Journal of Non-Crystalline Solids 319 (2003) 129135 www.elsevier.

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The interaction of femtosecond and nanosecond laser pulses with the surface of glass
Mohammad R. Kasaai *, Vijayalakshmi Kacham, Francis Theberge, See Leang Chin
Department of Physics, Engineering Physics and Optics and Centre for Optics, Photonics and Laser (COPL), Universit Laval, Quebec City, Que., Canada, G1K 7P4 e Received 9 April 2002; received in revised form 19 September 2002

Abstract The interaction of femtosecond and nanosecond laser pulses with the surface of glass was compared. The glass was placed inside a vacuum chamber. The laser pulses were focused on the glass surface. The morphology of irradiated glass surfaces and of the materials ejected from the surfaces was examined by scanning electron and optical microscopy. During femtosecond laser irradiation, molten material was ejected from the interaction zone on the glass surface. Nanosecond laser pulses (15 mJ/pulse) induced cracks on the surface of glass, whereas the laser with an energy of 8 mJ/ pulse removed a thin layer from the surface through the sputtering process. In the former case, pieces of glass were ejected from the interaction zone, whereas spherical ne powder was produced in the latter case. The femtosecond laser can signicantly localize the damage zone. Interference fringes similar to liquid waves were generated on the surface. This indicates that the glass was melted locally by the femtosecond laser irradiation. Shock waves generated by the nanosecond laser (15 mJ/pulse) caused cracks in the glass. The femtosecond laser has advantages over the nanosecond laser due to the creation of a smaller and more precise hole with lower pulse energy and/or a lower repetition rate. 2002 Elsevier Science B.V. All rights reserved.

1. Introduction The interaction of laser light with the surface of materials yields changes in their physical states or their properties locally. The results obtained from the interaction of short pulses are dierent from those obtained from long pulses [1]. Ultra-short

* Corresponding author. Present address: Acti Lab Pharma, 2245, Chemin Saint-Francois, Dorval, Que., Canada, H9P 1K3. Tel.: +1-514 421 2000; fax: +1-514 421 4434. E-mail address: reza_kasaai@hotmail.com (M.R. Kasaai).

pulsed lasers induced changes in the refractive index of glasses, damage inside the glasses through explosion, compaction and densication processes [211]. Short pulses induced damage on surfaces of materials via heating and ablation processes [12,13]. Melting of semiconductors via non-thermal process [14] and melting of glasses by femtosecond laser pulses [15] have been also reported. We have recently reported [16] the formation of a crystalline phase in the ejected materials during the interaction of amorphous fused silica by femtosecond Tisapphire laser pulses (800 nm, 150 fs, 1 kHz).

0022-3093/03/$ - see front matter 2002 Elsevier Science B.V. All rights reserved. doi:10.1016/S0022-3093(02)01909-9

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Lasers with dierent pulse widths (from nansosecond to femtosecond) induced damage on the surfaces of transparent, ceramic, optical or wide band gap materials through ablation, sputtering or breakdown process. The interaction of picosecond laser pulses with sapphire induced damage on its surface via ablation process [1719]. Nanosecond, picosecond and femtosecond lasers result in breakdown and plasma emission in fused silica and calcium uoride [20,21]. The interaction of picosecond laser with As2 Te3 CaCl2 PbCl2 and Sb2 Se3 BaCl2 PbCl2 glasses induced an-harmonic electron-vibration [22,23]. This eect results in unsymmetrical charge density in the glasses. This eect can be used as a powerful tool for investigation of picosecond IR non-linear optics processes. The glasses can be used as a promising material for picosecond IR laser devices. Long pulses generated by excimer and YAG lasers induced damage in dierent glasses and thin lms via heating and melting processes [2426]. An excimer laser also induced crystallization on thin lms made from amorphous silicon through the melting process [27]. Short pulses caused damage on at silicon target through the heating process [28]. Microsecond and nanosecond lasers induced damage via ablation process and thermal decomposition of aluminum nitride, whereas a nonthermal ablation process occurred without any change in chemical composition of the surface using a femtosecond laser [29]. A nanosecond ultraviolet laser pulses also induced changes in the refractive index of glasses [30,31]. Glasses are the most common optical material and have diverse applications in optics. Glasses are advantageous over other optical materials such as liquid and single crystals because of their availability, cost and interesting properties such as chemical, weather and heat resistance and transparency in the regions of visible and near-infrared light. These characteristics and properties make them an interesting material for optical technology. In addition, the use of glass has raised considerable interest in the investigations of laser material interactions for writing optical wave guides, which have potentials in photonics and telecommunication applications [32,33]. This application is based upon the change in the mor-

phology and properties of the materials in the interaction zones. Studies on the morphology and the properties of the interaction zone help us to understand the mechanism of the interaction. These studies also make a better use of glass devices when they are exposed to the laser light. The morphology of damage induced by femtosecond and nanosecond lasers has studied by many researchers. However, a comparison of surface morphological changes induced by the lasers has not been yet fully investigated. This paper provides: additional information on the morphology of the interaction zones; comparing the morphology of the interaction zones induced by nanosecond and femtosecond lasers; comparing the mechanisms of the interaction processes; and comparing the possibility of cutting thin lms and the creation of micro-holes on the surface of thin lms of ceramic materials such as glasses.

2. Experimental details 2.1. Femtosecond laser beamsurface interaction process A silicate microscopic glass slide with a thickness of 1 mm was placed inside a vacuum chamber (1:0 107 Torr). A femtosecond Tisapphire laser beam (800 nm, 200 fs, 10 Hz) with an energy of 5 mJ/pulse and a beam diameter of 2 cm was focused using a fused silica window with antireection coating onto the surface of the glass and a 15-cm focal length lens. The direction of the incident laser beam was perpendicular to the surface of the glass sample. The sample was translated slowly by hand using a micrometer during the irradiation. The irradiation time was about 5 s. 2.2. Nanosecond laser beamsurface interaction process A fused silica plate with a diameter of 25.4 mm was xed at 5 cm from an antireection-coated window (diameter 50 mm) inside a vacuum chamber. The chamber was rst degassed using a turbo vacuum pump, and the pressure of the chamber before exposing to the laser irradiation

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was set at 1:0 102 mmHg. While the chamber was under vacuum, a nanosecond laser beam (532 nm, 6 ns, 1 kHz) with an energy of 15 mJ/pulse was focused on the surface of the glass using a 10-cm focal length lens. The position of the glass was changed periodically (at $15 s intervals). The total irradiation lasted 2 min. Similar process was performed with an energy of 8 mJ/pulse for a total irradiation time of 60 min. The direction of the incident laser beam was perpendicular to the surface of the glass sample at the two dierent conditions (15 and 8 mJ/pulse). 2.3. Characterization 2.3.1. Optical microscopy (OM) The morphology of the glass surface irradiated by femtosecond laser and of the ejected material, which was obtained from lasersurface interactions, was determined by OM. 2.3.2. Scanning electron microscopy (SEM) The morphology of the irradiated glass surface and of the cross-section of the micro-holes created on the surface by nanosecond laser pulses was measured by a SEM.

Molten materials were ejected from the interaction zone and splashed out on the glass surface around the irradiation regions. Interference fringes between neighboring waves were created (Fig. 2). Fig. 3 shows the irradiated glass surface by nanosecond laser pulses (532 nm, 6 ns, 1 kHz) with a high energy of 15 mJ/pulse. The interaction zone turned into a completely cracked and shattered state. Pieces of glass were collected from the

Fig. 2. OM micrograph of the interference fringes of liquid waves created by femtosecond laser.

3. Results Fig. 1 shows the irradiated glass surface by femtosecond laser pulses (800 nm, 200 fs, 10 Hz).

Fig. 1. OM micrograph of the glass irradiated by femtosecond laser pulses.

Fig. 3. SEM micrograph for irradiated glass surface by nanosecond laser pulses. The energy of the laser pulses was 15 mJ/ pulse.

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Fig. 4. OM micrograph of ejected material in glass pieces form. The energy of nanosecond laser pulses was 15 mJ/pulse.

Fig. 6. SEM micrograph of a cross-section of the irradiated glass surface by nanosecond laser. The energy of the laser pulses was 8 mJ/pulse.

Fig. 5. SEM micrograph for irradiated glass surface by nanosecond laser pulses. The energy of nanosecond laser pulses was 8 mJ/pulse.

Fig. 7. OM micrograph of ejected material in ne powder form. The energy of nanosecond laser pulses was 8 mJ/pulse.

4. Discussion chamber and its optical microscope image is shown in Fig. 4. Fig. 5 shows the irradiated glass surface by nanosecond laser pulses (532 nm, 6 ns, 1 kHz) with a lower energy of 8 mJ/pulse. The cross-section of the interaction zone is shown in Fig. 6. A trace amount of ne powder was collected inside the chamber. The latter was ejected from the interaction zone during the interaction process. Fig. 7 shows the morphology of the ejected powder. The interference created on the surface of irradiated glass is similar to the interference of water waves when circular waves are created on a calm water surface [34]. The results indicate that the glass was melted in the interaction zone during the interaction process. When the laser pulses are stopped or the position of irradiation is changed, local solidication of the melt takes place. However, the solidication of the melt occurs slowly

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due to the low thermal conductivity of the glass. We have recently reported [16] that femtosecond laser with a repetition rate of 1 kHz (800 nm, 150 fs) induced damage on the glass surface via a local melting process. We have earlier reported the relationship between the band gap energy of transparent condensed media and supercontinuum generation [35,36]. During the propagation of a femtosecond laser pulses in a transparent condensed medium, self-focusing of the pulses occurs and results in a strong laser eld. The strong laser eld excites the electrons from the valence to the conduction bands through multiphoton absorption. The laser pulse undergoes self-phase modulation giving rise to a strong blue shift of the frequency. The laser pulse becomes white (supercontinuum) in the forward direction. We observed the emission of white light during the interaction of femtosecond laser pulses with the glass surface under the experimental (800 nm, 200 fs, 10 Hz) and earlier reported conditions (800 nm, 150 fs, 1 kHz) [16]. The facts explained in the above paragraph indicate the following. The non-linear interaction of femtosecond lasers leads to the formation of free electrons by exciting them from the valence to the conduction bands [35,36]. A fraction of the absorbed energy by free electrons was transformed into heat after relaxation. The amount of absorbed energy by the interaction zone would be about 3% of the pulse energy (150 mJ/pulse) [35,36]. The temperature of the irradiated glass increases with the number of pulses. For a sucient number of pulses, the glass will ultimately melt locally. Energy from successive pulses was transferred to the melt and caused splashing a part of the molten material out and produced liquid interference fringes. The rest of the molten material will stay on the glass surface (in the interaction zone) as a pool of liquid that solidies later. It is obvious by comparing Figs. 3 and 4 that melting process has not taken place using such nanosecond pulses. The physical form of the ejected glass pieces obtained from nanosecond laser irradiation is similar to the original glass. The interaction of the laser gives rise to a breakdown plasma and generation of shock wave. Such process was not taken place using femtosecond laser.

The morphology of the irradiated glass with a low energy is dierent from the one obtained with a high energy (see Figs. 3 and 5). The irradiated glass surface obtained from a low energy seems to be the result of the removal of a thin layer from the surface. The physical form of the irradiated glass surface and the formation of the spherical ne powder obtained from a low energy suggest that the laser induced damage through the sputtering process. There was a threshold limit for the energy of the pulses where the interaction of the laser pulses and the glass surface started to occur (about 5 mJ/pulse). Brand and Tam [17] reported that when a sapphire surface was irradiated by picosecond laser pulses (266 nm, 30 ps), material was removed from the surface through the sputtering process. Spherical molten droplets were ejected from the interaction zone, when transparent material surfaces were irradiated by picosecond lasers [17,18]. Kandidov et al. [37] reported that a thin lm was removed from the surface of a glass without melting process, when it was exposed to nanosecond laser irradiation (532 nm, 15 ns). The dimensions of the damage zones induced by nanosecond and femtosecond laser under the current (800 nm, 200 fs, 10 Hz) and previous conditions (800 nm, 150 fs, 1 kHz) [16] are presented in Table 1. The diameter of a micro-hole created by femtosecond laser (Fig. 1) was estimated to be 45 lm, whereas the damage zone induced by nanosecond laser (Figs. 5 and 6) was estimated to be 90 lm. The depth of the microholes created by nanosecond pulses was estimated to be 100 lm (Fig. 6), while the depth of the microhole created by femtosecond laser (800 nm, 150 fs, 1 kHz) [16] was estimated to be 60 lm. With nanosecond laser, the smallest micro-holes that can be created are larger than that created by femtosecond laser. The pulse energy required for nanosecond laser to achieve ablation is much higher than that of femtosecond laser. Femtosecond laser pulses signicantly localized the damage zone compared to nanosecond laser. Thus, femtosecond laser has advantages over nanosecond laser due to the creation of a smaller and more precise hole with a lower energy of pulse and/or a lower repetition rate. In addition, both lasers have potential to cut thin lms made from ceramic

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Table 1 The experimental conditions for the lasersurface interactions and dimensions of the interaction zones Laser Irradiation conditions Wavelength (nm) Femtoseconda Femtosecondb Nanosecondb Nanosecondb
a b

Pulse duration (s) 1:5 1013 2:0 1013 6:0 109 6:0 109

Repetition rate (Hz) 1000 10 1000 1000

Energy (mJ/pulse) 0.5 5.0 8.0 15.0

Exposure time (s) 15 $5 15 15

Principal physical consequence Melting Melting Sputtering Cracking

Dimensions of interaction zones Diameter (lm) 12 3 45 90 15 Depth (lm) 60 100

800 800 532 532

Previous work. This work.

materials such as glasses with similar advantages mentioned above for femtosecond laser. It can be also concluded that the femtosecond laser should be more eective than nanosecond laser in writing a precise wave-guide inside transparent materials with a lower energy of pulse and/or a lower repetition rate based on our previous results [16].

Acknowledgements The authors are grateful to S. Lagac, J.P. e Tremblay and M. Choquette for their assistance with the laser and SEM. We acknowledge the nancial support of Natural Science and Engineering Research Council of Canada (NSERC), the Canadian Institute for Photonic Innovations (CIPI), Fonds pour la Formation de Chercheurs et a lAide  la Recherche (FCAR), Defense a Research Establishement Valcartier (DREV) of Canada and Canada Research Chairs Program. References
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5. Conclusions The interaction of femtosecond and nanosecond laser pulses with the surface of glass was compared. During femtosecond laser irradiation, material was ejected from the interaction zone on the glass surface. Interference fringes similar to liquid waves were formed. Nanosecond laser pulses with an energy of 15 mJ/pulse-induced cracks on the surface of glass and pieces of glass were ejected from the interaction zone. While, nanosecond laser with an energy of 8 mJ/pulse-induced damage on the surface through the sputtering process and ejected spherical ne powder from the interaction zone. Femtosecond laser compared to nanosecond laser can localize the damage zone. The results indicate that the glass was melted locally by femtosecond laser radiation. Shock waves generated by more energetic nanosecond laser caused cracks on the glass surface. Femtosecond laser has advantages over nanosecond lasers due to the creation of a smaller and more precise hole with a lower energy of pulse and/or a lower repetition rate. This can be applied to create microholes on other surfaces of ceramic materials.

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