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High-throughput laser micro-machining demands precise control of the laser beam position to achieve optimal efficiency, but existing methods can be both time-consuming and cost-prohibitive. In this paper, we demonstrate a new high-throughput micro-machining technique based on rapidly scanning the laser focal point along the optical axis using an acoustically driven variable focal length lens. Our results show that this scanning method enables higher machining rates over a range of defocus distances and that the effect becomes more significant as the laser energy is increased. In a specific example of silicon, we achieve a nearly threefold increase in the machining rate, while maintaining sharp side walls and a small spot size. This method has great potential for improving the micro-machining efficiency of conventional systems and also opens the door to applying laser machining to workpieces with uneven topography that have been traditionally difficult to process.

Long-lived excitons formed upon visible light absorption play an essential role in photovoltaics, photocatalysis, and even in high-density information storage. Here, we describe a self-assembled two-dimensional metal-organic crystal, composed of graphene-supported macrocycles, each hosting a single FeN₄ center, where a single carbon monoxide molecule can adsorb. In this heme-like biomimetic model system, excitons are generated by visible laser light upon a spin transition associated with the layer 2D crystallinity, and are simultaneously detected via the carbon monoxide ligand stretching mode at room temperature and near-ambient pressure. The proposed mechanism is supported by the results of infrared and time-resolved pump-probe spectroscopies, and by ab initio theoretical methods, opening a path towards the handling of exciton dynamics on 2D biomimetic crystals.

Molecular scale information about the structure of surfactants at interfaces underlies their application in consumer products. In this study the non-linear optical technique of Sum Frequency Generation (SFG) vibrational spectroscopy has been used to investigate the structure and temporal behaviour of two cationic surfactants used frequently in hair conditioners. SFG spectra of films of behenyltrimethylammonium methosulfate (BTMS) and behenyltrimethylammonium chloride (BTAC) were recorded at the air/water interface and on glass slides following Langmuir Blodgett (LB) deposition. The assignment of the BTMS and BTAC spectral features (resonances) to the C---H stretching modes of the surfactants was consolidated by comparison with the SFG spectrum of deuterated cetyltrimethylammonium bromide (d-CTAB) and by recording spectra on D₂O as well as on water. The C---H resonances arise from the methylene and methyl groups of the tail and head-groups of the surfactants. A slow collapse mechanism was observed following film compression of both BTAC and BTMS. The change in molecular structure of the films undergoing this slow collapse was followed by recording sequential SFG spectra in the C---H region, and by monitoring the SFG intensity at specific wavenumbers over time. Additionally, LB deposition onto glass was used to capture the state of the film during the slow collapse, and these SFG spectra showed close similarity to the corresponding spectra on water. Complementary Atomic Force Microscopy (AFM) was used to elucidate the layering of the compressed and relaxed films deposited onto mica by LB deposition.

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.

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.

The laser oxidation of thin metallic films followed by its selective chemical etching is a promising method for the formation of binary metal structures on the glass substrates. It is important to confirm that even a single ultrashort laser pulse irradiation is able to create the protective oxide layer that makes possible to imprint the thermochemical image.

Results of the thermo-chemical treatment of thin chromium films irradiated by picosecond laser pulse utilizing two and four beam interference combined with the chemical etching are presented. The spatial resolution of this method can be high enough due to thermo-chemical sharpening and can be close to the diffraction limit. Micro-Raman spectroscopy was applied for characterization of the chemical composition of the protective oxide layers formed under atmospheric conditions on the surface of thin chromium films.

Quantitative concentrations measurements using time-resolved laser-induced fluorescence have been demonstrated for nitric oxide (NO) in flame. Fluorescence lifetimes measured using a picosecond Nd:YAG laser and optical parametric amplifier system have been used to directly compensate the measured signal for collisional quenching and evaluate NO concentration. The full evaluation also includes the spectral overlap between the ∼15 cm⁻¹ broad laser pulse and multiple NO absorption lines as well as the populations of the probed energy levels. Effective fluorescence lifetimes of 1.2 and 1.5 ns were measured in prepared NO/N₂/O₂ mixtures at ambient pressure and temperature and in a premixed NH₃-seeded CH₄/N₂/O₂ flame, respectively. Concentrations evaluated from measurements in NO/N₂/O₂ mixtures with NO concentrations of 100–600 ppm were in agreement with set values within 3% at higher concentrations. An accuracy of 13% was estimated by analysis of experimental uncertainties. An NO profile measured in the flame showed concentrations of ∼1000 ppm in the post-flame region and is in good agreement with NO concentrations predicted by a chemical mechanism for NH₃ combustion. An accuracy of 16% was estimated for the flame measurements. The direct concentration evaluation from time-resolved fluorescence allows for quantitative measurements in flames where the composition of major species and their collisional quenching on the probed species is unknown. In particular, this is valid for non-stationary turbulent combustion and implementation of the presented approach for measurements under such conditions is discussed.

The lipopeptide surfactin produced by certain strains of Bacillus subtilis is a powerful biosurfactant possessing potentially useful antimicrobial properties. In order to better understand its surface behavior, we have used surface sensitive sum frequency generation (SFG) vibrational spectroscopy in the C—H and C═O stretching regions to determine its structure at the air/water interface. Using surfactin with the leucine groups of the peptide ring perdeuterated, we have shown that a majority of the SFG signals arise from the 4 leucine residues. We find that surfactin forms a robust film, and that its structure is not affected by the number density at the interface or by pH variation of the subphase. The spectra show that the ring of the molecule lies in the plane of the surface rather than perpendicular to it, with the tail lying above this, also in the plane of the interface.

In this chapter, we present a number of sensitive measurement modalities for the study and analysis of human cancer-affected colon and gastric tissue using terahertz (THz) spectroscopy. Considerable advancements have been reached in characterization of bio-tissue with some accuracy, although too dawn, and still long and exhaustive work have to be done towards well-established and reliable applications. The advent of the THz-time-domain spectroscopy (THz-TDS) test modality at a sub-picosecond time resolution has arguably fostered an intensive work in this field’s research line. The chapter addresses some basic theoretical aspects of this measurement modality with the presentation of general experimental laboratory setup diagrams for THz generation and detection, sample preparation aspects, samples optical parameters calculation procedures and data analysis.