Damage performance of TiO2/SiO2 thin film components induced by a long-pulsed laser

In order to study the long-pulsed laser induced damage performance of optical thin films, damage experiments of TiO₂/SiO₂ films irradiated by a laser with 1 ms pulse duration and 1064 nm wavelength are performed. In the experiments, the damage threshold of the thin films is measured. The damages are observed to occur in isolated spots, which enlighten the inducement of the defects and impurities originated in the films. The threshold goes down when the laser spot size decreases. But there exists a minimum threshold, which cannot be further reduced by decreasing the laser spot size. Optical microscopy reveals a cone-shaped cavity in the film substrate. Changes of the damaged sizes in film components with laser fluence are also investigated. The results show that the damage efficiency increases with the laser fluence before the shielding effects start to act.     

Microfabrication of gold dots in SiO2/TiO2 glass films by two-photon absorption

Photogeneration of Au nanoparticles in SiO₂/TiO₂ glass films was carried out by two-photon absorption with a femtosecond pulse laser. Exquisite microdot-arrays of Au with micrometer spatial resolution were achieved by scanning of the focused laser beam. These structures were constructed in SiO₂/TiO₂ glass films by a sol–gel method. The sol–gel method demonstrated that Au dots microarray are fabricated at any position by two-photon absorption in the glass. The results show the utility of a two-photon absorption technique in the fabrication of complicated patterns with metal particles.     

F2 laser induced oxidation of inorganic material

Transparent SiO₂ thin films were selectively fabricated on Si wafer by 157 nm F₂ laser in N₂/O₂ gas atmosphere. The F₂ laser photochemically produced active O(¹D) atoms from O₂ molecules in the gas atmosphere; strong oxidation reaction could be induced to fabricate SiO₂ thin films only on the irradiated areas of Si wafer. The oxidation reaction was sensitive to the single pulse fluence of F₂ laser. The irradiated areas were swelled and the height was approximately 500-1000 nm at the 205-mJ/cm² single pulse fluence for 60 min laser irradiation. The fabricated thin films were analytically identified to be SiO₂ by the Fourier-transform IR spectroscopy. The SiO₂ thin films could be also removed by subsequent chemical etching to fabricate micro-holes 50 nm in depth on Si wafer for microfabrication.     

Different crystallization processes of as-deposited amorphous Ge2Sb2Te5 films on nano- and picosecond single laser pulse irradiation

The crystallization dynamics of as-deposited amorphous Ge₂Sb₂Te₅ films induced by nano- and picosecond single laser pulse irradiation is studied using in situ reflectivity measurements. Compared with nanosecond laser pulse, the typical recalescence phenomenon did not appear during the picosecond laser pulse-induced crystallization processes when the pulse fluence gradually increased from crystallization to ablation threshold. The absence of melting and recalescence phenomenon significantly decreased the crystallization time from hundreds to a few tens of nanoseconds. The role of pulse duration time scale on the crystallization process is qualitatively analyzed.     

Morphology and composition on Al surface irradiated by femtosecond laser pulses

We study the surface chemicals and structures of aluminum plates irradiated by scanning femtosecond laser pulses in air for a wide range of laser fluence from 0.38 to 33.6 J/cm². X-ray photoelectron spectroscopy and X-ray diffraction analyses indicate clearly that crystalline anorthic Al(OH)₃ is formed under femtosecond laser pulse irradiation. Besides aluminum hydroxide, crystalline Al₂O₃ is also found in the samples irradiated at high laser fluence. Field emission scanning electron microscopy demonstrates that the surfaces of the samples irradiated with low laser fluence are colloidal-like and that nanoparticles with a few nanometers in size are embedded in glue-like substances. For high laser fluence irradiated samples, the surfaces are highly porous and covered by nanoparticles with uniform size of less than 20 nm.     

Control of electrical resistance of TiO2 films by short-pulse laser irradiation

Titanium dioxide (TiO₂) films were irradiated with a femtosecond laser beam to alter their electrical resistances. The TiO₂ film was produced by aerosol beam deposition. The wavelength, pulse duration, and repetition rate of the femtosecond laser scanned across the sample surface were 800 nm, 100 fs, and 1 kHz, respectively. By attenuating the laser fluence on the TiO₂ film, a range was found in which the electrical resistance of the TiO₂ film was varied even though the morphology of the film surface was not changed.     

308nm激光作用下V2O5非晶薄膜的变异

研究了在308nm准分子激光辐照下，V₂O₅非晶薄膜性质的变化-利用X射线衍射、X射线光电子能谱及扫描电子显微镜等多种测试方法进行了分析比较，确定V₂O₅非晶薄膜性质的变化是由于高功率密度的准分子激光作用，造成V₂O₅薄膜的快速升温熔化和快速冷凝重构，使其中的氧产生缺位，引起化学配比偏离所致- 关键词：     

Femtosecond laser ablation of crystals SiO2 and YAG

Damage threshold of crystals SiO₂ and YAG against 60-900 fs, 800 nm laser pulses are reported. The breakdown mechanisms were discussed based on the double-flux model and Keldysh theory. We found that impact ionization plays the important role in the femtosecond laser-induced damage in crystalline SiO₂, while the roles of photoionization and impact ionization in YAG crystals depend on the laser pulse durations.     

Surface texturing of Si, porous Si and TiO2 by laser ablation

Excimer laser ablation at 308 nm has been used to texture the surfaces of a variety of materials of interest for optoelectronic and biotechnological applications. Using a range of pre- and post-processing methods, we are able to produce nano-, micro- and meso-scale features over large areas rapidly in materials such as crystalline Si, porous silicon and TiO₂. Texturing of porous silicon leads to the growth of crystalline dendritic structures, which distinguishes them dramatically from the conical pillars formed from crystalline silicon. Regular arrays of Si microdots are formed by irradiating a Si surface pre-covered with a Cr thin film grating. Nano-crystalline porous TiO₂ films are easily ablated or compacted with laser irradiation. However, at low enough laser fluence, surface roughening without complete loss of porosity is possible.     

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.     

Analyses of surface coloration on TiO2 film irradiated with excimer laser

TiO₂ film of around 850 nm in thickness was deposited on a soda-lime glass by PVD sputtering and irradiated using one pulse of krypton-fluorine (KrF) excimer laser (wavelength of 248 nm and pulse duration of 25 ns) with varying fluence. The color of the irradiated area became darker with increasing laser fluence. Irradiated surfaces were characterized using optical microscopy, scanning electron microscopy, Raman spectroscopy and atomic force microscopy. Surface undergoes thermal annealing at low laser fluence of 400 and 590 mJ/cm². Microcracks at medium laser fluence of 1000 mJ/cm² are attributed to surface melting and solidification. Hydrodynamic ablation is proposed to explain the formation of micropores and networks at higher laser fluence of 1100 and 1200 mJ/cm². The darkening effect is explained in terms of trapping of light in the surface defects formed rather than anatase to rutile phase transformation as reported by others. Controlled darkening of TiO₂ film might be used for adjustable filters.     

SEM/TEM characterization of periodical novel amorphous/nano-crystalline micro-composites obtained by laser interference structuring: The system HAlO-Al·Al2O3

Layers of the metastable, amorphous HAlO are synthesized by chemical vapor deposition from the molecular compound tert-butoxyalane ([^tBu-O-AlH₂]₂). At temperatures above 500 °C, these layers transform to biphasic Al·Al₂O₃ due to the elimination of di-hydrogen. The interaction of HAlO films with short laser pulses causes partial transformation of amorphous HAlO into nano-crystalline Al·Al₂O₃. Using an interference pattern of two coherent high-power Nd:YAG laser beams produces local and periodic heating, inducing crystallization at equally distant lines in the HAlO layer. Depending on the laser fluence, different morphologies and different amounts of crystalline phases are obtained. In this study, the surface morphology and the distribution of crystalline phases of the structured samples are analyzed using SEM, FIB and TEM. The two-dimensional structures consist of periodic variations of morphology, chemical composition, and phase identity with a well-defined long-range order. When bio-functionalized, the structured samples may be used as carriers for structurally controlled cell-cultivation.     

Effect of CO2 laser-pulse mode quality on multiple photon absorption in SF6

Unimolecular multiple-photon absorption cross sections are measured for SF₆ for both single and multiple longitudinal mode CO₂ laser pulses at three different frequencies over a four-decade range of energy fluence. The results indicate only a weak dependence on pulse mode structure for fluence levels corresponding to as little as 0.02 photons absorbed per molecule.     

Femtosecond laser patterning of Ta0.1W0.9Ox/ITO thin film stack

Selective laser patterning of thin films in a multilayered structure is an emerging technology for process development and fabrication of optoelectronics and microelectronics devices. In this work, femtosecond laser patterning of electrochromic Ta_0.1W_0.9O_x film coated on ITO glass has been studied to understand the selective removal mechanism and to determine the optimal parameters for patterning process. A 775 nm Ti:sapphire laser with a pulse duration of 150 fs operating at 1 kHz was used to irradiate the thin film stacks with variations in process parameters such as laser fluence, feedrate and numerical aperture of objective lens. The surface morphologies of the laser irradiated regions have been examined using a scanning electron microscopy and an optical surface profiler. Morphological analysis indicates that the mechanism responsible for the removal of Ta_0.1W_0.9O_x thin films from the ITO glass is a combination of blistering and explosive fracture induced by abrupt thermal expansion. Although the pattern quality is divided into partial removal, complete removal, and ITO film damage, the ITO film surface is slightly melted even at the complete removal condition. Optimal process window, which results in complete removal of Ta_0.1W_0.9O_x thin film without ablation damage in the ITO layer, have been established. From this study, it is found that focusing lens with longer focal length is preferable for damage-free pattern generation and shorter machining time.     

Manufacturing of Nd:Gd3Ga5O12 ridge waveguide lasers by pulsed laser deposition and ultrafast laser micromachining

Laser radiation is used both for the deposition of the laser active thin films and for the micro structuring to define wave guiding structures for the fabrication of waveguide lasers. Thin films of crystalline and amorphous neodymium doped Gd₃Ga₅O₁₂ are grown on single crystal yttrium aluminium garnet by pulsed laser deposition using excimer laser radiation.Manufacturing of the laser active waveguides by micro structuring is done using femtosecond laser ablation of the deposited films. The structural and optical properties of the films and the morphology of the structured waveguides are determined in view of the design and the fabrication of compact and efficient diode pumped waveguide lasers. The resulting waveguides are polished, provided with resonator mirrors, pumped using diode lasers and the waveguide lasers are characterized. The spectroscopic properties of the amorphous waveguide are investigated and an infrared waveguide laser is demonstrated. To our knowledge, there have been no reports by other groups of the successful operation of a structured waveguide laser fabricated by this technique or of a waveguide laser made from amorphous neodymium doped Gd₃Ga₅O₁₂.     

Ta2O5 thin-films deposited by off-axis and on-axis pulsed laser deposition techniques

The crystalline properties of Ta₂O₅ thin films deposited by an off-axis aperture-installation-type pulsed laser deposition technique are investigated and the results are compared with the results for films deposited by the conventional on-axis technique. No significant difference in the substrate temperature dependence is seen between films deposited on-axis or off-axis at a pulse repetition frequency of 30 Hz. When the repetition frequency is lowered, the degree of c-axis orientation is increased in both films. This tendency is more pronounced in the off-axis films. Therefore it is found that the off-axis aperture-installation-type pulsed laser deposition technique is effective not only for decreasing the density of droplets, but also for obtaining more highly c-axis-oriented crystalline films.     

Guidelines for efficient direct ablation of dielectrics with single femtosecond pulses

We provide guidelines to femtosecond laser users to select ad hoc laser parameters, namely the fluence and pulse duration, in the context of the development of ablation processes at the surface of dielectrics using single femtosecond pulses. Our results and discussion are based on a comprehensive experimental and theoretical analysis of the energy deposition process at the surface of fused silica samples and of their postmortem ablation characteristics, in the range of intensities from 10¹³ to 10¹⁵ W/cm². We show experimentally and numerically that self-induced plasma transient properties at the pulse timescale dramatically determine the efficiency of energy deposition and affect the resulting ablation morphology. In practice, we determine that the precise measurement of two characteristic fluence values, namely the laser-induced ablation threshold F _th,LIAT and the fluence F _opt for maximum ablation efficiency, are only required to qualify the outcomes of laser ablation at the surface of a dielectric in an extended range of applied fluence.     

Growth of oriented Pb(ZrxTi1-x)O3 thin films on glass substrates by pulsed laser deposition

Oriented crystalline Pb(Zr_xTi_1-x)O₃ (x=0.53) (PZT) thin films were deposited on metallized glass substrates by pulsed laser deposition (1060-nm wavelength Nd:YAG laser light, 10-ns pulse duration, 10-Hz repetition rate, 0.35-J/pulse and 25-J/cm² laser fluence), from a commercial target at substrate temperatures in the range 380-400 °C. Thin films of 1-3 7m were grown on Au(111)/ Pt/NiCr/glass substrates with a rate of about 1 Å/pulse on an area of 1 cm². The deposited PZT films with perovskite structure were oriented along the (111) direction, as was revealed from X-ray diffraction spectra. Fourier transform infrared spectroscopy (FTIR) was performed on different PZT films so that their vibrational modes could be determined. Piezoelectric d₃₃ coefficients up to 30 pC/N were obtained on as-deposited films. Ferroelectric hysteresis loops at 100 Hz revealed a remanent polarization of 20 7C/cm² and a coercive field of 100 kV/cm.     

Pulsed laser deposition of Bi2Te3 thermoelectric films

Bi₂Te₃ is one of the most used materials for thermoelectric applications at ambient temperature. An improvement of thermoelectric performances through a suitable modification of electron and phonon transport mechanisms is predicted for low dimensional or nanostructured systems, but this requires a control of the material structure down to the nanoscale. We show that pulsed laser deposition provides control on film composition, phase and structure, necessary for a comprehension of the relationship between structure and thermoelectric properties. We have explored the role of deposition temperature, background inert gas type and pressure, laser fluence and target-to-substrate distance and we found the experimental condition ranges to obtain crystalline films containing the Bi₂Te₃ phase only, by comparing energy dispersive X-ray spectroscopy, Raman spectroscopy and X-ray diffraction analysis. Variations of substrate temperature and deposition gas pressure prove to be crucial also for the control of film morphology and crystallinity. Substrate type has no influence on film stoichiometry and crystallinity, but highly oriented growth can be achieved on mica due to van der Waals epitaxy.     

Light-induced ultrafast phase transitions in VO2 thin film

Vanadium dioxide shows a passive and reversible change from a monoclinic insulator phase to a metallic tetragonal rutile structure when the sample temperature is close to and over 68 °C. As a kind of functional material, VO₂ thin films deposited on fused quartz substrates were successfully prepared by the pulsed laser deposition (PLD) technique. With laser illumination at 400 nm on the obtained films, the phase transition (PT) occurred. The observed light-induced PT was as fast as the laser pulse duration of 100 fs. Using a femtosecond laser system, the relaxation processes in VO₂ were studied by optical pump-probe spectroscopy. Upon a laser excitation an instantaneous response in the transient reflectivity and transmission was observed followed by a relatively longer relaxation process. The alteration is dependent on pump power. The change in reflectance reached a maximum value at a pump pulse energy between 7 and 14 mJ/cm². The observed PT is associated with the optical interband transition in VO₂ thin film. It suggests that with a pump laser illuminating on the film, excitation from the d_θ,? - state of valence band to the unoccupied excited mixed d_θ,?-π* - state of the conduction band in the insulator phase occurs, followed by a resonant transition to an unoccupied excited mixed d_θ,?-π* - state of the metallic phase band.