V. N. Lednev

Thermal melting and ablation of silicon by femtosecond laser radiation

The space-time dynamics of thermal melting, subsurface cavitation, spallative ablation, and fragmentation ablation of the silicon surface excited by single IR femtosecond laser pulses is studied by timeresolved optical reflection microscopy. This dynamics is revealed by monitoring picosecond and (sub)nanosecond oscillations of probe pulse reflection, which is modulated by picosecond acoustic reverberations in the dynamically growing surface melt subjected to ablation and having another acoustic impedance, and by optical interference between the probe pulse replicas reflected by the spalled layer surface and the layer retained on the target surface. The acoustic reverberation periods change during the growth and ablation of the surface melt film, which makes it possible to quantitatively estimate the contributions of these processes to the thermal dynamics of the material surface. The results on the thermal dynamics of laser excitation are supported by dynamic measurements of the ablation parameters using noncontact ultrasonic diagnostics, scanning electron microscopy, atomic force microscopy, and optical interference microscopy of the modified regions appearing on the silicon surface after ablation.

Femtosecond laser-induced breakdown spectroscopy

The presented review summarizes nearly two decades of studies on femtosecond laser-induced breakdown spectrometry (fs-LIBS). When an ultra-short (<1 ps) laser pulse is used for ablation, the physics of laser-induced plasma changes dramatically in comparison with ablation by pico or nanosecond pulses. A femtosecond laser pulse interacts only with the electron subsystem, while nanosecond pulses continuously interact with different thermodynamic states of material, starting from solid through liquid into plasma. The properties of ultra-short laser radiation, the timescale of fs-laser ablation and the radiative properties of fs plasma are briefly described. We consider the advantages of fs-LIBS, namely, low ablation thresholds, high-spatial resolution, and rapid analysis of samples, which require minimal invasion and allow high-efficiency transportation of laser radiation in filamentation mode for remote analysis. Moreover, we discussed possible limitations of the technique and different approaches to overcome such constraints while retaining the unique possibilities of fs-LIBS.

Plasma stoichiometry correction method in laser-induced breakdown spectroscopy

The spectra correction approach for the quantitative analysis of alloys by laser-induced breakdown spectroscopy was proposed. A disproportion between the composition of the laser-plasma plume and the bulk sample is explained by the selective evaporation of components during the melting-evaporation stage. The Batanov-Bunkin-Prohorov-Fedorov phenomenon of the transparent wave propagation in a melted metal during the laser ablation was accounted for by the discussed approach. The proposed spectra correction procedure gives good results for the composition measurement of the Al alloy.

Laser beam profile influence on LIBS analytical capabilities: single vs. multimode beam†

Single vs. multimode laser beams have been compared for laser ablation on steel samples. Laser plasma properties and analytical capabilities (precision, limit of detection) were used as key parameters for comparison. Peak fluence at focal spot has been observed to be higher for Gaussian beam despite ∼14-fold lower pulse energy. A comparison of Gaussian and multimode beams with equal energy was carried out in order to estimate influence of beam profile only. Single mode lasing (Gaussian beam) results in better reproducibility of analytical signals compared to multimode lasing while laser energy reproducibility was the same for both cases. Precision improvements were attributed to more stable laser ablation due to better reproducibility of beam profile fluence at laser spot. Plasma temperature and electron density were higher for Gaussian laser beams. Calibration curves were obtained for four elements under study (Cr, Mn, Si, Cu). Two sampling (drilling and scanning procedures) and two optical detection schemes (side-view and optical fiber) were used to compare Gaussian and multimode beam profile influence on analytical capabilities of LIBS. We have found that multimode beam sampling was strongly influenced by surface effects (impurities, defects etc.). For all sampling and detection schemes, better precision was obtained if Gaussian beam was used for sampling. In case of single-spot sampling better limits of detection were achieved for multimode beam. If laser sources have the same wavelength and equal energy then quality of laser beam becomes a crucial parameter which determined laser ablation and analytical capabilities of LIBS.

Single-shot and single-spot measurement of laser ablation threshold for carbon nanotubes

A simple and convenient procedure for single-shot, single-spot ablation threshold measurement has been developed. It is based on the employment of cylindrical lens to obtain elliptical Gaussian laser spot. The ablated spot chords which are parallel to the minor axis were measured across the spot major axis which is proportional to the fluence cross-section thus providing wide range dependence of damaged spot size versus fluence in one spot measurement. For both conventional and new-developed procedures the ablation threshold for typical Nd:YAG laser parameters (1064 nm, 10 ns) has been measured as 50 mJ/cm2 which is one order of magnitude lower than that for a bulk graphite.

Remote sensing of seawater and drifting ice in Svalbard fjords by compact Raman lidar

A compact Raman lidar system for remote sensing of sea and drifting ice was developed at the Wave Research Center at the Prokhorov General Physics Institute of the Russian Academy of Sciences. The developed system is based on a diode-pumped solid-state YVO(4):Nd laser combined with a compact spectrograph equipped with a gated detector. The system exhibits high sensitivity and can be used for mapping or depth profiling of different parameters within many oceanographic problems. Light weight (∼20 kg) and low power consumption (300 W) make it possible to install the device on any vehicle, including unmanned aircraft or submarine systems. The Raman lidar presented was used for study and analysis of the different influence of the open sea and glaciers on water properties in Svalbard fjords. Temperature, phytoplankton, and dissolved organic matter distributions in the seawater were studied in the Ice Fjord, Van Mijen Fjord, and Rinders Fjord. Drifting ice and seawater in the Rinders Fjord were characterized by the Raman spectroscopy and fluorescence. It was found that the Paula Glacier strongly influences the water temperature and chlorophyll distributions in the Van Mijen Fjord and Rinders Fjord. Possible applications of compact lidar systems for express monitoring of seawater in places with high concentrations of floating ice or near cold streams in the Arctic Ocean are discussed.

Preablation electron and lattice dynamics on the silicon surface excited by a femtosecond laser pulse

The study of the time-resolved optical reflection from the silicon surface excited by single femtosecond laser pulses below and near the melting threshold reveals fast (less than 10 ps) Auger recombination of a photogenerated electron–hole plasma with simultaneous energy transfer to the lattice. The acoustic relaxation of the excited surface layer indicates (according to reported data) a characteristic depth of 150 nm of the introduction of the laser radiation energy, which is related to direct linear laser radiation absorption in the photoexcited material due to a decrease in the energy bandgap. The surface temperature, which is probed at a time delay of about 100 ps from the reflection thermomodulation of probe radiation and the integrated continuous thermal emission from the surface, increases with the laser fluence and, thus, favors a nonlinear increase in the fluorescence of sublimated silicon atoms. The surface temperature estimated near the picosecond melting threshold demonstrates a substantial (20%) overheating of the material with respect to the equilibrium melting temperature. Above the melting threshold, the delay of formation of the material melt decreases rapidly (from several tens of picoseconds to several fractions of a picosecond) when the laser fluence and, correspondingly, the surface temperature increase. In the times of acoustic relaxation of the absorbing layer and even later, the time modulation of the optical reflectivity of the material demonstrates acoustic reverberations with an increasing period, which are related to the formation of melt nuclei in the material.

Ice thickness measurements by Raman scattering

A compact Raman LIDAR system with a spectrograph was used for express ice thickness measurements. The difference between the Raman spectra of ice and liquid water is employed to locate the ice-water interface while elastic scattering was used for air--ice surface detection. This approach yields an error of only 2 mm for an 80 mm thick ice sample, indicating that it is a promising express noncontact thickness measurements technique in field experiments.

Femtosecond laser ablation of single-wall carbon nanotube-based material

Single- and multi-shot femtosecond laser surface ablation of a single-wall carbon nanotube-based substrate at 515- and 1030 nm wavelengths was studied by scanning electron microscopy and micro-Raman spectroscopy. The laser ablation proceeds in two ways: as the low-fluence mesoscopic shallow disintegration of the surface nanotube packing, preserving the individual integrity and the semiconducting character of the nanotubes or as the high-fluence deep material removal apparently triggered by the strong intrinsic or impurity-mediated ablation of the individual carbon nanotubes on the substrate surface.

Quantifying Raman OH-band spectra for remote water temperature measurements

Remote water temperature measurements by Raman scattering is a perspective tool for in situ and/or real-time studies for inaccessible areas such as the Arctic region. State-of-the-art laser remote temperature detection techniques are based on temperature-dependent transformation of the Raman OH stretching vibration band. This study compared different approaches quantifying Raman OH-band spectra transformation with temperature: the two-color technique, deconvolution procedure, Raman difference spectroscopy, and centroid technique. Distilled water was probed remotely by compact Raman LIDAR, and the results demonstrated that the Raman OH-band centroid technique achieved the best temperature measurement accuracy (±0.15°C).