High-vacuum time-resolved laser-induced incandescence of flame-generated soot

We have measured time-resolved laser-induced incandescence of flame-generated soot under high-vacuum conditions (4.1×10⁻⁶ mbar) at an excitation wavelength of 532 nm with laser fluences spanning 0.06–0.5 J/cm². We generated soot in an ethylene/air diffusion flame, introduced it into the vacuum system with an aerodynamic lens, heated it using a pulsed laser with a spatially homogeneous and temporally smooth laser profile, and recorded LII temporal profiles at 685 nm. At low laser fluences LII signal decay rates are slow, and LII signals persist beyond the residence time of the soot particles in the detection region. At these fluences, the temporal maximum of the LII signal increases nearly linearly with increasing laser fluence until reaching a plateau at ∼0.18 J/cm². At higher fluences, the LII signal maximum is independent of laser fluence within experimental uncertainty. At these fluences, the LII signal decays rapidly during the laser pulse. The fluence dependence of the vacuum LII signal is qualitatively similar to that observed under similar laser conditions in an atmospheric flame but requires higher fluences (by ∼0.03 J/cm²) for initiation. These data demonstrate the feasibility of recording vacuum LII temporal profiles of flame-generated soot under well-characterized conditions for model validation.     

Filming the invisible – time-resolved visualization of compressible flows

Essentially all processes in gasdynamics are invisible to the naked eye as they occur in a transparent medium. The task to observe them is further complicated by the fact that most of these processes are also transient, often with characteristic times that are considerably below the threshold of human perception. Both difficulties can be overcome by combining visualization methods that reveal changes in the transparent medium, and high-speed photography techniques that “stop” the motion of the flow. The traditional approach is to reconstruct a transient process from a series of single images, each taken in a different experiment at a different instant. This approach, which is still widely used today, can only be expected to give reliable results when the process is reproducible. Truly time-resolved visualization, which yields a sequence of flow images in a single experiment, has been attempted for more than a century, but many of the developed camera systems were characterized by a high level of complexity and limited quality of the results. Recent advances in digital high-speed photography have changed this situation and have provided the tools to investigate, with relative ease and in sufficient detail, the true development of a transient flow with characteristic time scales down to one microsecond. This paper discusses the potential and the limitations one encounters when using density-sensitive visualization techniques in time-resolved mode. Several examples illustrate how this approach can reveal and explain a number of previously undetected phenomena in a variety of highly transient compressible flows. It is demonstrated that time-resolved visualization offers numerous advantages which normally outweigh its shortcomings, mainly the often-encountered loss in resolution. Apart from the capability to track the location and/or shape of flow features in space and time, adequate time-resolved visualization allows one to observe the development of deliberately introduced near-isentropic perturbation wavelets. This new diagnostic tool can be used to qualitatively and quantitatively determine otherwise inaccessible thermodynamic properties of a compressible flow.     

Molecular dynamics simulations of laser-induced damage of nanostructures and solids

A theoretical approach to treat laser induced femtosecond structural changes in covalently bonded nanostructures and solids is described. Our approach consists in molecular dynamic simulations performed on the basis of time-dependent, many-body potential energy surfaces derived from tight-binding Hamiltonians. The shape and spectral composition of the laser pulse is explicitly taking into account in a non-perturbative way. We show a few examples of the application of this approach to describe the laser damage and healing of defects in carbon nanotubes with different chiralities and the ultrafast nonequilibrium melting of bulk germanium, initiated by the laser-induced softening and destabilization of transversal acoustic phonon modes.     

Pressure and composition dependences of acetone laser-induced fluorescence with excitation at 248, 266, and 308 nm

In previous studies, acetone has been successfully applied as a tracer for planar laser-induced fluorescence (PLIF) measurements of concentration and temperature. The desire to extend acetone PLIF capability to conditions of varying pressure and composition has motivated studies of the effects of these quantities on fluorescence yield. The present work explores pressure and composition effects over a 0.5 to 16 atm range for the three excitation wavelengths of greatest interest for diagnostics: 248, 266, and 308 nm. In accord with previous studies, fluorescence per acetone molecule is seen to increase with pressure, apparently towards a high-pressure limit for each wavelength, with the most significant effect observed at short wavelengths. Bath gas composition is also seen to affect fluorescence intensity, with an impact related to the effectiveness of the bath gas species at vibrationally relaxing excited acetone. A model of fluorescence yield considering the relative rates of intersystem crossing and vibrational relaxation for excited singlet acetone describes the measured pressure and composition dependences well. To explain an oxygen fluorescence quenching effect that is observed experimentally, a term is added to the model to represent oxygen-assisted intersystem crossing. The data and model results provide useful guidance for diagnostic applications. A key conclusion is that long excitation wavelengths are preferable from the standpoint of minimizing pressure and composition dependences. Received: 17 December 1998 / Revised version: 21 May 1999 / Published online: 30 July 1999     

An imaging approach for a contactless monitoring of the conservation state of metallic works of art

An easy-to-use and cheap diagnostic tool based on digital photography and 2D-FFT imaging processing is described that can be used to monitor the corrosion process occurring over time on the surface of metallic works of art in indoor and outdoor environments and to assess the stability of the materials employed for restoration. The proposed solution has the advantage of not requiring standard lighting and artifacts manipulation, that are not easily achievable in real applications. The imaging algorithm is capable of highlighting the changes in the surface uniformity due to the corrosion process and can be used to put in evidence the beginning of dangerous localized corrosion phenomena onto the metallic surface. Although this technique does not allow a quantitative measurement of the corrosion rate, it has proved to be an effective approach to assess the stability of protective coatings. The proposed processing has been tested in laboratory to asses the stability of SiO₂—like protective coatings deposited by PECVD on a set of silver reference alloys submitted to a tarnishing test in the presence of H₂S vapors.     

Polymer pixel enhancement by laser-induced forward transfer for sensor applications

This paper presents polymer pixel printing for applications in chemoselective sensors where nanosecond laser direct transfer methods, with a triazene polymer (TP) acting as a Dynamic Release Layer (DRL), are used. A systematic study of laser fluence, donor film morphology and both single- and multiple-pixel deposition were optimized with the final goal to obtain continuous pixels of sensitive polymers, polyethylenimine (PEI) and polyisobutylene (PIB), on SAW surfaces. Morphology characterization after the laser transfer has been performed by Optical Microscopy and Scanning Electron Microscopy (SEM). The responses of the coated transducers were measured after deposition with different laser fluences and it was found that a fluence under 625 mJ/cm² was required in order to prevent damage of the interdigital transducers (IDT) of the sensor devices. The sensitivity of the polymer coated devices to acetone concentrations gives an indication that LIFT can be used for printing sensitive polymer pixels onto transducer devices.     

Continuous 100 Hz planar laser-induced fluorescence applied to the study of combustion processes

In this paper, a 100?Hz planar laser-induced fluorescence system based on the off-shelf commercial laser and self-made intensified camera is presented, which is low cost and maintainable to be applied in practical combustion research. By using this device, 100?Hz continuously planar laser-induces fluorescence laser combustion diagnostics was conducted. To evaluate this device, both laboratorial combustors and a scramjet combustor were studied. In these experiments, the structure of flame and expansion and the oscillation process of combustion can be resolved.     

Raman spectroscopic study of femtosecond laser-induced phase transformation associated with ripple formation on single-crystal SiC

Raman spectroscopy was performed to investigate microscopic structural changes associated with a ripple structure formation initiated by femtosecond laser irradiation on the surface of single-crystal silicon carbide. The amorphous phases of silicon carbide, silicon, and carbon were observed. The intensity ratio between amorphous silicon carbide and silicon changed discretely at the boundary between fine and coarse ripples. The physical processes responsible for the formation of the ripple structure are discussed.     

Sensitivity of laser-induced upconversion fluorescence dynamics to exciting wavelength in Er<Superscript>3+</Superscript>-doped YAG

A novel sensitivity of laser-induced upconversion (UC) fluorescence dynamics to the exciting wavelength in Er³⁺:YAG crystal has been observed. The sensitivities to exciting wavelength variations are only 0.02 and 0.06 nm for ² G _9/2 and ² P _3/2 UC luminescence, respectively. The observation of this sensitivity reveals that when a certain level is populated by more than one UC mechanisms, a precise determination of suitable exciting wavelength is crucial because the competition between different UC mechanisms has a sensitive variation with exciting wavelength in near-resonant range.     

Investigation of the A2Σ- state of CuO by laser-induced fluorescence

The laser-induced fluorescence excitation spectrum of the A²Σ^－X²Π_3/2 transition of CuO in the 540－620nm region has been studied, where the CuO molecule was produced by using the technique of dc discharge reaction under a supersonic condition. We have recorded and rotationally analysed the 0－0, 1－0, 2－0 and 3－0 bands. The rotational constants of the upper state A²Σ^- were determined and vibrational constants improved. In addition, the lifetime measurement for the A²Σ^- state was carried out under the collision-free condition, and the lifetimes obtained are 469±2, 456±2, 488±3 and 490±4ns for v'=0, v'=1, v'=2 and v'=3 levels, respectively.     

Spectroscopic analysis of a laser-induced NaCl–water plasma. The influence of self-absorption

A spectroscopic study of the plasma plume created by a laser beam on the surface of NaCl aqueous solution is presented. Optical emission spectra are recorded and temporally analyzed; electron number density is determined from the Stark broadening of the NI nitrogen line, and temperature is obtained from relative intensity of OI oxygen lines. The intensity of an atomic line from sodium was used to quantitate its molar percentage in the Oceanic and Mediterranean sea, and calibration curves have been constructed for concentrations ranging up to 1.5%.     

The laser-induced fluorescence study of AΣ-XΠi band system of CuS

The laser-induced fluorescence excitation spectra of jet-cooled CuS molecules have been recorded in the energy range of 17 200-19 500 cm⁻¹. Fourteen observed vibronic bands have been assigned as three transition progressions: A²Σ⁻ (v′ = 0-4)-X²Π_3/2 (v″ = 0), A²Σ⁻ (v′ = 0-4)-X²Π_3/2 (v″ = 1), and A²Σ⁻ (v′ = 0-3)-X²Π_1/2 (v″ = 0). Spectroscopic constants of both the X²Π ground state and the A²Σ⁻ excited state of ⁶³CuS and ⁶⁵CuS were determined by analyzing their rotationally resolved spectra. Furthermore, the lifetimes of most observed bands were measured for the first time.     

In situ observation of cell-detachment process initiated by femtosecond laser-induced stress wave

When a stress wave generated by focusing a femtosecond laser is loaded on an animal cell adhered on a substrate, the cell is detached from the substrate. There are two possible mechanisms for the cell detachment: (a) The cell is detached from a scaffold coated on a glass plate, and (b) the cell is detached from the glass plate with the scaffold. In this work, we have studied the cell-detachment mechanism by visualizing the scaffold with a fluorescence probe of quantum dots. When the cell was detached from the substrate, fluorescence from the scaffold simultaneously disappeared from the glass plate, although the scaffold was not irradiated by the laser. This indicates that detachment due to the stress wave is attributed to mechanism (a). On the other hand, when the cell was detached from the substrate by a trypsin treatment, the fluorescence from the scaffold remained, suggesting mechanism (b). By comparing both results, it is considered that physiological damage of the cell membrane during the detachment process by femtosecond laser-induced stress wave is less than that due to the trypsin treatment.     

Spectroscopy of laser-produced cerium plasma for remote isotope analysis of nuclear fuel

A cerium oxide sample was ablated by 2nd harmonic radiation of Nd:YAG laser at a power density of 0.1 GW/cm². Time evolution of the ablation plume was investigated by laser absorption time-of-flight (TOF) measurement. It was found that the ablated ionic plume in vacuum consisted of two components having different velocities whereas the ablated neutral atoms had mainly a single component. The flow velocity perpendicular to the sample surface in vacuum was determined to be 3.5 km/s for neutral atoms, and 4.7 km/s and 9.3 km/s for singly charged ions. From the detailed plume evolution in ambient atmosphere with several pressures we obtained some experimental conditions suitable for isotope analysis of atomic cerium.     

Formation of absorbing heterogeneous plasma layer by femtosecond laser-induced melting and ablation of silicon

The experimental study of absorption in silicon in infrared and visible spectral ranges, where the photon energy is less or more than the bandgap width, is performed by means of the ultrafast interferometry technique. The exactly solvable model in the electromagnetic of heterogeneous lossy plasma layer was developed. The density of carriers, their frequency of collisions, absorbing depth of the probing waves, real and imaginary parts of dielectric function of nonuniform layer and their spatial gradients are determined from the reflectance data by means of this model subject to the pump fluence. The heterogeneity-induced effects are visualized due to comparison of obtained plasma parameters with those calculated in the framework of homogeneous plasma model It is shown that in the intensity range near thresholds of melting and ablation the absorption, occurring in both cases mainly within a thin (∼10 nm) absorbing layer (similarly to metals), is due to free carrier intraband absorption.     

On clustering of aerosol particles in homogeneous turbulent shear flows

The objective of this paper is to present a model for predicting clustering of aerosol particles in uniformly sheared turbulent flows laden with small heavy particles. The background of the model for predicting clustering is based on a kinetic equation for the two-point probability density function of the relative velocity distribution of two particles. The effect of clustering of particles in homogeneous turbulent shear flows is demonstrated and compared with known results of direct numerical simulations. It is shown that the universality of the clustering process can take place if the characteristic cluster size is smaller than the shear scale.     

Hydroxyl radical consumption following photolysis of vapor-phase hydrogen peroxide at 266?nm: Implications for?photofragmentation laser-induced fluorescence measurements of?hydrogen peroxide

The decay of OH concentration following photolysis of room-temperature vapor-phase hydrogen peroxide is studied as a function of photolysis fluence at 266 nm in an open air environment. The rate of decay is found to increase with increasing photolysis fluence, i.e., with increasing number of photodissociated H₂O₂(g) molecules. Single-exponential functions approximate the OH concentration decay rather well, even for higher photolysis levels, and the decay time is shown to be inversely proportional to the H₂O₂(g) concentration. For fluences of about 450 mJ/cm² the difference between a single-exponential decay and measured data is becoming evident after approximately 150 μs. Calculations based on a chemical kinetics model agree well with experimental data also for times >150 μs. By combining the model with measurements, the actual photolysis levels used in experiments are estimated. The best fit between measured data and the model suggests that about 1.1% of the H₂O₂(g) molecules are dissociated with a photolysis fluence of ∼450 mJ/cm², in reasonable agreement with a Beer–Lambert based estimation. Excitation scans did not unfold any differences between OH spectra recorded at different photolysis fluences.     

Flexible 3D deep microstructures of silica glass by laser-induced backside wet etching

The well-controlled fabrication of microtrenches including inclined features using normal incidence with gradual shifting of the irradiated area was demonstrated. Based on the variation of trench width depending on the laser fluence, the existence of gaps between the edge of the irradiated area and sidewall of the trench was shown. Because of these gaps, the shifted laser pulse can stay at the bottom of the trenches in the fabrication of the inclined features. In laser-induced backside wet etching (LIBWE), the photo-activated region generated within organic solution would act on the glass surface and results in etching. It was indicated that the photo-activated region generated at the bottom of the trenches acted not only on the bottom of the trench but also on the sidewalls. Based on such etching of the sidewall, fabrication of inclined features becomes possible. In this method, the tilting angle can be changed within one deep trench. Flexible structure formation deep inside the silica glass can be achieved.     

Geometric Phases for Wave Packets of the Landau Problem

The Landau problem of a charged particle in a plane with a uniform perpendicular magnetic field is analysed in two oscillator modes. The coherent states for the problem have been found out using a general definition of displaced states. The time evolution and the associated nonadiabatic geometric phase for both initially displaced and non-displaced wave packets have been studied. The path integral is derived in a simple way through the calculation of Gaussian integrals via the concept of coherent state wavefunctions.