Michael J. Nasse

Evidence of nanocrystalline semiconducting graphene monoxide during thermal reduction of graphene oxide in vacuum.

As silicon-based electronics are reaching the nanosize limits of the semiconductor roadmap, carbon-based nanoelectronics has become a rapidly growing field, with great interest in tuning the properties of carbon-based materials. Chemical functionalization is a proposed route, but syntheses of graphene oxide (G-O) produce disordered, nonstoichiometric materials with poor electronic properties. We report synthesis of an ordered, stoichiometric, solid-state carbon oxide that has never been observed in nature and coexists with graphene. Formation of this material, graphene monoxide (GMO), is achieved by annealing multilayered G-O. Our results indicate that the resulting thermally reduced G-O (TRG-O) consists of a two-dimensional nanocrystalline phase segregation: unoxidized graphitic regions are separated from highly oxidized regions of GMO. GMO has a quasi-hexagonal unit cell, an unusually high 1:1 O:C ratio, and a calculated direct band gap of ∼0.9 eV.

3D spectral imaging with synchrotron Fourier transform infrared spectro-microtomography

We report Fourier transform infrared spectro-microtomography, a nondestructive three-dimensional imaging approach that reveals the distribution of distinctive chemical compositions throughout an intact biological or materials sample. The method combines mid-infrared absorption contrast with computed tomographic data acquisition and reconstruction to enhance chemical and morphological localization by determining a complete infrared spectrum for every voxel (millions of spectra determined per sample).

Restoration and Spectral Recovery of Mid-Infrared Chemical Images

Fourier transform infrared (FTIR) microspectroscopy is a powerful technique for label-free chemical imaging that has supplied important chemical information about heterogeneous samples for many problems across a variety of disciplines. State-of-the-art synchrotron based infrared (IR) microspectrometers can yield high-resolution images, but are truly diffraction limited for only a small spectral range. Furthermore, a fundamental trade-off exists between the number of pixels, acquisition time and the signal-to-noise ratio, limiting the applicability of the technique. The recently commissioned infrared synchrotron beamline, infrared environmental imaging (IRENI), overcomes this trade off and delivers 4096-pixel diffraction limited IR images with high signal-to-noise ratio in under a minute. The spatial oversampling for all mid-IR wavelengths makes the IRENI data ideal for spatial image restoration techniques. Here, we measured and fitted wavelength-dependent point-spread-functions (PSFs) at IRENI for a 74× objective between the sample plane and detector. Noise-free wavelength-dependent theoretical PSFs are deconvoluted from images generated from narrow bandwidths (4 cm(-1)) over the entire mid-infrared range (4000-900 cm(-1)). The stack of restored images is used to reconstruct the spectra. Restored images of metallic test samples with features that are 2.5 μm and smaller are clearly improved in comparison to the raw data images for frequencies above 2000 cm(-1). Importantly, these spatial image restoration methods also work for samples with vibrational bands in the recorded mid-IR fingerprint region (900-1800 cm(-1)). Improved signal-to-noise spectra are reconstructed from the restored images as demonstrated for a mixture of spherical polystyrene beads in a polyurethane matrix. Finally, a freshly thawed retina tissue section is used to demonstrate the success of deconvolution achievable with a heterogeneous, irregularly shaped, biologically relevant sample with distinguishing spectroscopic features across the entire mid-IR spectral range.

High-spatial-resolution mapping of superhydrophobic cicada wing surface chemistry using infrared microspectroscopy and infrared imaging at two synchrotron beamlines.

The wings of some insects, such as cicadae, have been reported to possess a number of interesting and unusual qualities such as superhydrophobicity, anisotropic wetting and antibacterial properties. Here, the chemical composition of the wings of the Clanger cicada (Psaltoda claripennis) were characterized using infrared (IR) microspectroscopy. In addition, the data generated from two separate synchrotron IR facilities, the Australian Synchrotron Infrared Microspectroscopy beamline (AS-IRM) and the Synchrotron Radiation Center (SRC), University of Wisconsin-Madison, IRENI beamline, were analysed and compared. Characteristic peaks in the IR spectra of the wings were assigned primarily to aliphatic hydrocarbon and amide functionalities, which were considered to be an indication of the presence of waxy and proteinaceous components, respectively, in good agreement with the literature. Chemical distribution maps showed that, while the protein component was homogeneously distributed, a significant degree of heterogeneity was observed in the distribution of the waxy component, which may contribute to the self-cleaning and aerodynamic properties of the cicada wing. When comparing the data generated from the two beamlines, it was determined that the SRC IRENI beamline was capable of producing higher-spatial-resolution distribution images in a shorter time than was achievable at the AS-IRM beamline, but that spectral noise levels per pixel were considerably lower on the AS-IRM beamline, resulting in more favourable data where the detection of weak absorbances is required. The data generated by the two complementary synchrotron IR methods on the chemical composition of cicada wings will be immensely useful in understanding their unusual properties with a view to reproducing their characteristics in, for example, industry applications.

FLUTE: A versatile linac-based THz source

A new compact versatile linear accelerator named FLUTE is currently being designed at the Karlsruhe Institute of Technology. This paper presents the status of this 42 MeV machine. It will be used to generate strong (several 100 MV/m) ultra-short (~1 ps) THz pulses (up to ~4-25 THz) for photon science experiments, as well as to conduct a variety of accelerator studies. The latter range from comparing different coherent THz radiation generation schemes to compressing electron bunches and studying the electron beam stability. The bunch charge will cover a wide range (~100 pC-3 nC). Later we plan to also produce ultra-short x-ray pulses from the electron bunches, which, for example, could then be combined for THz pump-x-ray probe experiments.

Fast Mapping of Terahertz Bursting Thresholds and Characteristics at Synchrotron Light Sources

Dedicated optics with extremely short electron bunches enable synchrotron light sources to generate intense coherent THz radiation. The high degree of spatial compression in this so-called low-αc optics entails a complex longitudinal dynamics of the electron bunches, which can be probed studying the fluctuations in the emitted terahertz radiation caused by the micro-bunching instability (“bursting”). This article presents a “quasi-instantaneous” method for measuring the bursting characteristics by simultaneously collecting and evaluating the information from all bunches in a multi-bunch fill, reducing the measurement time from hours to seconds. This speed-up allows systematic studies of the bursting characteristics for various accelerator settings within a single fill of the machine, enabling a comprehensive comparison of the measured bursting thresholds with theoretical predictions by the bunched-beam theory. This paper introduces the method and presents first results obtained at the ANKA synchrotron radiation facility.

High-resolution chemical microscopy with multiple bright synchrotron beams

Fourier-transform IR (FTIR) microspectroscopy delivers chemical information without perturbing the sample and without the need for stains, dyes, or labels. It is an important tool in many disciplines, ranging from nanomaterials,1 pharmaceuticals,2 volcanic rocks,3 forensic4 and art conservation,5 to biomedical samples.6–8 Up to now,9 however, the optical resolution of available instruments was limited by fundamental trade-offs between acquisition time, signal-to-noise ratio (SNR), sample coverage, and spatial resolution. In microscopy, both source and detector characteristics are fundamental factors that affect the achievable spatial resolution. Benchtop thermal IR sources, like light bulbs, emit their light in all directions, which makes it impossible to collimate their light efficiently. The result is significant photon loss and effectively fewer photons arriving at the detector. Conventional single-synchrotron beams, on the other hand, can be collimated very efficiently, like lasers, and therefore work very well with confocal-type IR microscopes equipped with a single-element detector. However, even though state-of-the-art for high spatial resolution for many years,10 these systems are very slow and unable to cover larger sample areas, due to their raster-scanning mechanism. To solve this problem, we have now developed, for the first time, an IR imaging system that combines the speed and coverage advantage of wide-field benchtop setups with the high spatial resolution offered by multiple beams of bright synchrotron light.9 We use 12 bright but slightly defocused overlapping synchrotron beams, arranged in a 3 4 matrix, to illuminate a large sample area quasi-homogeneously.9, 11, 12 The sample is then Figure 1. Schematic of the 12-beam synchrotron Fourier transform IR imaging beamline (a) at the Synchrotron Radiation Center. M1–M4 are sets of toroidal, flat, parabolic, and flat mirrors that collect and rearrange the bending magnet radiation. (b) False-color screenshot of the 128 128 pixel focal plane array (FPA) showing the 12 overlapping beams illuminating an area of 50 50 m2 (scale bar 40 m). (c) Visible light photograph of the 4 3 beam matrix at the position indicated by the dashed box in (a). Scale bar 1.5cm.

Estimating and correcting interference fringes in infrared spectra in infrared hyperspectral imaging

Short-term acclimation response of individual cells of Thalassiosira weissflogii was monitored by Synchrotron FTIR imaging over the span of 75 minutes. The cells, collected from batch cultures, were maintained in a constant flow of medium, at an irradiance of 120 μmol m-2 s-1 and at 20 °C. Multiple internal reflections due to the micro fluidic channel were modeled, and showed that fringes are additive sinusoids to the pure absorption of the other components of the system. Preprocessing of the hyperspectral cube (x, y, Abs(λ)) included removing spectral fringe using an EMSC approach. Principal component analysis of the time series of hyperspectral cubes showed macromolecular pool variations (carbohydrates, lipids and DNA/RNA) of less than 2% after fringe correction.

An ultra-fast linear array detector for MHz line repetition rate spectroscopy

We developed a fast linear array detector to improve the acquisition rate and the resolution of Electro-Optical Spectral Decoding (EOSD) experimental setups currently installed at several light sources. The system consists of a detector board, an FPGA readout board and a high-throughput data link. InGaAs or Si sensors are used to detect near-infrared (NIR) or visible light. The data acquisition, the operation of the detector board and its synchronization with synchrotron machines are handled by the FPGA. The readout architecture is based on a high-throughput PCI-Express data link. In this paper we describe the system and we present preliminary measurements taken at the ANKA storage ring. A line-rate of 2.7 Mlps (lines per second) has been demonstrated.