Towards nanostructuring with femtosecond laser pulses

Detailed investigations of the possibilities for using femtosecond lasers for the nanostructuring of metal layers and transparent materials are reported. The aim is to develop a simple laser-based technology for fabricating two- and three-dimensional nanostructures with structure sizes on the order of several hundred nanometers. This is required for many applications in photonics, for the fabrication of photonic crystals and microoptical devices, for data storage, displays, etc. Measurements of thermionic electron emission from metal targets, which provide valuable information on the dynamics of femtosecond laser ablation, are discussed. Sub-wavelength microstructuring of metals is performed and the minimum structure size that can be fabricated in transparent materials is identified. Two-photon polymerization of hybrid polymers is demonstrated as a promising femtosecond laser-based nanofabrication technology. Received: 20 November 2002 / Accepted: 20 January 2003 / Published online: 28 May 2003 RID="*" ID="*"Corresponding author. Fax: +49-511/2788-100, E-mail: ch@lzh.de     

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     

Efficient submicron processing of metals with femtosecond UV pulses

The generation of submicron-sized holes on metal surfaces by applying femtosecond UV laser pulses was investigated. Different optical schemes based on a Schwarzschild-type reflective objective were used to reach optimized ablation quality and efficiency in different applications (hole ablation, through-hole drilling, generation of surface patterns consisting of holes, etc.). Submicron-sized holes and hole patterns were ablated onto metal surfaces and drilled through ∼5-μm-thick steel foils with 600-nm diameter on the output side. Using a special optical interferometric method, large-area surface processing of high-conductivity materials in the submicron regime was performed. Combining these techniques with the application of high-repetition-rate ultra-short UV laser sources, large-area sub-μm processing of all kinds of materials in industrial environments is possible. Received: 28 February 2002 / Accepted: 12 March 2002 / Published online: 25 October 2002 RID="*" ID="*"Corresponding author. Fax: +49-551/503599, E-mail: psimon@llg.gwdg.de     

Hybrid laser processing for microfabrication of glass

Hybrid laser processing for the precision microfabrication of glass materials, in which the interaction of a conventional pulsed laser beam and a medium on the material surface leads to effective ablation and modification, is reviewed. A major role of the medium is to produce strong absorption of the conventional laser beam by the material. Simultaneous irradiation by a vacuum ultraviolet (VUV) laser beam that possesses an extremely small laser fluence and an ultraviolet (UV) laser greatly improves the ablation quality and modification efficiency for fused silica (VUV-UV multiwavelength excitation process). The metal plasma generated by the laser beam effectively assists high-quality ablation of transparent materials by the same laser beam, resulting in microstructuring, cutting, color marking, printing, and selective metallization of glass materials (laser-induced plasma-assisted ablation (LIPAA)). The detailed discussion presented here includes the ablation mechanism of hybrid laser processing. Received: 18 December 2002 / Accepted: 20 January 2003 / Published online: 28 May 2003 RID="*" ID="*"Corresponding author. Fax: +81-48/462-4682, E-mail: ksugioka@postman.riken.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     

Concatenation of plasma filaments created in air by femtosecond infrared laser pulses

We report the first observation of the attachment of two single plasma filaments created collinearly in the atmosphere by IR femtosecond laser pulses. The linked filamentary structure is electrically conductive and emits sub-THz radiation over its entire length. Concatenation is achieved only for a specific time ordering between the two initial laser pulses. The pulse producing the filament closer to the laser source must be retarded with respect to the other pulse. This special time ordering is attributed to the acceleration of light in a self-guided pulse. Received: 4 March 2003 / Published online: 14 May 2003 RID="*" ID="*"Corresponding author. Fax: +33-1/6931-9996, E-mail: stzortz@ensta.fr     

Measurement of filament length generated by an intense femtosecond laser pulse using electromagnetic radiation detection

We present a new method to measure the length of a filament induced by the propagation of intense femtosecond laser pulses in air. We used an antenna to detect electromagnetic pulses radiated from multipole moments inside the filament oscillating at the plasma frequency. The results are compared with the values detected from the backscattered fluorescence induced by multiphoton ionization of nitrogen molecules excited inside the filament. The values are found to be in good agreement. Received: 6 November 2002 / Revised version: 27 January 2003 / Published online: 24 April 2003 RID="*" ID="*"Corresponding author. Fax: +1-418/656-2623, E-mail: shosseini@phy.ulaval.ca     

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     

High-power laser interactions with nanostructured materials

We use short-pulse high-power lasers to selectively modify the structure of nanolaminates and nanocrystals. It is demonstrated that femtosecond pulses can achieve excellent results for microscopic thin film removal. Laser pulses can also be used to modify the crystal structure of thin films. It is also demonstrated that coherent laser excitation promotes a selective modification of nanocrystals, resulting in changes of size, shape, and crystal structure. Received: 7 October 2002 / Accepted: 20 January 2003 / Published online: 28 May 2003 RID="*" ID="*"Corresponding author. Fax: +1-414/229-5589, E-mail: yakovlev@uwm.edu     

Spatial beam profiles of femtosecond X-ray pulses generated by laser Compton scattering from a low-emittance electron beam

Polarization-dependent spatial beam profiles of femtosecond X-ray pulses generated by a laser Compton scheme were measured. The X-ray pulses were generated by the interaction at an angle of 90° between 100-fs laser light and a 3-ps, 3π-mm mrad electron beam. The polarization of the laser light was linear in two different directions, either parallel or perpendicular to the electron beam axis. The measured profiles showed good agreement with theoretical results. Received: 5 July 2002 / Revised version: 17 October 2002 / Published online: 5 February 2003 RID="*" ID="*"Corresponding author. Fax: +81-424/684477, E-mail: msf_yorozu@shi.co.jp     

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     

Femtosecond waveguide writing: a new avenue to three-dimensional integrated optics

Using tightly focussed femtosecond laser pulses, waveguides can be fabricated inside various glasses and crystals. This technique has the potential to generate not only planar but three-dimensional photonic devices. In this paper we present, to the best of our knowledge, the first true three-dimensional integrated optical device, a 1×3 splitter fabricated in pure fused silica. The optical properties of this device and possibilities for the fabrication of complex high-density integrated optical elements are discussed. Received: 23 December 2002 / Accepted: 6 January 2003 / Published online: 28 March 2003 RID="*" ID="*"Corresponding author. Fax: +49-3641/65-7680, E-mail: nolte@iap.uni-jena.de     

High-power intracavity frequency doubling of a Ti:sapphire femtosecond oscillator

We demonstrate intracavity frequency doubling of a standard femtosecond Ti:sapphire oscillator. The cavity is extended with a pair of focusing mirrors and a 0.5-mm-thick BBO crystal. We achieve a repetition rate of 50 MHz and simultaneously generate 22 mW of 55-fs pulses at 810 nm and 200 mW of 73-fs pulses at 405 nm, which corresponds to 4 nJ per pulse. We create a total of 330-mW, 405-nm light when pumping the Ti:sapphire crystal with 5.7 W from an Ar-ion laser, corresponding to a conversion efficiency of 5.7%. No saturation is found, which implies that higher outputs can be achieved with higher pump rates. Preliminary results from the use of blue pulses as pump in an optical parametric amplifier seeded by pulses from a photonic crystal fiber are presented. Received: 27 January 2003 / Revised version: 27 March 2003 / Published online: 12 May 2003 RID="*" ID="*"Corresponding author. Fax: +45-861/96199, E-mail: tva@chem.au.dk     

Seven-terawatt Ti:sapphire laser system operating at 50 Hz with high beam quality for laser Compton femtosecond X-ray generation

We present a 7-TW Ti:sapphire laser system operating at 50 Hz for laser Compton femtosecond X-ray generation. This laser system delivers 8.4 W of average output power at a repetition rate of 50 Hz with a pulse width of 24 fs. It demonstrates successful management using a dynamically stable resonator in the regenerative amplifier and compensation for thermal lensing by a convex mirror in a ring-type four-pass power amplifier. We also present the results of closed-loop corrections for distorted wavefronts of amplified and compressed laser pulses, using an adaptive optical system consisting of a Shack–Hartmann-type wavefront sensor and a deformable mirror. This closed-loop correction results in dramatic improvements, reducing wavefront distortions below 0.05 λ rms. Received: 31 October 2002 / Revised version: 3 March 2003 / Published online: 5 May 2003 RID="*" ID="*"Corresponding author. Fax: +81-298/61-3349, E-mail: ito@festa.or.jp     

Spectral broadening of 40-fs Ti:sapphire laser pulses in photonic-molecule modes of a cobweb-microstructure fiber

Photonic-molecule modes of a cobweb-microstructure fiber allow efficient nonlinear optical spectral broadening of nanojoule femtosecond light pulses. Spectral widths of approximately 200 nm are achieved at the output of a 6-cm sample of such a fiber for 40-fs Ti:sapphire laser pulses with an energy of a few nanojoules coupled into photonic-molecule modes. Higher values of the group index and a lower group-velocity dispersion, attainable with higher-order photonic-molecule modes, allow the efficiency of spectral broadening of femtosecond laser pulses to be increased relative to the efficiency of spectral broadening in the fundamental photonic-molecule mode. Received: 9 June 2002 / Revised version: 29 June 2002 / Published online: 22 November 2002 RID="*" ID="*"Corresponding author. Fax: +7-095/939-3959, E-mail: zheltikov@top.phys.msu.su     

Practical uses of femtosecond laser micro-materials processing

We describe several approaches to basic femtosecond machining and materials processing that should lead to practical applications. Included are results on high-throughput deep hole drilling in glasses in ambient air, and precision high-speed micron-scale surface modification of composite materials and chalcogenide glasses. Ablation of soda-lime silicate glass and PbO lead-silicate is studied under three different sets of exposure conditions, for which both the wavelength and pulse duration are varied. Ablation rates are measured below and above the air ionization threshold. The differences observed are explained in terms of self-channeling in the ablated hole. Fabrication of practical devices such as waveguides and gratings is demonstrated in chalcogenide glass. Received: 11 December 2002 / Accepted: 20 January 2003 / Published online: 28 May 2003 RID="*" ID="*"Corresponding author. Fax: +1-407/8233-570, E-mail: mrichard@mail.ucf.edu     

Poincaré representation of polarization-shaped femtosecond laser pulses

The usage of Poincaré phase space for the representation of polarization-shaped femtosecond laser pulses is discussed. In these types of light fields the polarization state (i.e. ellipticity and orientation) changes as a function of time within a single laser pulse. Such deliberate variation can be achieved by frequency-domain femtosecond pulse shaping in which two polarization components are manipulated individually. Here it is shown how these light pulses can be represented as temporal trajectories through the ellipticity-orientation (Poincaré) phase space, whereas conventional light (either continuous-wave or pulsed) is determined by only one specific Poincaré location. General properties of parametric Poincaré trajectories are discussed, and their relation to experimentally accessible pulse-manipulation parameters (i.e. amplitudes and phases) determined. Specifically, it is shown how the maximum rate by which a given polarization state can be turned into a different one (at significant intensity levels) is limited by the spectral laser bandwidth. Apart from their direct usage in polarization-shaped pulse representation, Poincaré trajectories also form the basis for intuitive quasi-three-dimensional renderings of the electric field profile. There, the temporal evolution of polarization, intensity, and chirp is directly apparent in a single illustration. Received: 10 December 2002 / Published online: 24 April 2003 RID="*" ID="*"Corresponding author. Fax: +49-931/888-4906, E-mail: brixner@physik.uni-wuerzburg.de     

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     

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     

Morphology studies of the metal surfaces with enhanced absorption fabricated using interferometric femtosecond ablation

Recently, the enhancing of bulk metals optical absorption with focused femtosecond pulses was demonstrated. This absorption enhancement is caused by different nano- and micro-structures which are formed during laser ablation with ultrashort pulses. In this paper we study the evolution of the surface structures using interferometric ablation and compare it to normal fs-ablation. Previously we have shown that interferometric femtosecond ablation is an efficient method to fabricate absorbing metal surfaces. In this study we ablated large areas of hole-array structures with different pulse numbers in polished stainless steel and copper samples. The evolution of surface morphology and the depth of the holes for these structured surfaces are presented. In addition, the reflectance of laser generated surface structures are measured at the wavelength range of 200–2300 nm using a standard spectrophotometer.