Effect of ZnO plasma plume dynamics on laser ablation

The dynamic behaviors and optical properties of a ZnO plasma plume produced by pulsed laser ablation using a Nd:YAG laser (wavelength: 532 nm, pulse width: 3 ns) were studied by fast photography using a commercial gated charge coupled device (CCD) camera linked with a delay circuit and by optical emission spectroscopy at various ambient oxygen pressures. Fast photography was conducted with a resolving power of 0.25 μs and the expansion behaviors of the laser ablation plume were observed. Plasma plume expansion velocity decreased with oxygen partial pressure. The flow of the plasma plume in the early stage of expansion of up to 3 ms agreed well with the drag model.     

Characterization of a collinear double pulse laser-induced plasma at several ambient gas pressures by spectrally- and time-resolved imaging

A collinear double pulse laser-induced plasma was characterised by means of a spectrally and time resolved imaging technique. The beams of two Q-switched Nd:YAG lasers were focused on a brass target in a vacuum chamber to form the plasma. The plume emission intensity and spatial distribution were recorded with temporal resolution using an intensified CCD. Using a set of interference filters, we collected images of the emission from the major target components as well as from oxygen. Both the laser inter-pulse separation (in the range between 0 and 10 s) and the ambient air pressure value (in the range between 10⁵ and 10 Pa) were varied during the experiment. At atmospheric pressure, an enhancement of the line emission from the target elements was observed for delayed laser pulses compared to coincident pulses. However, this enhancement effect tends to fall at low pressure values, and a decrease of the signal is observed for pressures under about 10⁴ Pa. Moreover, it was observed that the evaluation of the enhancement factor strongly depends on the detector field of view. The propagation of the emitting plume was also studied at several pressures and inter-pulse delays.     

Temporal and spatial TaO emission generated from UV laser ablation of Ta and Ta2O5 in oxygen ambient

2 O₅ targets in oxygen ambient are presented. Line assignments indicate the presence of the excited Ta(I), Ta(II), and TaO in the plume. At higher oxygen pressure, a single peak appears in the TaO emission spectrum from the laser ablation of Ta while two peaks corresponding to a fast and a slow component of TaO emission are observed from the laser ablation of the Ta₂O₅ target by time-resolved emission spectroscopy. The delay times after laser pulse corresponding to two components of TaO emission from the laser ablation of Ta₂O₅ have been investigated as a function of oxygen pressure, laser fluence, and observation distance from the target surface. The two components of TaO emission could be attributed to different pathways for the generation of excited TaO molecules. A blast wave model is proposed to describe the behavior of the excited TaO in the plume of laser ablation of Ta₂O₅. Received: 1 February 1997/Accepted: 12 March 1997     

Subpicosecond laser ablation of copper and fused silica: Initiation threshold and plasma expansion

We investigated the subpicosecond laser ablation of copper and fused silica under 100 fs laser irradiation at 800 nm in vacuum by means of fast plume imaging and time- and space-resolved optical emission spectroscopy. We found that, to the difference of copper ablation, the laser-generated plasma from a fused silica target exhibited one “main” component only. The “slow” plasma component, observed during copper ablation and usually assigned to optical emission from nanoparticles was not detected by either plasma fast imaging or optical emission spectroscopy even when fused silica targets were submitted to the highest incident fluences used in our experiments. The characteristic expansion velocity of this unique component was about three times larger than the velocity of the fast plume component observed during copper ablation. The dependence of laser fluence on both plasma expansion and ablation rate was investigated and discussed in terms of ablation efficiency and initiation mechanisms.     

Effects of transverse magnetic field on a laser-produced Zn plasma plume and ZnO films grown by pulsed laser deposition

By adopting a fast photography and time-resolved optical emission spectrometry, we have investigated the effects of transverse magnetic field on the expansion dynamics and enrichment of Zn atoms and Zn⁺ ions in a plume produced by laser ablation of a Zn target in oxygen atmosphere. Plume splitting due to the magnetic field was apparent but the splitting patterns of Zn and Zn⁺ were totally different. The surface morphology and photoluminescence characteristics also changed significantly. In particular, the growth rate increased by as much as 2.4-4.3 times compared to the conventional PLD method.     

Plume temperature in the laser ablation of polyimide films measured by infrared emission spectroscopy

The infrared emission spectrum of the plume produced by KrF excimer laser ablation of polyimide films in air and in He was measured in the 680 to 1580 cm^–1 wavenumber range. Using 400 mJ/cm² laser pulses of 248 nm and 35 ns duration yielded a strong emission band characteristic of thev ₂ transitions of hot HCN molecules. Band counters calculations were carried out of thev ₂ emission expected from HCN in thermal equilibrium at various temperatures. They indicate that except for a slight deviation of the measured data from thermal equilibrium, the best fit of the observed results is obtained at a plume temperature of 2250±150K.     

Dynamics of a pulsed laser generated tin plasma expanding in an oxygen atmosphere

Semiconducting tin oxide can be successfully deposited by means of the laser ablation technique. In particular by ablating metallic tin in a controlled oxygen atmosphere, thin films of SnO _x have been deposited. The partial oxygen pressure at which the films are deposited strongly influences both the stoichiometry and the structural properties of the films. In this work, we present a study of the expansion dynamics of the plasma generated by ablating a tin target by means of a pulsed laser using time and space resolved optical emission spectroscopy and fast photography imaging of the expanding plasma. Both Sn I and Sn II optical emission lines have been observed from the time-integrated spectroscopy. Time resolved-measurements revealed the dynamics of the expanding plasma in the ambient oxygen atmosphere. Stoichiometry of the films has been determined by means of X-ray photoelectron spectroscopy and correlated to the expansion dynamics of the plasma.     

Collective behavior of laser-produced plasma from a multicomponent YBa2Cu3O7 target in air

2 Cu₃O₇, using a Q-switched Nd:YAG laser is investigated by time-resolved emission-spectroscopic techniques at various laser irradiances. It is observed that beyond a laser irradiance of 2.6×10¹¹ W cm^-2, the ejected plume collectively drifts away from the target with a sharp increase in velocity to 1.25×10⁶ cm s^-1, which is twice its velocity observed at lower laser irradiances. This sudden drift apparently occurs as a result of the formation of a charged double layer at the external plume boundary. This diffusion is collective, that is, the electrons and ions inside the plume diffuse together simultaneously and hence it is similar to the ambipolar diffusion of charged particles in a discharge plasma. Received: 30 January 1998/Revised version: 12 June 1998     

Plasma dynamics from laser ablated solid lithium

Emission plasma plume generated by pulsed laser ablation of a lithium solid target by a ruby laser (694 nm, 20 ns, 3 J) was subjected to optical emission spectroscopy: time and space resolved optical emission was characterised as a function of distance from the target surface. Propagation of the plume was studied through ambient background of argon gas. Spectroscopic observations can, in general, be used to analyse plume structure with respect to an appropriate theoretical plasma model. The plume expansion dynamics in this case could be explained through a shock wave propagation model wherein, the experimental observations made were seen to fit well with the theoretical predictions. Spectral information derived from measurement of peak intensity and line width determined the parameters, electron temperature (T _e) and electron number density (n _e), typically used to characterise laser produced plasma plume emission. These measurements were also used to validate the assumptions underlying the local thermodynamic equilibrium (LTE) model, invoked for the high density laser plasma under study. Some interesting results pertaining to the analysis of plume structure and spatio-temporal behaviour of T _e and n _e along the plume length will be presented and discussed.     

Titanium oxide nanostructured films by reactive pulsed laser deposition

Nanostructured titanium oxide thin films have been grown by nanosecond UV pulsed laser deposition (PLD) performed in a reactive background atmosphere. We exploited laser ablation of a Ti target at different pressures of pure oxygen and Ar:O₂ mixtures to show that film growth can be tuned at the nanoscale from compact and dense to columnar and to porous, leading to different morphology, density and structure (oxidized fraction and degree of crystallinity). We observed that the position of the substrate relative to the time integrated visible plume front is fundamental in the determination of film structure and morphology. Film growth and film properties can be related to a non-dimensional parameter L which is the ratio between the target-to-substrate distance and the visible plume length. In particular, surface morphology and degree of structural order are strictly related to L irrespective of the oxygen content, while the latter mainly affects the oxidized fraction in the film.     

Nanosecond and femtosecond ablation of La0.6Ca0.4CoO3: a comparison between plume dynamics and composition of the films

Thin films of La_0.6Ca_0.4CoO₃ were grown by pulsed laser ablation with nanosecond and femtosecond pulses. The films deposited with femtosecond pulses (248 nm, 500 fs pulse duration) exhibit a higher surface roughness and deficiency in the cobalt content compared to the films deposited with nanosecond pulses (248 nm, 20 ns pulse duration). The origin of these pronounced differences between the films grown by ns and fs ablation has been studied in detail by time-resolved optical emission spectroscopy and imaging. The plumes generated by nanosecond and femtosecond ablation were analyzed in vacuum and in a background pressure of 60 Pa of oxygen. The ns-induced plume in vacuum exhibits a spherical shape, while for femtosecond ablation the plume is more elongated along the expansion direction, but with similar velocities for ns and fs laser ablation. In the case of ablation in the background gas similar velocities of the plume species are observed for fs and ns laser ablation. The different film compositions are therefore not related to different kinetic energies and different distributions of various species in the plasma plume which has been identified as the origin of the deficiency of species for other materials.     

Microplasma generated at solid–solid interface and its application to nanostructure formation

The dynamics of the microplasmas created at a transparent solid–solid interface were investigated extensively. Microplasmas were generated at an interface between a carbon (C) or a germanium (Ge) target and a SiO₂ substrate by irradiating a KrF excimer laser beam onto the target, and the dynamics of the plasmas were investigated with the aid of optical emission spectroscopy. Although the emission spectra that contained the characteristic emission lines and the absorption bands originated from C and Ge species were observed from the C and Ge plasmas without the SiO₂ substrate, identical spectra were obtained from both the plasmas created at the C–SiO₂ and Ge–SiO₂ interfaces. Furthermore, the target and the Si substrate surfaces were examined with a scanning electron microscope. The SiO₂ substrate was smoothly etched and a nanostructure of a chain-like morphology was also observed in the deposits on the SiO₂ substrate.     

Gas pressure effects on the structure of CNx thin films deposited by laser ablation

Carbon nitride thin films with different nitrogen concentration have been deposited at different N₂ and N₂/Ar mixed partial pressures. Time-integrated optical emission spectroscopy measurements have been performed to gather information on the nature of the chemical species present in the plasma. Both the CN and C₂ molecular species have been observed. Fast photography imaging of the expanding plume revealed the change of the dynamics from a free expansion at low pressure to a shock wave formation followed then by the plume stopping upon increasing the gas pressure values. Raman and XPS spectroscopy measurements performed on the deposited thin films revealed that the films, structure strongly depends on the dynamics of the expansion plasma regime rather than on the partial pressure at which the deposition takes place.     

Observation of magnetic-field-enhanced excitation and ionization in the plume of KrF-laser-ablated magnesium

The influence of a magnetic field on the plume produced by KrF-laser ablation of magnesium in vacuum has been investigated using time-integrated photography, streak photography, spectroscopy and charge probes. Line emission spectra in the 200–600 nm interval and effective stream velocities for the plume obtained from the spatiotemporal emission from specific neutral and ion lines are reported. Time of flight velocities are also deduced from measurements using simple charge-collector probes. Changes in the plume structure and dynamics, and enhanced emission and ionization are observed in the presence of the field. A qualitative explanation of the results is given in terms of a magnetohydrodynamic model.     

Wavelength Shift Investigation of Optical Emission from Nanosecond Pulsed Laser Ablated Metal Al

The wavelength shift of optical emission from pulsed laser ablation of metal Al in 1atm air has been investigated by using the time-resolved optical emission spectroscopy (OES). The wavelength shift of OES has a second order exponential decay with time and was also found to be significantly influenced by the laser ablated pulse energy. By taking account of the shielding effect of free electrons inside of the plasma plume, the relation between the electron density and wavelength shift has been discussed.     

Pulsed laser deposition of TiO<Subscript>2</Subscript>: diagnostic of the plume and characterization of nanostructured deposits

Promising applications of TiO₂ nanostructures include the development of optical devices, sensors, photocatalysts and self-cleaning coatings. In view of their importance, research on the synthesis of nanosized TiO₂ is a particularly active field. In this work we report on the investigation of the effect of laser irradiation wavelength (Q-switched Nd:YAG laser at 532, 355 and 266 nm), the temperature of the substrate and the atmosphere of deposition (vacuum, Ar and O₂) that are suitable for obtaining nanostructured deposits from TiO₂ sintered targets. The ablation plume emission is characterized with spectral and temporal resolution by optical emission spectroscopy (OES), while the surface morphology and chemical states of the material deposited on a Si (100) substrate are examined by environmental scanning electron microscopy (ESEM) and atomic force microscopy (AFM) and by X-ray photoelectron spectroscopy (XPS), respectively. Deposits with nanostructured morphology with grain size down to 40 nm and keeping the stoichiometry of the targets were obtained at high temperature, while the highest concentration of particulates was observed at the longest laser wavelength of 532 nm on a substrate heated up to 650°C. In situ characterization of the ablation plume, carried out by OES, indicated the presence of emissions assigned to Ti I, Ti II and O I.     

Laser ablation of AsxSe100−x chalcogenide glasses: Plume investigations

The use of amorphous chalcogenides offers advantages such as remarkable optical properties like a wide transmission window (∼1-20 μm) depending upon composition, making them suitable for sensitive detection of clinical or environmental changes. They also present interesting high (non)linear refractive indices, photorefractive effects, and other properties interesting for wavelength conversion, all-optical switching or modulation, Raman and parametric amplification, laser sources for mid-IR, etc.Slab waveguides based on chalcogenide amorphous films with good adherence and controlled composition can be obtained using pulsed laser deposition allowing to design and to manufacture complex optical functions on waveguides within a small and compact chip. The aim of this work is to characterize the ejection plume obtained by laser ablation of As_xSe_100−x samples in order to get some insight on the process involved for optimizing the pulsed laser deposition process. The dynamics of the plume has been systematically investigated by ICCD camera fast imaging and space- and time-resolved optical emission spectroscopy for samples of various compositions.