O. Hollricher

Distance control in near-field optical microscopy with piezoelectrical shear-force detection suitable for imaging in liquids

We introduce an improved piezoelectric shear-force feedback system for tip-sample distance control in a scanning near-field optical microscope. A tapered glass fiber is glued into a metal tube and both are integrated in a mounting, sandwiched between two piezosegments. One of the piezoelements excites the fiber tip at mechanical resonance while the other one is used for detection. During surface approach the fiber resonance is damped by shear forces, which is registered by the second piezoelement and used for distance control. The main attractions of this setup are its simplicity, its compactness, and the lack of disturbing light sources. The fiber is easy accessible and tip exchange is simple. With an acceptable fiber amplitude of 5–10 nm (peak to peak) we obtained a topographical resolution of 5 pm/Hz. The geometry also allows the measurement of samples covered with a few millimeters of liquid, which is important for applications in biology and medicine.

An easy‐to‐use non‐optical shear‐force distance control for near‐field optical microscopes

We present an easy‐to‐use non‐optical shear‐force detection system for tip–sample distance control in scanning near‐field optical microscopes. The fibre tip is fixed in a four‐segmented piezo‐tube by a polymer, Polyisobutylene, which couples the tip stiffly to the piezo at frequencies of 10 kHz or more at room temperature. One segment of the piezo‐tube excites the fibre tip in resonance, while the other three segments detect the tip vibration in the manner of a piezo‐microphone. When the tip is damped by shear forces the induced voltage at the three segments changes and can easily be detected with a lock‐in amplifier. Further our method allows a fast and reproducible tip exchange with minor adjustments of mechanical or electrical components. We demonstrate the performance of our distance control on a holographically fabricated line pattern with 417 nm lattice spacing and 10 nm height. A height resolution of better than 1 nm is demonstrated.

Micromachined aperture probe tip for multifunctional scanning probe microscopy

A novel micromachined aperture tip has been developed for near-field scanning optical microscopy. The advantages of the new probe over commonly used fiber probes are illustrated. The aperture tip is fabricated in a reliable batch process which has the potential for implementation in micromachining processes of scanning probe microscopy sensors and therefore leads to new types of multifunctional probes. For evaluation purposes, the tip was attached to an optical fiber by a microassembly setup and subsequently installed in a near-field scanning optical microscope. First measurements of topographical and optical near-field patterns demonstrate the proper performance of the hybrid probe.

Method to produce high-resolution scanning near-field optical microscope probes by beveling optical fibers

A new two-step method to fabricate scanning near-field optical microscope (SNOM) probes with an aperture size clearly below 100 nm has been developed. For the first step, a chemical etching process is used in which an optical fiber is dipped with its acrylate jacket into hydrofluoric acid to get a suitable tapered shape of the fiber. The second step consists of beveling the etched fiber using a modified micropipette beveler to obtain a tip diameter in the nanometer range as well as a smooth surface to allow a good aluminum metallization by evaporation. By varying the beveling angle tapered shapes with different cone angles can be obtained. First transmission experiments with our probes show an optical resolution below 80 nm. In comparison to fiber tips obtained by a standard heating and pulling method, the transmission efficiency of these tips is up to three orders of magnitude higher due to the optimized tapered shape.

Influence of environmental conditions on shear–force distance control in near-field optical microscopy

In our experiments we show, that a contaminating water film is very important for the shear–force distance control in near-field optical microscopy. This is demonstrated at the transition between a hydrophilic glass surface and a hydrophobic Langmuir–Blodgett film of arachidic acid at different relative humidities. This contaminating water film is one, if not the important reason for the damping of an oscillating fiber during surface approach. It is further shown, that the bulk viscosity of water alone cannot be responsible for the observed damping effect. A thickness dependent viscosity of this water film is proposed. These observations can also explain, why the shear–force distance control works on nearly all surfaces at ambient conditions, but fails to work at very low temperatures.

Influence of protective layers on the blinking of fluorescent single molecules observed by confocal microscopy and scanning near field optical microscopy

Transitions of fluorescent Rhodamine 6G dye molecules into metastable dark states with lifetimes of several seconds were observed by single-molecule detection (SMD) using far-field confocal microscopy. The samples were protected with different organic thin films and were characterized using atomic force microscopy. The data are compared to published models: The best fit is found with a model suggesting that oxygen migration or polarity changes are responsible for the transitions. For further studies with molecules close to each other, we studied the capability of cantilever-SNOM sensors for SMD. Using an α-SNOM we were able to demonstrate 40 nm optical resolution of these new near-field tips for single-molecule fluorescence imaging in direct comparison with confocal microscopy on samples of Rhodamine 6G molecules protected by PMMA.

Piezoelectrical shear-force control on soft biological samples in aqueous solution

In order to apply scanning near-field optical microscopy to life science, it is essential to have an accurate distance feedback that also works on soft biological samples in liquids. In this letter, we report measurements of neuron cells in aqueous solution using an advanced piezoelectrical shear-force detection setup. Simultaneously obtained topographical and fluorescence images are presented, demonstrating a resolution below 100 nm in the optical image. The influence of the water level on the shear-force signal and the interaction between near-field probe and soft organic samples are discussed. Stable feedback in fluids is obtained with tip–sample interaction forces below 100 pN.

Piezoelectrical shear-force distance control in near-field optical microscopy for biological applications.

We present a piezoelectrical shear-force distance control setup for scanning near-field optical microscopy. The setup is compact and tip exchange is easy. The topographical sensitivity is comparable to optical feedback systems. With an acceptable vibration amplitude of 5-10 nm we obtained a topographical resolution of 5 pm/square root of Hz. Because there is no laser necessary for tip position feedback, there is no extraneous light to interfere with spectroscopic and other low-light level experiments. Our technique permits measurements of soft biological samples in aqueous solution, which opens up many possible applications of near-field optical microscopy in biology and medicine.

Shear-force distance control at megahertz frequencies for near-field scanning optical microscopy

We show that the use of fiber overtone resonance modes up to 3 MHz for shear-force distance control has two advantages for near-field microscopy. The higher dither frequency allows a shorter feedback loop time delay, which in turn allows scanning speeds of 100 μm/s on a sample with, for example, a 150 nm height variation over a 1 μm distance. Experiments on a hard semiconductor device and on a soft polymer sample demonstrate a factor of 5 improvement in scanning speed when the dither frequency is increased by a factor of 20. The second advantage is a reduction of the minimum lateral force required for height regulation, which is important for soft samples. Modeling the piezoelectric detection system as a harmonic oscillator indicates a factor of 33 increase in lateral force sensitivity when using the third overtone resonance of a typical fiber tip. This result is confirmed experimentally by immersing the tip into water.

Application of a near-field optical microscope to investigate the fluorescence energy transfer between chromophores embedded in Langmuir-Blodgett films

Scanning near-field optical microscopy (SNOM) was used to investigate the fluorescence energy transfer between a monomolecular film of monomethin oxacyanine and a layer of monomethin thiacyanine in arachidic acid. The donor and acceptor chromophores are fixed in Langmuir-Blodgett (LB) films, spaced by the identical chains of the arachidic acid and dye, respectively. The length of these hydrophobic chains guarantees a fixed distance between the different kinds of chromophores. The dye molecules are oriented parallel to the plane of the LB film. In the LB layer assembly, a step was prepared to separate two different regions. One area contains both kinds of chromphores, whereas in the other area only the donor dyes are present. We used the SNOM technique because of the possibility to measure simultaneously the fluorescence behaviour and topographical structure.