Boron isotope enrichment in nanosecond pulsed laser-ablation plume

Boron isotopic enrichment is observed in the laser ablation of B₄C target using nanosecond (ns) wide 532 nm laser beam of a Nd-YAG laser. B¹⁰/B¹¹ ratio of 0.9 against the natural abundance of 0.25 is obtained at a laser power density of 8×10⁸ W/cm² (fluence of 6.4 J/cm²). The enrichment as a function of laser power density is demonstrated using a quadrupole mass spectrometer. Apart from higher enrichment factor, only singly charged ions are found in the laser plume from the B₄C target, in contrast to the multiply charged ions from the BN target reported in a recent report using femtosecond (fs) laser pulses. This study indicates the possibility of using less expensive, widely used ns lasers, which can also yield a higher throughput per pulse than a fs laser for isotope enrichment. Received: 28 September 2001 / Accepted: 4 February 2002 / Published online: 3 June 2002 RID="*" ID="*"Corresponding author. Fax: +91-4114/480-065, E-mail: mj@igcar.ernet.in     

Short-pulse UV laser ablation of solid and liquid metals: indium

2 to 2.5 mJ/cm² when a 0.5 ps pulse is used instead of a 15 ns laser pulse. Measurements on liquid indium show a different behavior. With 15 ns laser pulses the threshold fluence is lowered by a factor of ∼3 from 100 mJ/cm² for solid indium to 30 mJ/cm² for liquid indium. In contrast, measurements with 0.5 ps laser pulses do not show any change in the ablation threshold and are independent of the phase of the metal at 2.5 mJ/cm². This behavior could be explained by thermal diffusion and heat conduction during the laser pulse and demonstrates in an independent way the energy lost into the material when long laser pulses are applied. Time-of-flight measurements to investigate the underlying ablation mechanism show thermal behavior of the ablated indium atoms for both ps and ns ablation and can be fitted to Maxwell-Boltzmann distributions. Received: 2 December 1996/Accepted: 11 December 1996     

Femtosecond laser ablation characteristics of nickel-based superalloy C263

Femtosecond laser (180 fs, 775 nm, 1 kHz) ablation characteristics of the nickel-based superalloy C263 are investigated. The single pulse ablation threshold is measured to be 0.26±0.03 J/cm² and the incubation parameter ξ=0.72±0.03 by also measuring the dependence of ablation threshold on the number of laser pulses. The ablation rate exhibits two logarithmic dependencies on fluence corresponding to ablation determined by the optical penetration depth at fluences below ∼5 J/cm² (for single pulse) and by the electron thermal diffusion length above that fluence. The central surface morphology of ablated craters (dimples) with laser fluence and number of laser pulses shows the development of several kinds of periodic structures (ripples) with different periodicities as well as the formation of resolidified material and holes at the centre of the ablated crater at high fluences. The debris produced during ablation consists of crystalline C263 oxidized nanoparticles with diameters of ∼2–20 nm (for F=9.6 J/cm²). The mechanisms involved in femtosecond laser microprocessing of the superalloy C263 as well as in the synthesis of C263 nanoparticles are elucidated and discussed in terms of the properties of the material.     

In situ observation of dynamics of plasma self-channeling and bulk modification in silica glasses induced by a high-intensity femtosecond laser

The time-resolved dynamics of plasma self-channeling and refractive index bulk modification in silica glasses were first observed in situ using a high-intensity femtosecond (110 fs) Ti:sapphire laser (λ_p=790 nm). Plasma channeling is induced in silica glass at an irradiation higher than an input intensity of 1.5×10¹² W/cm² and photoinduces either the refractive-index modification or optical crack modification. In the domain of refractive-index modification, the lifetime of induced plasma self-channeling was 20 ps and the structural transition time for forming the refractive-index change was 10 ps. In the domain of optical cracks, however, the lifetime of induced plasma formation was 30 ps and the structural transition time for forming the optical cracks was 40 ps. According to electron spin resonance spectroscopic (ESP) measurement, it was found that the defect concentration of the SiE^′ center increased significantly in the refractive index modification region. A maximum value of the refractive-index change Δn was measured to be 1.6×10^-2. The intensity profile of the output beam transmitted through the refractive-index modification showed that the bulk modification produced a permanent optical waveguide. Received: 8 April 2002 / Accepted: 12 April 2002 / Published online: 22 November 2002 RID="*" ID="*"Corresponding author. Fax: +81-48/462-4682, E-mail: shcho@riken.go.jp     

Tritium recovery from co-deposited layers using 193-nm laser

Recovery of tritium from co-deposited layers formed in deuterium–tritium plasma operations of the TFTR (Tokamak Fusion Test Reactor) was investigated by the use of an ArF excimer laser operating at the wavelength of 193 nm. At the laser energy density of 0.1 J/cm², a transient spike of the tritium-release rate was observed at initial irradiation. Hydrogen isotopes were released in the form of hydrogen-isotope molecules during the laser irradiation in vacuum, suggesting that tritium can be recovered readily from the released gases. In a second experiment, hydrogen (tritium) recovery from the co-deposited layers on JT-60 tiles that had experienced hydrogen-plasma operations was investigated by laser ablation with a focused beam of the excimer laser. The removal rate of the co-deposited layers was quite low when the laser energy density was smaller than the ablation threshold (1.0 J/cm²), but reached 1.1 μm/pulse at the laser energy density of 7.6 J/cm². The effective absorption coefficient in the co-deposited layers at the laser wavelength was determined to be 1.9 μm^-1. The temperature of the surface during the irradiation at the laser energy density of 0.5 J/cm² was measured on the basis of Planck’s law of radiation, and the maximum temperature during the irradiation decreased from 3570 K at the initial irradiation to 2550 K at the 1000th pulse of the irradiation. Received: 5 August 2002 / Accepted: 7 August 2002 / Published online: 28 October 2002 RID="*" ID="*"Corresponding author. Fax: +81-29/2825917, E-mail: shu@tpl.tokai.jaeri.go.jp     

Femtosecond-laser-induced nanostructure formed on hard thin films of TiN and DLC

We report observation of nanostructures formed on thin TiN and DLC films that were irradiated by 800- and 267-nm, femtosecond (fs) Ti:sapphire laser pulses at an energy fluence slightly above the ablation threshold. On the ablated thin-film surfaces, the linearly polarized fs pulses produce arrays of fine periodic structures that are almost oriented to the direction perpendicular to the laser polarization, while the circularly polarized light forms fine-dot structures. The size of these surface structures is 1/10–1/5 of the laser wavelength and decreases with a decrease in the laser wavelength. Received: 3 September 2002 / Accepted: 4 September 2002 / Published online: 17 December 2002 RID="*" ID="*"Corresponding author. Fax: +81-778/62-3306, E-mail: yasuma@fukui-nct.ac.jp     

Laser-based photoacoustic ammonia sensors for industrial applications

An industrial trace-ammonia sensor based on photoacoustic spectroscopy and CO₂ lasers has been developed for measuring ammonia with a 1σ detection limit of 220 parts-per-trillion (ppt) in an integration time of 30 s. The instrument response time for measuring ammonia was 200 s, limited by adsorption effects due to the polar nature of ammonia. The minimum detectable fractional absorbance was 2.0×10^-7, and the minimum normalized detectable absorption coefficient for this system was 2.4×10^-7 W cm^-1/z. The 9R(30) transition of the CO₂ laser at 9.22 μm with 2 W of output power was used to probe the strong sR(5,K) multiplet of ammonia at the same wavelength. This sensor was demonstrated with an optically multiplexed configuration for simultaneous measurement in four cells. Received: 3 April 2002 / Revised version: 31 May 2002 / Published online: 21 August 2002 RID="*" ID="*"Corresponding author. Fax: +1-310/458-0171, E-mail: webber@pranalytica.com     

Ablation with a single micropatterned KrF laser pulse: quantitative evidence of transient liquid microflow driven by the plume pressure gradient at the surface of polyesters

A microscopic flow of a transient liquid film produced by KrF laser ablation is evidenced on targets of PET and PEN. Experiments were done by using single pulses of the excimer laser beam micropatterned with the aid of submicron projection optics and grating masks. The samples of various crystalline states, ablated with a grating-forming beam (period Λ=3.7 μm), were precisely measured by atomic force microscopy, in order to evidence any deviation from the ablation behavior predicted by the current theory (combination of ablation curve and beam profile). This was confirmed by comparing various behaviors dependent on the polymer nature (PC, PET and PEN). PC is a normally ablating polymer in the sense that the ablated profile can be predicted with previous theory neglecting liquid-flow effects. This case is called ‘dry’ ablation and PC is used as a reference material. But, for some particular samples like crystalline PET, it is revealed that during ablation a film of transient liquid, composed of various components, which are discussed, can flow under the transient action of the gradient of the pressure of the ablation plume and resolidify at the border of the spot after the end of the pulse. This mechanism is further supported by a hydrodynamics theoretical model in which a laser-induced viscosity drop and the gradient of the plume pressure play an important role. The volume of displaced liquid increases with fluence (0.5 to 2 J/cm²) and satisfactory quantitative agreement is obtained with the present model. The same experiment done on the same PET polymer but prepared in the amorphous state does not show microflow, and such an amorphous sample behaves like the reference PC (‘dry’ ablation). The reasons for this surprising result are discussed. Received: 31 October 2002 / Accepted: 4 November 2002 / Published online: 22 January 2003 RID="*" ID="*"Present address: ST Microelectronics, Crolles, France RID="**" ID="**"Corresponding author. Fax: +33-556/84-6645, E-mail: s.lazare@lpcm.u-bordeaux1.fr     

Deposition of nanoparticles during laser ablation of nanoparticle-containing targets

We analyze the morphology of ablated nanoparticles after their laser-induced deposition on various substrates. We show that, at moderate laser intensity of the 210 ps pulses on the surface of nanoparticle-containing materials (<5×10⁹ W?cm^?2), the deposited material remains approximately the same as the initial nanoparticles. We compare these deposited nanoparticles with the debris obtained by the laser ablation of bulk material of the same origin as nanoparticles at different intensities of laser radiation. The presence of nanoparticles in laser plumes allowed for analyzing high-order nonlinear optical properties of nanoparticles. The efficient high-order harmonic generation was achieved during propagation of femtosecond pulses through such plasmas.     

A comparative study of the ionic keV X-ray line emission from plasma produced by the femtosecond,picosecond and nanosecond duration laser pulses

We report here an experimental study of the ionic keV X-ray line emission from magnesium plasma produced by laser pulses of three widely different pulse durations (FWHM) of 45 fs, 25 ps and 3 ns, at a constant laser fluence of ∼1.5 × 10⁴ J cm^− 2. It is observed that the X-ray yield of the resonance lines from the higher ionization states such as H- and He-like ions decreases on decreasing the laser pulse duration, even though the peak laser intensities of 3.5 × 10¹⁷ W cm^− 2 for the 45 fs pulses and 6.2 × 10¹⁴ W cm^− 2 for the 25 ps pulses are much higher than 5 × 10¹² W cm^− 2 for the 3 ns laser pulse. The results were explained in terms of the ionization equilibrium time for different ionization states in the heated plasma. The study can be useful to make optimum choice of the laser pulse duration to produce short pulse intense X-ray line emission from the plasma and to get the knowledge of the degree of ionization in the plasma.     

Quantitative analysis of dilute mixtures of SO<Subscript>2</Subscript> in N<Subscript>2</Subscript> at 7.4 μm by difference frequency spectroscopy

We describe a 7.4-μm source based on difference frequency generation with 6.5 mW of 1278-nm radiation from an extended cavity laser and 66 mW of 1544-nm radiation from another extended cavity laser, amplified in an erbium-doped fibre amplifier. Optimum focusing of the input beams in the 5×5×10-mm³ AgGaSe₂ crystal, and the spatial and temporal characteristics of the output beam, are determined. The source is used for accurate determination of line parameters for selected lines of the ν₃ band of SO₂, centred at 1361 cm^-1. Subsequently, these lines are used for performing quantitative analysis of gas mixtures containing SO₂ at concentration levels down to 4 ppm without relying on any calibration with certified gas mixtures. This demonstrates the potential of infrared spectroscopy as a primary method for low-concentration gas analysis. Received: 16 January 2003 / Revised version: 19 February 2003 / Published online: 9 April 2003 RID="*" ID="*"Corresponding author. Fax: +45-4593/1137, E-mail: jh@dfm.dtu.dk     

Ultrashort-pulse laser ablation of indium phosphide in air

Ablation of indium phosphide wafers in air was performed with low repetition rate ultrashort laser pulses (130 fs, 10 Hz) of 800 nm wavelength. The relationships between the dimensions of the craters and the ablation parameters were analyzed. The ablation threshold fluence depends on the number of pulses applied to the same spot. The single-pulse ablation threshold value was estimated to be φ_th(1)=0.16 J/cm². The dependence of the threshold fluence on the number of laser pulses indicates an incubation effect. Morphological and chemical changes of the ablated regions were characterized by means of scanning electron microscopy and Auger electron spectroscopy. Received: 30 May 2000 / Accepted: 31 May 2000 / Published online: 23 August 2000     

Cavity-enhanced absorption: detection of nitrogen dioxide and iodine monoxide using a violet laser diode

We present an application of cavity-enhanced absorption spectroscopy with an off-axis alignment of the cavity formed by two spherical mirrors and with time integration of the cavity-output intensity for detection of nitrogen dioxide (NO₂) and iodine monoxide (IO) radicals using a violet laser diode at λ=404.278 nm. A noise-equivalent (1σ≡ root-mean-square variation of the signal) fractional absorption for one optical pass of 4.5×10^-8 was demonstrated with a mirror reflectivity of ∼0.99925, a cavity length of 0.22 m and a lock-in-amplifier time constant of 3 s. Noise-equivalent detection sensitivities towards nitrogen dioxide of 1.8×10¹⁰ molecule cm^-3 and towards the IO radical of 3.3×10⁹ molecule cm^-3 were achieved in flow tubes with an inner diameter of 4 cm for a lock-in-amplifier time constant of 3 s. Alkyl peroxy radicals were detected using chemical titration with excess nitric oxide (RO₂+NO→RO+NO₂). Measurement of oxygen-atom concentrations was accomplished by determining the depletion of NO₂ in the reaction NO₂+O→NO+O₂. Noise-equivalent concentrations of alkyl peroxy radicals and oxygen atoms were 3×10¹⁰ molecule cm^-3 in the discharge-flow-tube experiments. Received: 4 February 2003 / Revised version: 10 March 2003 / Published online: 12 May 2003 RID="*" ID="*"Corresponding author. Fax: +44-1865/275-410, E-mail: vlk@physchem.ox.ac.uk     

Modification of the fused silica glass network associated with waveguide fabrication using femtosecond laser pulses

Atomic-scale structural changes have been observed in the glass network of fused silica after modification by tightly focused 800-nm, 130-fs laser pulses at fluences between 5 and 200 J cm^-2. Raman spectroscopy of the modified glass shows an increase in the 490 and 605-cm^-1 peaks, indicating an increase in the number of 4- and 3-membered ring structures in the silica network. These results provide evidence that densification of the glass occurs after exposure to fs pulses. Fluorescence spectroscopy of the modified glass shows a broad fluorescence band at 630 nm, indicating the formation of non-bridging oxygen hole centers (NBOHC) by fs pulses. Waveguides that support the fundamental mode at 633 nm have been fabricated inside fused silica by scanning the glass along the fs laser beam axis. The index changes are estimated to be approximately 0.07×10^-3. Received: 17 December 2001 / Accepted: 9 July 2002 / Published online: 25 October 2002 RID="*" ID="*"Corresponding author. Fax: +1-925/423-2463, E-mail: dmkrol@ucdavis.edu     

Femtosecond laser micromilling of Si wafers

Femtosecond laser micromilling of silicon is investigated using a regeneratively amplified 775 nm Ti:Sapphire laser with a pulse duration of 150 fs operating at 1 kHz repetition rate. The morphological observation and topological analysis of craters fabricated by single-shot laser irradiation indicated that the material removal is thermal in nature and there are two distinct ablation regimes of low fluence and higher fluence with logarithmical relations between the ablation depth and the laser fluence. Crater patterns were categorized into four characteristic groups and their formation mechanisms were investigated. Femtosecond laser micromilling of pockets in silicon was performed. The effect of process parameters such as pulse energy, translation speed, and the number of passes on the material removal rate and the formation of cone-shaped microstructures were investigated. The results indicate that the microstructuring mechanism has a strong dependence on the polarization, the number of passes and laser fluence. The optimal laser fluence range for Si micromilling was found to be 2-8 J/cm² and the milling efficiency attains its maximum between 10 and 20 J/cm².     

Sub-part-per-billion detection of nitric oxide in air using a thermoelectrically cooled mid-infrared quantum cascade laser spectrometer

Non-cryogenic, laser-absorption spectroscopy in the mid-infrared has wide applications for practical detection of trace gases in the atmosphere. We report measurements of nitric oxide in air with a detection limit less than 1 nmole/mole (<1 ppbv) using a thermoelectrically cooled quantum cascade laser operated in pulsed mode at 5.26 μm and coupled to a 210-m path length multiple-pass absorption cell at reduced pressure (50 Torr). The sensitivity of the system is enhanced by operating under pulsing conditions which reduce the laser line width to 0.010 cm^-1 (300 MHz) HWHM, and by normalizing pulse-to-pulse intensity variations with temporal gating on a single HgCdTe detector. The system is demonstrated by detecting nitric oxide in outside air and comparing results to a conventional tunable diode laser spectrometer sampling from a common inlet. A detection precision of 0.12 ppb Hz^-1/2 is achieved with a liquid-nitrogen-cooled detector. This detection precision corresponds to an absorbance precision of 1×10^-5 Hz^-1/2 or an absorbance precision per unit path length of 5×10^-10 cm^-1 Hz^-1/2. A precision of 0.3 ppb Hz^-1/2 is obtained using a thermoelectrically cooled detector, which allows continuous unattended operation over extended time periods with a totally cryogen-free instrument. Received: 1 May 2002 / Revised version: 6 June 2002 / Published online: 21 August 2002 RID="*" ID="*"Corresponding author. Fax: +1-978/663-4918, E-mail: ddn@aerodyne.com     

Influence of laser pulse width on absolute EUV-yield from Xe-clusters

Using 50 fs ( ∼ 2×10¹⁸ W/cm²) and 2 ps ( ∼ 5×10¹⁶ W/cm²) pulses from a Ti:Sa multi-TW laser at 800 nm wavelength large Xe-clusters ( 10⁵...10⁶ atoms per cluster) have been excited. Absolute yield measurements of EUV-emission in a wavelength range between 10 nm and 15 nm in combination with cluster target variation were carried out. The ps-laser pulse has resulted in about 30% enhanced and spatially more uniform EUV-emission compared to fs-laser excitation. Circularly polarized laser light instead of linear polarization results in enhanced emission which is probably caused by electrons gaining higher energies by the polarization dependent optical field ionization process. An absolute emission efficiency at 13.4 nm of up to 0.8% in 2π sr and 2.2% bandwidth has been obtained. Received 11 January 2001 and Received in final form 27 March 2001     

Oxygen plasma and high pressure H<Subscript>2</Subscript>O vapor heat treatments used to fabricate polycrystalline silicon thin film transistors

Oxygen plasma and high pressure H₂O vapor heat treatment were applied to fabrication of n-channel polycrystalline silicon thin film transistors (poly-Si TFTs). 13.56 MHz-oxygen-plasma treatment at 250 °C, 100 W for 5 min effectively reduced defect states of 25-nm-thick silicon films crystallized by 30 ns-pulsed XeCl excimer laser irradiation. 1.3×10⁶-Pa-H₂O vapor heat treatment at 260 °C for 3 h was carried out in order to improve electrical properties of SiO_x gate insulators and SiO_x/Si interfaces. A carrier mobility of 470 cm²/V s and a low threshold voltage of 1.8 V were achieved for TFTs fabricated with crystallization at 285 mJ/cm². Received: 18 November 2002 / Accepted: 25 November 2002 / Published online: 11 April 2003 RID="*" ID="*"Corresponding author. Fax: +81-42/388-7109, E-mail: tsamesim@cc.tuat.ac.jp     

Cavity-enhanced absorption spectroscopy with a rapidly swept diode laser

Cavity-enhanced absorption spectroscopy is explained in terms of the transmission function of a rapidly swept interferometer, and the integrated transmission is shown to be proportional to the cavity ringdown time. The technique is demonstrated on the b¹Σ_g ⁺-X³Σ_g ^-  (1,0) band in molecular oxygen at 687 nm using a tunable diode laser and a relative-ly high-Q optical cavity (finesse ≈4000). A detection limit of 3×10^-8 cm^-1 s^1/2 is achieved for a 0.8 cm^-1 scanning range. Received: 24 June 2002 / Revised version: 5 August 2002 / Published online: 15 November 2002 RID="*" ID="*"Corresponding author. Fax: +44-1865/275410, E-mail: peverall@physchem.ox.ac.uk     

Passive Q-switching of 1.44 μm and 1.34 μm diode-pumped Nd:YAG lasers with a V:YAG saturable absorber

Spectroscopic data of a V³⁺:YAG passive Q-switch crystal were measured. The absorption recovery time was determined to be of 37±7 ns and the ground state absorption cross section was estimated to be 0.7×10^-18 cm² at 1.44 μm and 3.5×10^-18 cm² at 1.34 μm. Passively Q-switched operation of diode pumped 1.44 μm and 1.3 μm Nd:YAG lasers was demonstrated using this crystal as saturable absorber. Average output powers of 1.42 W (1.44 μm) and 1.56 W (1.34 μm) and pulse energies of 24 μJ (1.44 μm) and 25 μJ (1.34 μm) were observed, respectively. Received: 19 August 2002 / Published online: 12 February 2003 RID="*" ID="*"Corresponding author. Fax: +49-40/42838-6281, E-mail: kretschmann@physnet.uni-hamburg.de