Florian Huth

Optical nano-imaging of gate-tunable graphene plasmons

The ability to manipulate optical fields and the energy flow of light is central to modern information and communication technologies, as well as quantum information processing schemes. However, because photons do not possess charge, a way of controlling them efficiently by electrical means has so far proved elusive. A promising way to achieve electric control of light could be through plasmon polaritons—coupled excitations of photons and charge carriers—in graphene. In this two-dimensional sheet of carbon atoms, it is expected that plasmon polaritons and their associated optical fields can readily be tuned electrically by varying the graphene carrier density. Although evidence of optical graphene plasmon resonances has recently been obtained spectroscopically, no experiments so far have directly resolved propagating plasmons in real space. Here we launch and detect propagating optical plasmons in tapered graphene nanostructures using near-field scattering microscopy with infrared excitation light. We provide real-space images of plasmon fields, and find that the extracted plasmon wavelength is very short—more than 40 times smaller than the wavelength of illumination. We exploit this strong optical field confinement to turn a graphene nanostructure into a tunable resonant plasmonic cavity with extremely small mode volume. The cavity resonance is controlled in situ by gating the graphene, and in particular, complete switching on and off of the plasmon modes is demonstrated, thus paving the way towards graphene-based optical transistors. This successful alliance between nanoelectronics and nano-optics enables the development of active subwavelength-scale optics and a plethora of nano-optoelectronic devices and functionalities, such as tunable metamaterials, nanoscale optical processing, and strongly enhanced light–matter interactions for quantum devices and biosensing applications.

Nano-FTIR Absorption Spectroscopy of Molecular Fingerprints at 20 nm Spatial Resolution

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. Nano-FTIR can thus make use of standard infrared databases of molecular vibrations to identify organic materials in ultrasmall quantities and at ultrahigh spatial resolution. As an application example we demonstrate the identification of a nanoscale PDMS contamination on a PMMA sample.

Infrared-spectroscopic nanoimaging with a thermal source

Fourier-transform infrared (FTIR) spectroscopy is a widely used analytical tool for chemical identification of inorganic, organic and biomedical materials, as well as for exploring conduction phenomena. Because of the diffraction limit, however, conventional FTIR cannot be applied for nanoscale imaging. Here we demonstrate a novel FTIR system that allows for infrared-spectroscopic nanoimaging of dielectric properties (nano-FTIR). Based on superfocusing of thermal radiation with an infrared antenna, detection of the scattered light, and strong signal enhancement employing an asymmetric FTIR spectrometer, we improve the spatial resolution of conventional infrared spectroscopy by more than two orders of magnitude. By mapping a semiconductor device, we demonstrate spectroscopic identification of silicon oxides and quantification of the free-carrier concentration in doped Si regions with a spatial resolution better than 100  nm. We envisage nano-FTIR becoming a powerful tool for chemical identification of nanomaterials, as well as for quantitative and contact-free measurement of the local free-carrier concentration and mobility in doped nanostructures.

Structural analysis and mapping of individual protein complexes by infrared nanospectroscopy

Mid-infrared spectroscopy is a widely used tool for material identification and secondary structure analysis in chemistry, biology and biochemistry. However, the diffraction limit prevents nanoscale protein studies. Here we introduce mapping of protein structure with 30 nm lateral resolution and sensitivity to individual protein complexes by Fourier transform infrared nanospectroscopy (nano-FTIR). We present local broadband spectra of one virus, ferritin complexes, purple membranes and insulin aggregates, which can be interpreted in terms of their α-helical and/or β-sheet structure. Applying nano-FTIR for studying insulin fibrils—a model system widely used in neurodegenerative disease research—we find clear evidence that 3-nm-thin amyloid-like fibrils contain a large amount of α-helical structure. This reveals the surprisingly high level of protein organization in the fibril’s periphery, which might explain why fibrils associate. We envision a wide application potential of nano-FTIR, including cellular receptor in vitro mapping and analysis of proteins within quaternary structures.

Plasmonic nickel nanoantennas.

The fundamental optical properties of pure nickel nanostructures are studied by far-field extinction spectroscopy and optical near-field microscopy, providing direct experimental evidence of the existence of particle plasmon resonances predicted by theory. Experimental and calculated near-field maps allow for unambiguous identification of dipolar plasmon modes. By comparing calculated near-field and far-field spectra, dramatic shifts are found between the near-field and far-field plasmon resonances, which are much stronger than in gold nanoantennas. Based on a simple damped harmonic oscillator model to describe plasmonic resonances, it is possible to explain these shifts as due to plasmon damping.

Resonant Antenna Probes for Tip-Enhanced Infrared Near-Field Microscopy

We report the development of infrared-resonant antenna probes for tip-enhanced optical microscopy. We employ focused-ion-beam machining to fabricate high-aspect ratio gold cones, which replace the standard tip of a commercial Si-based atomic force microscopy cantilever. Calculations show large field enhancements at the tip apex due to geometrical antenna resonances in the cones, which can be precisely tuned throughout a broad spectral range from visible to terahertz frequencies by adjusting the cone length. Spectroscopic analysis of these probes by electron energy loss spectroscopy, Fourier transform infrared spectroscopy, and Fourier transform infrared near-field spectroscopy corroborates their functionality as resonant antennas and verifies the broad tunability. By employing the novel probes in a scattering-type near-field microscope and imaging a single tobacco mosaic virus (TMV), we experimentally demonstrate high-performance mid-infrared nanoimaging of molecular absorption. Our probes offer excellent perspectives for optical nanoimaging and nanospectroscopy, pushing the detection and resolution limits in many applications, including nanoscale infrared mapping of organic, molecular, and biological materials, nanocomposites, or nanodevices.

Quantitative Measurement of Local Infrared Absorption and Dielectric Function with Tip-Enhanced Near-Field Microscopy.

Scattering-type scanning near-field optical microscopy (s-SNOM) and Fourier transform infrared nanospectroscopy (nano-FTIR) are emerging tools for nanoscale chemical material identification. Here, we push s-SNOM and nano-FTIR one important step further by enabling them to quantitatively measure local dielectric constants and infrared absorption. Our technique is based on an analytical model, which allows for a simple inversion of the near-field scattering problem. It yields the dielectric permittivity and absorption of samples with 2 orders of magnitude improved spatial resolution compared to far-field measurements and is applicable to a large class of samples including polymers and biological matter. We verify the capabilities by determining the local dielectric permittivity of a PMMA film from nano-FTIR measurements, which is in excellent agreement with far-field ellipsometric data. We further obtain local infrared absorption spectra with unprecedented accuracy in peak position and shape, which is the key to quantitative chemometrics on the nanometer scale.

Near-field imaging and nano-Fourier-transform infrared spectroscopy using broadband synchrotron radiation

We demonstrate scanning near-field optical microscopy with a spatial resolution below 100 nm by using low intensity broadband synchrotron radiation in the IR regime. The use of such a broadband radiation source opens up the possibility to perform nano-Fourier-transform infrared spectroscopy over a wide spectral range.

Enhanced resolution in subsurface near-field optical microscopy

We report an experimental analysis of the capabilities of scattering-type scanning near-field optical microscopy for mapping sub-surface features at varying depths. For the first time, we demonstrate experimentally that both the spatial resolution and depth contrast can be improved in subsurface microscopy by demodulating the measured near-field signal at higher harmonics of the probes tapping frequency and by operating at smaller tapping amplitudes. Our findings are qualitatively supported by a simple dipole model.

Nanoscale Chemical Mapping by Local Infrared Spectroscopy (nano-FTIR)

Research and development of nanomaterials, especially those made of organic molecules, has rapidly increased in the last couple of years. Novel nanomaterials exhibit extraordinary material properties and will have a huge impact on chemical, pharmaceutical, and microelectronic products of the near future.