this technique.     

Evaluation of nano-optical probe from scanning near-field optical microscope images

We studied a nanometre-sized optical probe in a scanning near-field optical microscope. The probe profile is determined by using a knife-edge method and a modulated transfer function evaluation method which uses nanometre-sized line-and-space tungsten patterns (with spaces 1 μm to 50 nm apart) on SiO₂ substrates. The aluminium-covered, pipette-pulled fibre probe used here has two optical probes: one with a large diameter (350 nm) and the other with a small diameter (10 nm). The small-diameter probe has an optical intensity ≈63 times larger than that of the large-diameter probe, but the power is about 1/25 of that of the large probe.     

High-resolution constant-height imaging with apertured silicon cantilever probes

We present high-resolution aperture probes based on non-contact silicon atomic force microscopy (AFM) cantilevers for simultaneous AFM and near-infrared scanning near-field optical microscopy (SNOM). For use in near-field optical microscopy, conventional AFM cantilevers are modified by covering their tip side with an opaque aluminium layer. To fabricate an aperture, this metal layer is opened at the end of the polyhedral probe using focused ion beams (FIB). Here we show that apertures of less than 50 nm can be obtained using this technique, which actually yield a resolution of about 50 nm, corresponding to λ/20 at the wavelength used. To exclude artefacts induced by distance control, we work in constant-height mode. Our attention is particularly focused on the distance dependence of resolution and to the influence of slight cantilever bending on the optical images when scanning at such low scan heights, where first small attractive forces exerted on the cantilever become detectable.     

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.     

The effect of deformation on the lateral resolution of atomic force microscopy

A computer model based on the elastic properties of rubber is introduced for the evaluation of the lateral resolution in atomic force microscopy of deformable specimens. The computational results show that, if the full width at half-height can be defined as the lateral resolution, it is continuously improved at greater probe forces, at the expense of a reduced molecular height. In fact, even for a probe that is bigger than the molecule, the real size of the molecule can be 'recovered' at about 25% compression. This result demonstrates that for a better lateral resolution, a greater probe force can be beneficial, provided that the molecule is not moved or damaged and the response remains elastic. Measurements on isolated low-density lipoproteins (LDL) show that with 26% vertical compression, the lateral size measured in atomic force microscopy is only about 72% of the value predicted by a simple convolution, and is only slightly larger (≈ 13%) than the known size of LDL. Therefore, the results on LDL provide a direct support for the conclusions of the computational model.     

Inducing superconductivity at a nanoscale: photodoping with a near-field scanning optical microscope

The local modification of an insulating GdBa₂Cu₃O_6.5 thin film, made superconducting by illumination with a near-field scanning optical microscope (NSOM), is reported. A 100-nm aperture NSOM probe acts as a sub-wavelength light source of wavelength λ_exc = 480–650 nm, locally generating photocarriers in an otherwise insulating GdBa₂–Cu₃O_6.5 thin film. Of the photogenerated electron–hole pairs, electrons are trapped in the crystallographic lattice, defining an electrostatic confining potential to enable the holes to move. Reflectance measurements at λ = 1.55 μm at room temperature show that photocarriers can be induced and constrained to move on a ≈200 nm scale for all investigated λ_exc. Photogenerated wires present a superconducting critical temperature T _c = 12 K with a critical current density J _c = 10⁴ A cm⁻². Exploiting the flexibility provided by photodoping through a NSOM probe, a junction was written by photodoping a wire with a narrow (≈ 50 nm) under-illuminated gap. The strong magnetic field modulation of the critical current provides a clear signature of the existence of a Josephson effect in the junction.     

High-resolution scanning near-field EBIC microscopy: application to the characterisation of a shallow ion implanted p+-n silicon junction

High-resolution electron beam induced current (EBIC) analyses were carried out on a shallow ion implanted p⁺–n silicon junction in a scanning electron microscope (SEM) and a scanning probe microscope (SPM) hybrid system. With this scanning near-field EBIC microscope, a sample can be conventionally imaged by SEM, its local topography investigated by SPM and high-resolution EBIC image simultaneously obtained. It is shown that the EBIC imaging capabilities of this combined instrument allows the study of p–n junctions with a resolution of about 20 nm.     

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 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.     

Towards phonon photonics: scattering-type near-field optical microscopy reveals phonon-enhanced near-field interaction

Diffraction limits the spatial resolution in classical microscopy or the dimensions of optical circuits to about half the illumination wavelength. Scanning near-field microscopy can overcome this limitation by exploiting the evanescent near fields existing close to any illuminated object. We use a scattering-type near-field optical microscope (s-SNOM) that uses the illuminated metal tip of an atomic force microscope (AFM) to act as scattering near-field probe. The presented images are direct evidence that the s-SNOM enables optical imaging at a spatial resolution on a 10 nm scale, independent of the wavelength used (λ=633 nm and 10 μm). Operating the microscope at specific mid-infrared frequencies we found a tip-induced phonon-polariton resonance on flat polar crystals such as SiC and Si₃N₄. Being a spectral fingerprint of any polar material such phonon-enhanced near-field interaction has enormous applicability in nondestructive, material-specific infrared microscopy at nanoscale resolution. The potential of s-SNOM to study eigenfields of surface polaritons in nanostructures opens the door to the development of phonon photonics—a proposed infrared nanotechnology that uses localized or propagating surface phonon polaritons for probing, manipulating and guiding infrared light in nanoscale devices, analogous to plasmon photonics.     

Fabrication and observation of a standard sample for near-field optical microscopy

We fabricated a standard sample for a near-field optical microscope using scanning probe lithography. The sample contains a wedged pattern, which allows the measurement of various sizes within one image. The optical resolution of our near-field optical microscope has been evaluated as 40 nm, which was obtained by measuring the narrowest separable gap width of the wedged pattern. Thus a standard sample containing the wedged pattern enables clear evaluation of the resolution.     

Near-field optics on silicon–electrolyte junctions

A technique allowing near-field photocurrent (PC) mapping of silicon surfaces in contact with an electrolyte is presented. The illumination source is an optical fibre tip with a 100-nm aperture. A shear force detection system controls the tip–sample distance while scanning the tip across the silicon–electrolyte interface. Topographic and PC images on SiO₂/Si mesas both show 300 nm resolution. It is shown that this PC contrast is induced by the tip–topography interaction and hence the PC resolution is limited by the resolution of the topography. Indeed, PC mapping on topography-less patterned porous-silicon/silicon samples shows that the lateral resolution is only limited by the aperture size which is of the order of 100 nm.     

Nano-slit probes for near-field optical microscopy fabricated by focused ion beams

The near-field probes described in this paper are based on metallized non-contact atomic force microscope cantilevers made of silicon. For application in high-resolution near-field optical/infrared microscopy, we use aperture probes with the aperture being fabricated by focused ion beams. This technique allows us to create apertures of sub-wavelength dimensions with different geometries. In this paper we present the use of slit-shaped apertures which show a polarization-dependent transmission efficiency and a lateral resolution of < 100 nm at a wavelength of 1064 nm. As a test sample to characterize the near-field probes we investigated gold/palladium structures, deposited on an ultrathin chromium sublayer on a silicon wafer, in constant-height mode.     

Scanning force images through the 'Milliscope'– a probe microscope with very wide scan range

The effectiveness and adequacy of a home-built scanning force microscope (SFM) able to cover a volume of ∼1.2 × 1.2 × 0.13 mm³ (X × Y × Z) were tested on calibrating objects, as well as on cytological and histological samples. The instrument was designed for matching the magnification range of an optical microscope (∼ 20–1200×) but its dynamics were one or two orders of magnitude higher, thanks to a lateral resolution of about 10 nm. Images ranging in size from 1.2 × 1.2 mm² to 1 × 1 µm² showed a quality comparable to that given by other SFMs on similar materials. The 'Milliscope' is a curious but effective imaging tool whose operating range overlaps at one extreme with a goldsmith's eyepiece, and at the other with an electron microscope. The intrinsic limits of scanning probe techniques and of the available SFM cantilevers prevented us taking complete advantage of the wide height range of our scanner. However, our results show that an instrument having a very wide scan area, obtained through simple, inexpensive and intrinsically linear techniques, can give a good performance even at small scan sizes. This encourages us to develop wide scan instruments, which could further increase the already extensive use of scanning force microscopy in biology.     

Non-optical tip–sample distance control method for scanning near-field optical microscopy using a piezoresistive micro cantilever

A piezoresistive micro cantilever is applied to monitor the displacement of an optical fibre probe and to control tip–sample distance. The piezoresistive cantilever was originally made for a self-sensitive atomic force microscopy (AFM) probe and has dimensions of 400 µm length, 50 µm width and 5 µm thickness with a resistive strain sensor at the bottom of the cantilever. We attach the piezoresistive cantilever tip to the upper side of a vibrating bent optical fibre probe and monitor the resistance change amplitude of the strain sensor caused by the optical fibre displacement. By using this resistance change to control the tip–sample distance, the two-cantilever system successfully provides topographic and near-field optical images of standard samples in a scanning near-field optical microscopy (SNOM)/AFM system. A resonant characteristic of the two-cantilever system is also simulated using a mechanical model, and the results of simulation correspond to the experimental results of resonance characteristics.     

Coaxial scanning near‐field optical microscope tips: an alternative for conventional tips with high transmission efficiency?

Since the development of the first scanning near-field optical microscope, great effort has been put into the development of near-field optical probe tips with a good lateral resolution of the order of several tens of nanometres and a high power throughput. Several groups have proposed the use of scanning near-field optical tips with a coaxial structure. From electromagnetic theory, it is known that such structures have no cut-off frequency and a power transmission close to unity. In this paper we discuss some topics concerning the stimulation of optical coaxial waves and their propagation behaviour.     

Near-field spectroscopy of single quantum dots at room temperature

The observation of photoluminescence spectra of self-assembled single InGaAs quantum dots at room temperature was performed under weak excitation conditions using a near-field scanning optical microscope. Operation in illumination-collection mode with a highly sensitive double-tapered optical fibre probe enabled detection of weak photoluminescence signals at room temperature with high efficiency and high spatial resolution. Each single quantum dot was imaged with a spatial resolution of about 250 nm, which corresponded to a quarter of the wavelength of the photoluminescence from quantum dots. The photoluminescence yields of individual quantum dots were widely distributed and were found to decrease with photoluminescence energy. This result serves as a clue to be pursued for better understanding of the thermal excitation of the carrier from confined states in quantum dots.