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In this work, we present a compact laser-produced plasma source of X-rays, developed and characterized for application in soft X-ray contact microscopy (SXCM). The source is based on a double stream gas puff target, irradiated with a commercially available Nd:YAG laser, delivering pulses with energy up to 740 mJ and 4 ns pulse duration at 10 Hz repetition rate. The target is formed by pulsed injection of a stream of high-Z gas (argon) into a cloud of low Z-gas (helium) by using an electromagnetic valve with a double nozzle setup. The source is designed to irradiate specimens, both in vacuum and in helium atmosphere with nanosecond pulses of soft X-rays in the ‘‘water-window” spectral range. The source is capable of delivering a photon fluence of about 1.09 x 10³ photon/µm²/pulse at a sample placed in vacuum at a distance of about 20 mm downstream the source. It can also deliver a photon fluence of about 9.31 x 10² - photons/µm²/pulse at a sample placed in a helium atmosphere at the same position. The source design and results of the characterization measurements as well as the optimization of the source are presented and discussed. The source was successfully applied in the preliminary experiments on soft X-ray contact microscopy and images of microstructures and biological specimens with ~80 nm half-pitch spatial resolution, obtained in helium atmosphere, are presented.

Significant questions remain in respect to cellulose’s structure and polymorphs, particularly the cellulose surface layers and the bulk crystalline core as well as the conformational differences. Total Internal Reflection Sum Frequency Generation Vibrational Spectroscopy (TIR-SFG-VS) combined with conventional SFG-VS (non-TIR) enables selectively characterizing the molecular structures of surface layers and the crystalline core of cellulose, revealing their differences for the first time. From the SFG spectra in the C-H and O-H regions, we found that the surface layers of Avicel are essentially amorphous while the surface layers of Iβ cellulose are crystalline but with different structural and spectroscopic signatures compared with its crystalline core. The differences between hydrogen bonding networks of cellulose surface and crystalline core were also shown by the SFG signal. The discovery here represents yet another instance of the importance of spectroscopic observations in transformative advances to understand the structure of the cellulosic biomass.

Solar cells that operate efficiently under indoor lighting are of great practical interest as they can serve as electric power sources for portable electronics and devices for wireless sensor networks or the Internet of Things. Here, we demonstrate a dye-sensitized solar cell (DSC) that achieves very high power-conversion efficiencies (PCEs) under ambient light conditions. Our photosystem combines two judiciously designed sensitizers, coded D35 and XY1, with the copper complex Cu(II/I)(tmby) as a redox shuttle (tmby, 4,4′,6,6′-tetramethyl-2,2′-bipyridine), and features a high open-circuit photovoltage of 1.1 V. The DSC achieves an external quantum efficiency for photocurrent generation that exceeds 90% across the whole visible domain from 400 to 650 nm, and achieves power outputs of 15.6 and 88.5 μW cm^–2 at 200 and 1,000 lux, respectively, under illumination from a model Osram 930 warm-white fluorescent light tube. This translates into a PCE of 28.9%.

Here we present the excited state dynamics of jet-cooled 6-thioguanine (6-TG), using resonance-enhanced multiphoton ionization (REMPI), IR–UV double resonance spectroscopy, and pump–probe spectroscopy in the nanosecond and picosecond time domains. We report data on two thiol tautomers, which appear to have different excited state dynamics. These decay to a dark state, possibly a triplet state, with rates depending on tautomer form and on excitation wavelength, with the fastest rate on the order of 10¹⁰ s^–1. We also compare 6-TG with 9-enolguanine, for which we observed decay to a dark state with a 2 orders of magnitude smaller rate. At increased excitation energy (∼+500 cm^–1) an additional pathway appears for the predominant thiol tautomer. Moreover, the excited state dynamics for 6-TG thiols is different from that recently predicted for thiones.

We present resonant two-photon ionization (R2PI) spectra of isocytosine (isoC) and pump–probe results on two of its tautomers. IsoC is one of a handful of alternative bases that have been proposed in scenarios of prebiotic chemistry. It is structurally similar to both cytosine (C) and guanine (G). We compare the excited-state dynamics with the Watson–Crick (WC) C and G tautomeric forms. These results suggest that the excited-state dynamics of WC form of G may primarily depend on the heterocyclic substructure of the pyrimidine moiety, which is chemically identical to isoC. For WC isoC we find a single excited-state decay with a rate of ∼10¹⁰ s^–1, while the enol form has multiple decay rates, the fastest of which is 7 times slower than for WC isoC. The excited-state dynamics of isoC exhibits striking similarities with that of G, more so than with the photodynamics of C.

Recently the quantum dots (QDs) synthesis from single source precursors (SSPs) showed a potential interest for patterning formation of nano-composites. In this approach the SSPs have to be mixed with a matrix that afterwards is treated selectively to obtain the desired nanocomposite. The study of the generation of the QDs from the SSPs is, therefore, crucial for the definition of its behaviour within the polymeric matrix. The formation of the CdS QDs via thermolysis of the cadmium diethyldithiocarbamate (CdDDTC) was performed and studied in the presence of a non coordinating solvent such as octadecene (ODE) in presence of myristic acid (MA) as ligand. The precursor is then studied in combination with the poly(methyl methacrylate) (PMMA) polymer for the generation of the CdS QDs under the laser irradiation within a film. The effect of the laser has been studied both on neat PMMA and on the polymer/precursor blend film with the aid of the fluorescence microscope. The results are used to identify the optimal laser parameters to obtain the decomposition of the precursor and to evaluate the effect of the laser irradiation on the polymer.

Pulsed laser melting in liquid (PLML) has emerged as a facile approach to synthesize submicron spheres (SMSs) for various applications. Typically lasers with long pulse durations in the nanosecond regime are used. However, recent findings show that during melting the energy absorbed by the particle will be dissipated promptly after laser-matter interaction following the temperature decrease within tens of nanoseconds and hence limiting the efficiency of longer pulse widths. Here, the feasibility to utilize a picosecond laser to synthesize Ge SMSs (200~1000 nm in diameter) is demonstrated by irradiating polydisperse Ge powders in water and isopropanol. Through analyzing the educt size dependent SMSs formation mechanism, we find that Ge powders (200~1000 nm) are directly transformed into SMSs during PLML via reshaping, while comparatively larger powders (1000~2000 nm) are split into daughter SMSs via liquid droplet bisection. Furthermore, the contribution of powders larger than 2000 nm and smaller than 200 nm to form SMSs is discussed. This work shows that compared to nanosecond lasers, picosecond lasers are also suitable to produce SMSs if the pulse duration is longer than the material electron-phonon coupling period to allow thermal relaxation.

We report a target-enclosing, hybrid tomograph with a total of 768 elements based on capacitive micromachined ultrasound transducer technology and providing fast, high-resolution 2-D/3-D photoacoustic and ultrasound tomography tailored to finger imaging.A freely programmable ultrasound beamforming platform sampling data at 80 MHz was developed to realize plane wave transmission under multiple angles. A multiplexing unit enables the connection and control of a large number of elements. Fast image reconstruction is provided by GPU processing. The tomograph is composed of four independent and fully automated movable arc-shaped transducers, allowing imaging of all three finger joints. The system benefits from photoacoustics, yielding high optical contrast and enabling visualization of finger vascularization, and ultrasound provides morphologic information on joints and surrounding tissue. A diode-pumped, Q-switched Nd:YAG laser and an optical parametric oscillator are used to broaden the spectrum of emitted wavelengths to provide multispectral imaging. Custom-made optical fiber bundles enable illumination of the region of interest in the plane of acoustic detection. Precision in positioning of the probe in motion is ensured by use of a motor-driven guide slide. The current position of the probe is encoded by the stage and used to relate ultrasound and photoacoustic signals to the corresponding region of interest of the suspicious finger joint. The system is characterized in phantoms and a healthy human finger in vivo. The results obtained promise to provide new opportunities in finger diagnostics and establish photoacoustic/ultrasoundtomography in medical routine.

Biomedical imaging used for medical diagnosis constantly requires improvement in the characteristics for imaging devices. The sensing devices are one of the most important pieces to improve in order to get images with better quality. In this thesis, it is proposed the use of interferometric fiber-optic sensors (which offer the advantages inherent to optical fibers) as devices to detect pressure/acoustic signals generated by the photoacoustic effect. It is explored the capability of using fiber-optic interferometric hydrophones in order to determine the thickness of a material derived from the acoustic signal generated when a sample is illuminated. In addition, the analysis of photoacoustic signals generated by the excitation of nanoparticles of an anisotropic material as absorption centers. Finally, the cross-section of a metallic sample was photoacoustically imaged by acquiring the pressure signals generated.

Photoacoustic imaging has emerged as a promising technique to improve preclinical and clinical imaging by providing users with label-free optical contrast of tissue. Here, we present a proof-of-concept study for noninvasive in vivo murine lipid imaging using 1210 nm light to investigate differences in periaortic fat among mice of different gender, genotypes, and maturation. Acquired lipid signals suggest that adult male apoE^−/− mice have greater periaortic fat accumulation compared to adolescent males, apoE^−/− females, and wild-type mice. These results demonstrate the potential of photoacoustic tomography for studying vascular pathophysiology and improving the diagnosis of lipid-based diseases.