Dynamic temporal pulse shaping in advanced ultrafast laser material processing

Phase-manipulated ultrafast laser pulses and temporally tailored pulse trains with THz repetition rates are promising new tools for quality micromachining of brittle dielectrics, allowing to adapt the laser energy delivery rate to the material properties for optimal processing. Different materials respond with specific reaction pathways to the sudden energy input depending on the efficiency of electron generation and on the ability to release the energy into the lattice. The sequential energy delivery with judiciously chosen pulse trains may induce softening of the material during the initial steps of excitation and change the energy coupling for the subsequent steps. We show that this can result in lower stress, cleaner structures, and allow for a material-dependent optimization process. Received: 7 October 2002 / Accepted: 20 January 2003 / Published online: 28 May 2003 RID="*" ID="*"Corresponding author. Fax: +49-30/6392-1229, E-mail: stoian@mbi-berlin.de RID="**" ID="**"Now at Katana Technologies GmbH, Albert-Einstein-Ring 7, 14532 Kleinmachnow, Germany     

A high-sensitivity in situ optical diagnostic technique for laser cleaning of transparent substrates

A differential optical transmission technique has been used to monitor in situ the efficiency of laser cleaning for the removal of sub-micrometer-sized particles on substrates transparent at the monitoring wavelength. This technique has been applied to the removal of sub-micrometer polystyrene particles on polyimide substrates using laser pulses of 30 ps duration at 292 nm while probing the material transmission at 633 nm. The sensitivity achieved -1/10⁴ for the transmission changes induced upon single-pulse laser exposure – allows us to monitor the removal of just a few sub-micron-sized particles from the probed region inside the irradiated area. Received: 2 October 2002 / Accepted: 7 October 2002 / Published online: 29 January 2003 RID="*" ID="*"Corresponding author. Fax: +33-3/87844082, E-mail: nchaoui@iut.univ-metz.fr RID="**" ID="**"Present address: Laboratoire de Chimie et Applications, Institut Universitaire de Technologie de Metz, Département Chimie, Rue Victor Demange, 57500 Saint-Avold, France     

All-reflective interferometric autocorrelator for the measurement of ultra-short optical pulses

We have developed a novel interferometric autocorrelator composed of only reflective elements, which functions as a beam splitter and an optical delay line. Analytical expressions are derived to give second-order autocorrelation functions and deconvolution factors for various conditions. The measurement of femtosecond laser pulses by interferometric autocorrelation is demonstrated in the visible region. The results are compared with those by calculation. Received: 9 December 2002 Revised version: 18 February 2003 / Published online: 5 May 2003 RID="*" ID="*"Present address: Department of Physics, Tokai University, 1117 Kitakaname, Hiratsuka, Kanagawa 259-1207, Japan RID="**" ID="**"Corresponding author. Fax: +81-48/462-4682, E-mail: asuda@postman.riken.go.jp     

Transmission and scanning electron microscopy studies of single femtosecond- laser-pulse ablation of silicon

The final state of the material resulting from laser irradiation of silicon using 130 fs pulses at 790 nm was studied using a number of techniques including scanning and transmission electron microscopies, as well as atomic force microscopy. Structural details and the level of damage to the nearby solid following irradiation were characterized and are discussed in the context of recent dynamical studies. Received: 28 September 2001 / Accepted: 3 March 2002 / Published online: 19 July 2002 RID="*" ID="*"Department of Engineering Physics, McMaster University, Hamilton, Ontario, L8S 4M1, Canada RID="**" ID="**"Corresponding author. Fax: +1-905/521-2773, E-mail: borowia@mcmaster.ca RID="***" ID="***"Present address: Department of Physics and Astronomy, University of Glasgow, Glasgow, G12 8QQ, UK RID="****" ID="****"Department of Materials Science and the CEMD, McMaster University, Hamilton, Ontario, L8S 4M1, Canada RID="*****" ID="*****"Departments of Engineering Physics, and Physics and Astronomy, and the CEMD, McMaster University, Hamilton, Ontario, L8S 4M1, Canada     

Time-resolved thermal lens study on the heat dissipation effects in solid polymeric matrices used as laser dyes

A dual-beam pulsed-laser time-resolved thermal lens (TRTL) has been used to study the heat dissipation effects in solid polymers employed as laser dyes. The laser-dye samples studied are polymer solutions of rhodamine 6G (Rh6G), namely homopolymers of methyl methacrylate (MMA) and copolymers of methyl methacrylate and 2-hydroxyethyl methacrylate (HEMA) with MMA:HEMA compositions 1:1 and 7:3 vol./vol., where the dye is either dissolved or modified and copolymerized with methacrylate monomers. The long-term stability of the laser material is independent of the thermal diffusivity of the samples, as determined by the TRTL technique. This suggests that the rate of heat dissipation does not play a major role in the photostability of the samples. In contrast, the TRTL experiments have revealed permanent changes in the optical properties of the polymers when subjected to a large number of laser pulses. This is explained in terms of permanent plastic deformation of the matrices. Received: 19 June 2002 / Revised version: 1 August 2002 / Published online: 15 November 2002 RID="*" ID="*"Dedicated to Prof. S.E. Braslavsky on the occasion of her 60th birthday. This work was presented at the V Congreso de Fotoquímica, Torremolinos, Spain, 2001 RID="**" ID="**"Corresponding author. Fax: +34-93/205-6266, E-mail: s.nonell@iqs.es     

Novel technique for the measurement of fiber dispersion properties

We present a novel method for measuring the linear and nonlinear dispersion properties of conventional and micro-structured fibers. It is based on the automated compensation of phase modulations using a high-resolution pulse-shaping device. No tunable laser source is required. Received: 20 December 2002 / Published online: 19 March 2003 RID="*" ID="*"Corresponding author. Fax: +49-3641/947202, E-mail: stobrawa@ioq.uni-jena.de RID="**" ID="**"Present address: Carl Zeiss Meditec AG, G?schwitzer Strasse 51–52, 07745 Jena, Germany     

The application of quasi-phase-matched parametric light sources to practical infrared chemical sensing systems

Quasi-phase-matched (QPM) materials allow the generation of spectroscopically useful infrared radiation in an efficient and broadly tunable format. Here, we describe several applications of QPM-based light sources to remote and local chemical sensing. The remote systems are gas imagers that employ a fiber-pumped continuous-wave optical parametric oscillator or a microlaser-pumped, diode-seeded optical parametric amplifier as the illumination source. Technology described for local sensing includes a cavity ring down spectrometer that employs a novel optical parametric generator–amplifier to achieve ≥350 cm^-1 of contiguous tuning and a long-wave infrared light source based on QPM GaAs. In each case the use of QPM materials in conjunction with effective pump sources instills simplicity and ruggedness into the sensing systems. Received: 15 April 2002 / Revised version: 6 June 2002 / Published online: 12 September 2002 RID="*" ID="*"Corresponding author. Fax: +1-925/294-2595, E-mail: tjkulp@sandia.gov RID="**" ID="**"Present address: Corning Inc., Corning, NY 14831, USA RID="*" ID="*"Present address: Corning Inc., Corning, NY 14831, USA RID="**" ID="**"Present address: Blue Leaf Networks, Sunnyvale, CA 94086, USA RID="***" ID="***"Present address: Sandia National Laboratories, Albuquerque, NM 87185, USA     

Characterization of nonlinear optical parameters of polymethine dyes

We investigated nonlinear refraction, nonlinear absorption, and saturable absorption of polymethine dyes by the Z-scan technique (λ=1064 nm). The analysis of simultaneous appearance of several nonlinear optical processes in dye solutions excited by picosecond pulses was carried out. The saturable absorption was analyzed taking into account various models. Nonlinear refractive indices, nonlinear absorption coefficients, and saturation intensities of various polymethine dyes were measured. Received: 27 December 2002 / Revised version: 6 March 2003 / Published online: 5 May 2003 RID="*" ID="*"Corresponding author. Fax: +81-471/363-366, E-mail: r_ganeev@issp.u-tokyo.ac.jp RID="**" ID="**"Present address: The Institute for Solid State Physics, The Tokyo University, 5-1-5 Kashiwanoha, Kashiwa, Chiba 277-8581, Japan     

Studies of high-repetition-rate laser plasma EUV sources from droplet targets

The water droplet laser plasma source has been shown to have many attractive features as a continuous, almost debris-free source for extreme ultraviolet (EUV) and X-ray applications. Through a dual experimental and theoretical study, we analyze the interaction physics between the laser light and the target. The hydrodynamic laser plasma simulation code, Medusa103 is used to model the electron density distribution for comparison to electron density distributions obtained through Abel inversion of plasma interferograms. In addition, flat field EUV spectra are compared to synthetic spectra calculated with the atomic physics code RATION. Received: 31 October 2002 / Accepted: 8 February 2003 / Published online: 28 May 2003 RID="*" ID="*"Present address: Naval Reseach Laboratory, Washington D.C. RID="**" ID="**"Present address: Xtreme Technologies, G?ttingen, Germany. RID="***" ID="***"Corresponding author. Fax: +1-407/823-3570, E-mail: mrichard@mail.ucf.edu     

A 7-W diode-pumped Nd:YVO4 cw laser at 1.34 μm

A Nd:YVO₄ laser, end-pumped by a fiber-coupled diode-laser array, generates 7.3 W of output power at 1342 nm, the highest so far reported for this host crystal. The slope efficiency is 40% and the output-beam divergence is close to the diffraction limit. An important point in attaining such results is the choice of crystals with low Nd concentration. Received: 16 July 2002 / Published online: 25 October 2002 RID="*" ID="*"Corresponding author. Fax: +39-050/844333, E-mail: dilieto@df.unipi.it RID="**" ID="**"Permanent address: Scuola Normale Superiore, Piazza dei Cavalieri 7, Pisa, Italy     

Amplification and wave mixing of induced and spontaneous emission in semiconductor laser amplifiers

We theoretically describe and experimentally investigate the spatio-spectral wave mixing of induced and spontaneous emission in large-area InGaAs-semiconductor laser amplifiers. The dynamic light-matter-coupling is described by a spatially resolved theory based on Maxwell–Bloch–Langevin equations, taking into account many-body-carrier interactions, energy transfer between the carrier and phonon systems and, in particular, the spatio-temporal interplay of stimulated and amplified spontaneous emission and the noise caused by spontaneous emission. Our numerical model reveals the fundamental physical processes which are responsible for the spectral power distribution of the amplified laser light and predicts the emission properties of high-power semiconductor laser amplifiers, such as emission spectra and input power–output power characteristics. Received:30October2002/Revisedversion:21November2002 / Published online: 12 February 2003 RID="*" ID="*"Corresponding author. Fax: +49-711/6862-349, E-mail: Edeltraud.Gehrig@dlr.de RID="**" ID="**"Also at: Institute of Physics, Tampere University of Technology, P.O. Box 692, FIN-33101, Tampere, Finland RID="***" ID="***"Present address: Heidelberger Druckmaschinen AG, Speyerer Strasse 6, 69115 Heidelberg, Germany RID="****" ID="****"Present address: Lightbit Corporation, 411 Clyde Avenue, Mountain View, CA 94043, USA     

Characterization of laser-ablated and chemically reduced silver colloids in aqueous solution by UV/VIS spectroscopy and STM/SEM microscopy

Silver colloids in aqueous solution were studied by different scanning microscopy techniques and UV/VIS spectroscopy. The silver colloids were produced either by chemical reduction or by nanosecond laser ablation from a solid silver foil in water. Variation of laser power and ablation time leads to solutions of metal clusters of different sizes in water. We characterized the electronic absorption of the clusters by UV/VIS spectroscopy. STM (scanning tunneling microscope) imaging of the metal colloids shows atomic resolution of rod- or tenon-like silver clusters up to 10-nm length formed by laser ablation. Our scanning electron microscope measurements, however, show that much larger silver colloids up to 5-μm length are also formed, which are not visible in the STM due to their roughness. We correlate them with the long-wavelength tail of the multimodal UV/VIS spectrum. The silver colloids obtained by chemical reduction are generally larger and their electronic spectra are red-shifted compared to the laser-ablated clusters. Irradiation of the colloid solution with nanosecond laser pulses of appropriate fluence at 532 nm and 355 nm initially reduced the colloid size. Longer irradiation at 355 nm, however, leads to the formation of larger colloids again. There seems to be a critical lower particle size, where silver clusters in aqueous solution become unstable and start to coagulate. Received: 24 June 2002 / Revised version: 25 July 2002 / Published online: 25 October 2002 RID="*" ID="*"This work is part of the thesis of H. M?ltgen RID="**" ID="**"Corresponding author. Fax: +49-211/811-5195, E-mail: kleinermanns@uni-duesseldorf.de     

Narrow-bandwidth diode-laser-based blue and ultraviolet light source

A compact, tunable and narrow-bandwidth laser source for blue and ultraviolet radiation is presented. A grating-stabilized diode laser at 922 nm is frequency-stabilized to below 100 Hz relative to a reference resonator. Injection of the diode-laser light into a tapered amplifier yields a power of 0.5 W. In a first frequency-doubling stage, more than 200 mW of blue light at 461 nm is generated by use of a periodically poled KTP crystal. Subsequent second-harmonic generation employing a BBO crystal leads to about 1 mW of ultraviolet light at 231 nm. Received: 12 August 2002 / Published online: 15 January 2003 RID="*" ID="*"Corresponding author. Fax: +49-89/32905-200, E-mail: christian.schwedes@mpq.mpg.de RID="**" ID="**"Present address: PTB, Bundesallee 100, 38116 Braunschweig, Germany     

A compact frequency-doubled 10-kHz PRF copper-vapour-laser-pumped dye laser

A 10-kHz pulse-repetition-frequency dye-laser master-oscillator power amplifier, end-pumped by a copper vapour laser (CVL), is reported. This laser was based on recently available, lightweight and compact CVL and dye laser components. Dye laser tunability was achieved from 592 to 622 nm and, when the oscillator was etalon line-narrowed, up to 1.5 W of single-etalon-mode output was obtained from the amplifier at the 608-nm peak tuning wavelength. By frequency doubling this amplified output in a BBO crystal we obtained up to 225 mW of 5-GHz 308-nm output, which is suitable for the performance of tropospheric hydroxyl radical concentration measurements. Received: 16 July 2002 / Revised version: 6 November 2002 / Published online: 5 February 2003 RID="*" ID="*"Present address: Department of Geography, University of Cambridge, Cambridge, CB2 3EN, UK RID="**" ID="**"Corresponding author. Fax: +44-1865/272400, E-mail: d.coutts1@physics.ox.ac.uk     

Grooving an alumina surface as a means to inhibit secondary electron emission under grazing incidence

We observe charge multiplication of photoemitted electrons in cylindrical alumina cells, containing cesium vapor, submitted to a longitudinal electric field and to intense laser pulses. We present several diagnoses allowing us to attribute this charge multiplication to efficient secondary electron emission (SEE) from the accelerated photoelectrons colliding with the inner wall at grazing incidence. Machining millimeter-size triangular grooves on the initially smooth inner wall, so as to prevent grazing incidence, is shown to be efficient in reducing SEE. The atomic signal characteristic of the space charge accumulated close to the anode is found to be reduced by more than one order of magnitude. This result is of important significance, not only for our parity-violation experiment in cesium vapor, but also for experiments and techniques involving SEE at grazing incidence. Laboratoire de l’Ecole Normale Supérieure associé au CNRS (UMR 8552) et à l’Université Pierre et Marie Curie. Received: 25 June 2002 / Revised version: 11 September 2002 / Published online: 15 November 2002 RID="*" ID="*"Present address: Institute for Physical Research, Ashtarak-2, 378 410 Armenia. RID="**" ID="**"Corresponding author. Fax: +33-1/4432-3434, E-mail:marianne@lkb.ens.fr     

Coherent coupling of a single <Superscript>40</Superscript>Ca<Superscript>+</Superscript> ion to a high-finesse optical cavity

We demonstrate coherent coupling of the quadrupole S_1/2D_5/2 optical transition of a single trapped ⁴⁰Ca⁺ ion to the standing wave field of a high-finesse cavity. The dependence of the coupling on temporal dynamics and spatial variations of the intracavity field is investigated in detail. By precisely controlling the position of the ion in the cavity standing wave field and by selectively exciting vibrational state-changing transitions the ion’s quantized vibration in the trap is deterministically coupled to the cavity mode. We confirm coherent interaction of ion and cavity field by exciting Rabi oscillations with short resonant laser pulses injected into the cavity, which is frequency-stabilized to the atomic transition. Received: 23 August 2002 / Published online: 8 January 2003 RID="*" ID="*"Corresponding author. E-mail: christoph.becher@uibk.ac.at RID="**" ID="**"Present address: Time and Frequency Division, National Institute of Standards and Technology, Boulder, CO 80305, USA     

Adaptive shaping of two-cycle visible pulses using a flexible mirror

We present a double-pass non-collinear optical parametric amplifier (NOPA) that delivers 4-fs visible–near-infrared pulses. The paper discusses geometrical and temporal properties of the NOPA configuration, which allow us to broaden the gain band of simultaneous parametric amplification in excess of 250 THz. The key elements of the bandwidth enhancement include (i) the use of a broadband second-harmonic pump, (ii) optimization of the incidence angle of all monochromatic spectral components of the pump in order to produce a favorable offset of the corresponding phase-matching curves, and (iii) selection of the chirp rate and time delay between the stretched pump and seed pulses. We next devise a two-stage compressor that incorporates a flexible mirror for adaptive pulse shaping and develop a simple and trustworthy feedback loop based on a one-dimensional spectral measurement. Our rapid numerical algorithm for adaptive control of the flexible membrane is found superior to more complex search routines that are less resistant to the fluctuations of the laser intensity. The automated optimization procedure results in the generation of two-cycle pulses with a carrier wavelength at ∼600 nm. The absence of deep modulation on the parametrically amplified spectrum in combination with the adaptive phase correction lead to a high quality of the temporal profile and allow concentrating 90% of the pulse energy within only a 7.5-fs time window. Received: 8 April 2002 / Revised version: 26 June 2002 / Published online: 25 September 2002 RID="*" ID="*"Present address: Institut für Photonik, Technische Universit?t Wien, Gusshausstrasse 27, 1040 Vienna, Austria RID="**" ID="**"Corresponding author. Fax: +81-3/5841-4165, E-mail: kobayashi@phys.s.u-tokyo.ac.jp     

Orientation studies of Si-phthalocyanine sulfonic acids cast on SiOx substrates

Layers of dihydroxy silicon phthalocyanine tetrasulfonic acid and oligo-μ-oxo silicon phthalocyanine tetrasulfonic acid were prepared by solution-casting methods. The purity of the material was checked by X-ray photoemission spectroscopy. The orientation of the molecules in respect to the substrate plane was investigated by angle-dependent near-edge X-ray absorption fine-structure spectroscopy. The morphology was characterized by atomic force microscopy. Most samples exhibited a significant orientation that was accompanied by crystalline structures; others had no orientation at all with a dominant amorphous morphology. This behavior indicates that several preparation parameters affect the crystallinity and the orientation of the phthalocyanines. Received: 16 January 2002 / Accepted: 11 February 2002 / Published online: 3 May 2002 RID="*" ID="*"Corresponding author. Fax: +1-919/515-7331, E-mail: harald_ade@ncsu.edu RID="**" ID="**"Present address: Southern Illinois University, Physics, Mailcode 4401, Carbondale, IL 62901, USA     

Femtosecond pulsed-laser deposition of BaTiO<Subscript>3</Subscript>

The elemental composition and the surface morphology of thin films grown by laser ablation of barium titanate with femtosecond pulses at 620 nm laser wavelength have been systematically studied according to the experimental pulsed-laser deposition parameters : laser energy density, oxygen pressure, substrate temperature, target–substrate distance and substrate position (in- and off-axis geometry). Firstly, even at high temperature (700 °C), the deposits consist of coalesced particles up to 1-μm in size, mixed in a poorly crystallised tetragonal BaTiO₃ thin film. The particles formed in femtosecond pulsed-laser deposition induce a high surface roughness, which is observed whatever the experimental growth conditions and does not correspond to the droplets often observed during laser ablation in the nanosecond regime. As shown by plasma expansion dynamics, these particles propagate toward the substrate in the plasma plume with a low velocity, and are assumed to be produced by gas-phase reactions. Moreover, the cationic concentration evaluated through the Ba/Ti ratio strongly depends on the oxygen pressure in the ablation chamber and the angular position of the substrate along the normal to the target at laser impact. Indeed, the films appear to be enriched in the heavy element (Ba) when the substrate is located at high angular deviation. This fact is correlated to an increase in the lighter species (i.e. Ti) in the central part of the plasma plume. Received: 30 April 2002 / Accepted: 26 August 2002 / Published online: 8 January 2003 RID="*" ID="*"Corresponding author. Fax: +33-1/4354-2878, E-mail: millon@gps.jussieu.fr RID="**" ID="**"Also at: LSMCL, Université de Metz, 57078 Metz Cedex 3, France     

Fundamentals and advantages of ultrafast micro-structuring of transparent materials

Experimental investigations using femtosecond and picosecond laser pulses at 800 nm illuminate the distinctions between the dynamics and nature of ultrafast processing of dielectrics compared with semiconductors and metals. Dielectric materials are strongly charged at the surface on the sub-ps time scale and undergo an impulsive Coulomb explosion prior to thermal ablation. Provided the laser pulse width remains in the ps or sub-ps time domain, this effect can be exploited for processing. In the case of thermal ablation alone, the high localization of energy accompanied by ultrafast laser micro-structuring is of great advantage also for high quality processing of thin metallic or semiconducting layers, in which the surface charge is effectively quenched. Received: 17 January 2003 / Accepted: 8 February 2003 / Published online: 28 May 2003 RID="*" ID="*"Corresponding author. Fax: +49-30/670-53-500, E-mail: d.ashkenasi@lmtb.dt RID="**" ID="**"Present address: LMTB GmbH, Berlin, Fabeckstr. 60–62, D-14195 Berlin, Germany