Jean-Blaise Brubach

Performance of the AILES THz‐Infrared beamline at SOLEIL for High resolution spectroscopy

The new THz beamline (AILES) located at the third generation Synchrotron Radiation source SOLEIL is now operating for applications in a wide variety of research themes. In particular, this source with its adapted optics allows high resolution spectroscopic measurements of molecules in the entire infrared and THz range. This presentation focuses on the performances concerning flux, spectral range and stability for molecular spectroscopy. Thanks to these performances, the coupling of synchrotron radiation from a highly stable third generation source with high resolution FTIR spectrometer and with a long path cell (150 m or more) can be particularly advantageous. This fact is related to the optics of the beamline permitting the entire source to be used without aperture stop (entrance iris), even for measurements at highest‐resolution of ∼0.1 μeV (10−3 cm−1).

Observing microscopic structures of a relativistic object using a time-stretch strategy

Emission of light by a single electron moving on a curved trajectory (synchrotron radiation) is one of the most well-known fundamental radiation phenomena. However experimental situations are more complex as they involve many electrons, each being exposed to the radiation of its neighbors. This interaction has dramatic consequences, one of the most spectacular being the spontaneous formation of spatial structures inside electrons bunches. This fundamental effect is actively studied as it represents one of the most fundamental limitations in electron accelerators, and at the same time a source of intense terahertz radiation (Coherent Synchrotron Radiation, or CSR). Here we demonstrate the possibility to directly observe the electron bunch microstructures with subpicosecond resolution, in a storage ring accelerator. The principle is to monitor the terahertz pulses emitted by the structures, using a strategy from photonics, time-stretch, consisting in slowing-down the phenomena before recording. This opens the way to unpreceeded possibilities for analyzing and mastering new generation high power coherent synchrotron sources.

Coherent synchrotron radiation for broadband terahertz spectroscopy

We present the first high resolution (10(-3) cm(-1)) interferometric measurements in the 200-750 GHz range using coherent synchrotron radiation, achieved with a low momentum compaction factor. The effect of microbunching on spectra is shown, depending on the bunch current. A high signal-to-noise ratio is reached thanks to an artifact correction system based on a double detection scheme. Combined to the broad emitted spectral range and high flux (up to 10(5) times the incoherent radiation), this study demonstrates that coherent synchrotron radiation can now be used for stability-demanding applications, such as gas-phase studies of unstable molecules.

Infrared near-field imaging and spectroscopy based on thermal or synchrotron radiation

We demonstrate the coupling of a scattering near-field scanning optical microscope combined with a Fourier transform infrared spectrometer. The set-up operates using either the near-field thermal emission from the sample itself, which is proportional to the electromagnetic local density of states, or with an external infrared synchrotron source, which is broadband and highly brilliant. We perform imaging and spectroscopy measurements with sub-wavelength spatial resolution in the mid-infrared range on surfaces made of silicon carbide and gold and demonstrate the capabilities of the two configurations for super-resolved near-field mid-infrared hyperspectral imaging and that the simple use of a properly chosen bandpass filter on the detector allows one to image the spatial distribution of materials with sub-wavelength resolution by studying the contrast in the near-field images.

Differential Scanning Calorimetry Study of the Structure of Water Confined within AOT Lamellar Mesophases

We combined thermal analysis with FT-IR measurements to solve the structure of the water network confined within lamellar bilayers of AOT surfactant. Unlike previous FT-IR analyses that allowed us only to point out spectroscopic molecular components characterized by their local connectivity, differential scanning calorimetry (DSC) allowed us to identify homogeneous thermal populations listed as low, medium and high temperature. HT water was identified with bulk water, and LT water, as hydration water closely linked with surfactants heads. MT water was assigned to a disrupted network of water corresponding to a layer of 0.5 nm modified by the effect of confinement created by the vicinity of the surfactant bilayer. It appears from this study that the actual extent of confinement influence is lower than expected, at least for lamellar structures. Each thermal population was finally described by a different distribution of the spectroscopic components identified in parallel by FT-IR.

Improved mid infrared detector for high spectral or spatial resolution and synchrotron radiation use

When using bright, small effective size sources, such as synchrotron radiation light beam, for broadband spectroscopy at spectral or spatial high resolution for mid-IR FTIR measurements, a marked detectivity improvement can be achieved by setting up a device matching the detector optical étendue to that of the source. Further improvement can be achieved by reducing the background unmodulated flux and other intrinsic noise sources using a lower temperature cryogen, such as liquid helium. By the combined use of cooled apertures, cold reimaging optics, filters and adapted detector polarization, and preamplification electronics, the sensitivity of a HgCdTe photoconductive IR detector can be improved by a significant factor with respect to standard commercial devices (more than one order of magnitude on average over 6-20 μm region) and the usable spectral range extended to longer wavelengths. The performances of such an optimized detector developed on the AILES Beamline at SOLEIL are presented here.

Electrochemically Induced Far-Infrared Difference Spectroscopy on Metalloproteins Using Advanced Synchrotron Technology

New information on a proteins structure, intra- and intermolecular hydrogen bonds, or metal-ligand bond properties can be unraveled in the far-infrared (far-IR)-terahertz-domain (600-3 cm(-1) or 18-0.1 THz). In this study, we compare the performances of thermal sources with synchrotron far-IR to record reaction-induced Fourier transform infrared (FT-IR) difference signals with proteins in solution. Using the model protein Cu-azurin placed in a short path length electrochemical cell adapted for transmission spectroscopy in vacuum-purged optics, we show that minute spectral shifts induced by metal isotope labeling or temperature changes are detected using the far-IR beamline AILES of the synchrotron SOLEIL. On one hand, these data allow us to identify modes involving Cu-ligand vibrations and pave the way for the analysis of metal sites or metal redox states of proteins not amenable to resonance Raman spectroscopy. On another hand, small band shifts or changes in band intensity upon temperature modifications show that far-IR difference spectroscopy allows one to extract from a complex background hydrogen-bonding signatures directly relevant to the protein function. For Cu-azurin, a temperature-sensitive IR mode involving Cu(II)-His vibrations points to the role of a hydrogen bond between a Cu histidine ligand and the water solvent in tuning the Cu(II)-histidine bond properties. Furthermore, these experimental data support the possible role of a His117-water interaction in electron-transfer activity of Cu-azurin proposed by theoretical studies.

Optical investigation of the thermoelectric topological crystalline insulatorPb0.77Sn0.23Se

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Competing coexisting phases in 2D water

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Insulator–metal transition of VO2 ultrathin films on silicon: evidence for an electronic origin by infrared spectroscopy

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