Publications by authors named "Fritz Keilmann"

Scattering scanning near-field optical microscopy (s-SNOM) is a powerful technique for mid-infrared spectroscopy at nanometer length scales. By investigating objects in aqueous environments through ultrathin membranes, s-SNOM has recently been extended toward label-free nanoscopy of the dynamics of living cells and nanoparticles, assessing both the optical and the mechanical interactions between the tip, the membrane and the liquid suspension underneath. Here, the study reports that the tapping AFM tip induces a reversible nanometric deformation of the membrane manifested as either an indentation or protrusion.

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Photonic metasurfaces offer exceptional control over light at the nanoscale, facilitating applications spanning from biosensing, and nonlinear optics to photocatalysis. Many metasurfaces, especially resonant ones, rely on periodicity for the collective mode to form, which makes them subject to the influences of finite size effects, defects, and edge effects, which have considerable negative impact at the application level. These aspects are especially important for quasi-bound state in the continuum (BIC) metasurfaces, for which the collective mode is highly sensitive to perturbations due to high-quality factors and strong near-field enhancement.

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The preservation of oral health over a person's lifespan is a key factor for a high quality of life. Sustaining oral health requires high-end dental materials with a plethora of attributes such as durability, non-toxicity and ease of application. The combination of different requirements leads to increasing miniaturization and complexity of the material components such as the composite and adhesives, which makes the precise characterization of the material blend challenging.

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Infrared fingerprint spectra can reveal the chemical nature of materials down to 20-nm detail, far below the diffraction limit, when probed by scattering-type scanning near-field optical microscopy (s-SNOM). But this was impossible with living cells or aqueous processes as in corrosion, due to water-related absorption and tip contamination. Here, we demonstrate infrared s-SNOM of water-suspended objects by probing them through a 10-nm thick SiN membrane.

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Polymer brush coatings are effective in preventing blood coagulation or bacterial attachment, but their chain conformation, while vital for this effect, was never characterized in high spatial resolution. Here, we report mid-infrared spectroscopic nanoscopy studies of few-nanometer-thin poly(ethylene oxide) (PEO) films which reveal marked spectral variations along the surface at a length scale smaller than 100 nm and originating only from the physical conformation of the chains. The conformation and average orientation of the polymer chains in the layer is extracted from the spectra with the aid of theoretic modeling, confirming the spontaneous formation of a crystalline phase.

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At terahertz (THz) frequencies, scattering-type scanning near-field optical microscopy (s-SNOM) based on continuous wave sources mostly relies on cryogenic and bulky detectors, which represents a major constraint for its practical application. Here, we devise a THz s-SNOM system that provides both amplitude and phase contrast and achieves nanoscale (60-70nm) in-plane spatial resolution. It features a quantum cascade laser that simultaneously emits THz frequency light and senses the backscattered optical field through a voltage modulation induced inherently through the self-mixing technique.

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We investigated phonon-polaritons in hexagonal boron nitride-a naturally hyperbolic van der Waals material-by means of the scattering-type scanning near-field optical microscopy. Real-space nanoimages we have obtained detail how the polaritons are launched when the light incident on a thin hexagonal boron nitride slab is scattered by various intrinsic and extrinsic inhomogeneities, including sample edges, metallic nanodisks deposited on its top surface, random defects, and surface impurities. The scanned tip of the near-field microscope is itself a polariton launcher whose efficiency proves to be superior to all the other types of polariton launchers we studied.

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A method has been developed to stabilize and transfer nanofilms of functional organic semiconductors. The method is based on crosslinking of their topmost layers by low energy electron irradiation. The films can then be detached from their original substrates and subsequently deposited onto new solid or holey substrates retaining their structural integrity.

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Scattering scanning near-field optical microscopy (s-SNOM) has emerged as a powerful nanoscale spectroscopic tool capable of characterizing individual biomacromolecules and molecular materials. However, applications of scattering-based near-field techniques in the infrared (IR) to native biosystems still await a solution of how to implement the required aqueous environment. In this work, we demonstrate an IR-compatible liquid cell architecture that enables near-field imaging and nanospectroscopy by taking advantage of the unique properties of graphene.

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Advances in the spatial resolution of modern analytical techniques have tremendously augmented the scientific insight gained from the analysis of natural samples. Yet, while techniques for the elemental and structural characterization of samples have achieved sub-nanometre spatial resolution, infrared spectral mapping of geochemical samples at vibrational 'fingerprint' wavelengths has remained restricted to spatial scales >10 μm. Nevertheless, infrared spectroscopy remains an invaluable contactless probe of chemical structure, details of which offer clues to the formation history of minerals.

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We report on time-resolved mid-infrared (mid-IR) near-field spectroscopy of the narrow bandgap semiconductor InAs. The dominant effect we observed pertains to the dynamics of photoexcited carriers and associated surface plasmons. A novel combination of pump-probe techniques and near-field nanospectroscopy accesses high momentum plasmons and demonstrates efficient, subpicosecond photomodulation of the surface plasmon dispersion with subsequent tens of picoseconds decay under ambient conditions.

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Controlling the domain size and degree of crystallization in organic films is highly important for electronic applications such as organic photovoltaics, but suitable nanoscale mapping is very difficult. Here we apply infrared-spectroscopic nano-imaging to directly determine the local crystallinity of organic thin films with 20-nm resolution. We find that state-of-the-art pentacene films (grown on SiO2 at elevated temperature) are structurally not homogeneous but exhibit two interpenetrating phases at sub-micrometre scale, documented by a shifted vibrational resonance.

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Pump-probe spectroscopy is central for exploring ultrafast dynamics of fundamental excitations, collective modes, and energy transfer processes. Typically carried out using conventional diffraction-limited optics, pump-probe experiments inherently average over local chemical, compositional, and electronic inhomogeneities. Here, we circumvent this deficiency and introduce pump-probe infrared spectroscopy with ∼ 20 nm spatial resolution, far below the diffraction limit, which is accomplished using a scattering scanning near-field optical microscope (s-SNOM).

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A recently developed ultra-resolving near-field infrared nanoscope is applied to investigate methyl methacrylate embedded, un-decalcified human bone sections. Results show detail at a resolution of 30 nm. Specific contrasting of mineral components is enabled by choosing an appropriate infrared wavelength, here 9.

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We demonstrate Fourier transform infrared nanospectroscopy (nano-FTIR) based on a scattering-type scanning near-field optical microscope (s-SNOM) equipped with a coherent-continuum infrared light source. We show that the method can straightforwardly determine the infrared absorption spectrum of organic samples with a spatial resolution of 20 nm, corresponding to a probed volume as small as 10 zeptoliter (10(-20) L). Corroborated by theory, the nano-FTIR absorption spectra correlate well with conventional FTIR absorption spectra, as experimentally demonstrated with poly(methyl methacrylate) (PMMA) samples.

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Methods for imaging of nanocomposites based on X-ray, electron, tunneling or force microscopy provide information about the shapes of nanoparticles; however, all of these methods fail on chemical recognition. Neither do they allow local identification of mineral type. We demonstrate that infrared near-field microscopy solves these requirements at 20 nm spatial resolution, highlighting, in its first application to natural nanostructures, the mineral particles in shell and bone.

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We report on infrared (IR) nanoscopy of 2D plasmon excitations of Dirac fermions in graphene. This is achieved by confining mid-IR radiation at the apex of a nanoscale tip: an approach yielding 2 orders of magnitude increase in the value of in-plane component of incident wavevector q compared to free space propagation. At these high wavevectors, the Dirac plasmon is found to dramatically enhance the near-field interaction with mid-IR surface phonons of SiO(2) substrate.

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We demonstrate continuous infrared spectra from 20 nm sample spots, by combining dispersive Fourier-transform infrared spectroscopy (FTIR) with scattering near-field microscopy (s-SNOM). With the "apertureless" tip of a standard AFM cantilever in one arm of a Michelson interferometer the spectra arise simultaneously in amplitude and phase. The effect of near-field phonon resonance of SiC is used to verify background-free s-SNOM operation, and to determine the absolute scattering efficiency, at 6 cm(-1) spectral resolution.

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We introduce a new concept of spectroscopic near-field optical microscopy that records broad infrared spectra at each pixel during scanning. Two coherent beams with harmonic frequency-comb spectra are employed, one for illuminating the scanning tip, the other as reference for multi-heterodyne detection of the scattered light. Our implementation yields 200 cm(-1) wide amplitude and phase spectra centered at 950 cm(-1) (this band can be tuned between 700 and 1400 cm(-1)).

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We demonstrate that scattering near-field microscopy (s-SNOM) can determine infrared "fingerprint" spectra of individual poly(methyl methacrylate) nanobeads and viruses as small as 18 nm. Amplitude and phase spectra are found surprisingly strong, even at a probed volume of only 10(-20) l, and robust in regard to particle size and substrate. This makes infrared spectroscopic s-SNOM a versatile tool for chemical and-in the case of protein-secondary-structure identification.

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We demonstrate real-time recording of chemical vapor fluc-tuations from 22m away with a fast Fourier-transform infrared (FTIR) spectrometer that uses a laser-like infrared probing beam generated from two 10-fs Ti:sapphire lasers. The FTIR's broad 9-12 microm spectrum in the "molecular fingerprint" region is dispersed by fast heterodyne self-scanning, enabling spectra at 2cm-1 resolution to be recorded in 70 micros snapshots. We achieve continuous acquisition at a rate of 950 IR spectra per second by actively manipulating the repetition rate of one laser.

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We describe ultraresolution microscopy far beyond the classical Abbe diffraction limit of one half wavelength (lambda/2), and also beyond the practical limit (ca. lambda/10) of aperture-based scanning near-field optical microscopy (SNOM). The 'apertureless' SNOM discussed here uses light scattering from a sharp tip (hence scattering-type or s-SNOM) and has no lambda-related resolution limit.

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A novel type of Fourier-transform infrared spectrometer (FTIR) is demonstrated. It is based on two Ti:sapphire lasers emitting femtosecond pulse trains with slightly different repetition frequencies. Two mid-infrared beams-derived from those lasers by rectification in GaSe-are superimposed upon a detector to produce purely time-domain interferograms that encode the infrared spectrum.

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A highly promising tool for nanoscale material characterization exploits local optical/infrared light scattering simultaneously with standard atomic force microscopy imaging. Thus, both the topography and the local optical/infrared properties of a sample surface can be mapped at better than 20 nm spatial resolution.

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