Sub-picosecond UV-laser ablation of Ni films

Laser ablation of thin Ni films on fused silica by 0.5 ps KrF-excimer-laser pulses at 248 nm is reported. The onset of material removal from different film thicknesses (0.1, 0.3, 0.6 and 1.0 m) was measured in a laser ionization time-of-flight mass spectrometer by the amount of Ni atoms vs laser fluence. Significant amounts of metal atoms are already evaporated at laser fluences around 20 mJ/cm², a threshold up to 100 times smaller compared to the one for 14 ns pulses. In contrast to ns laser pulses, the ablation threshold for 0.5 ps pulses is independent of the film thickness. These results reflect the importance of thermal diffusion in laser ablation of strongly absorbing and thermally good conducting materials and prove that for ablation with short pulses, energy loss to the bulk is minimized.     

Influence of film thickness on laser ablation of hydrogenated amorphous carbon films

Single-pulse damage thresholds of hydrogenated amorphous carbon (a-C:H) films were measured for 8-ns laser pulses at 532-nm wavelength. Layer thicknesses from below the optical penetration depth to above the thermal diffusion length (60 nm–13 μm) were examined. After correction of the damage-threshold values for the fraction of energy effectively absorbed by the material, the damage threshold was found to increase linearly with the layer thickness, also for film thicknesses below the optical penetration depth of a-C:H. The threshold fluence reached the bulk value for a layer thickness equal to the thermal diffusion length. The thermal diffusion coefficient was obtained from fitting the experimental data. Several phenomena like graphitization, blistering, exfoliation, and ablation were observed for different fluence regimes and film thicknesses. PACS 79.20.Ds; 06.60.Jn; 78.66.Jg     

Influence of thermal diffusion on the laser ablation of thin polymer films

The laser ablation of a photosensitive triazene polymer was investigated with a ns XeCl excimer laser over a broad range of thicknesses (10–400 nm). We found that the ablation threshold fluence increased dramatically with decreasing film thickness for films thinner than 50 nm. Ablation on substrates with different thermal properties (sapphire, fused silica, PMMA) was investigated as well, and a clear influence of the substrate material was obtained. A mathematical model combining thermal diffusion and absorption effects was used to explain the experimental data. The model is in good agreement with the experimental data and shows that heat diffusion into the substrate plays a crucial role for the ablation process of very thin films. PACS 52.38.Mf; 44.05.+e; 81.05.Lg     

UV-laser ablation of ductile and brittle metal films

Single-shot laser damage of Ni and Cr films on fused silica substrates has been studied as a function of film thickness, utilizing 248 nm/14 ns pulses and detection by probe beam deflection. Threshold fluences for visible damage and vaporization are compared to predictions of the heat diffusion model. The model fits thresholds for visible damage well and identifies their origin, which is melting for Ni films and brittle-to-ductile phase transition for Cr films. When predicting thresholds for vaporization, the diffusion model is of limited success in case of Ni films but fails completely for Cr films, indicating that transient thermal properties of the material should be taken into account. Microscopic inspection shows that Cr films rupture at low fluences before entering the common sequence of melting and vaporizing with increasing fluence. 17 December 1996/Accepted: 17 December 1996     

355 nm nanosecond pulsed Nd:YAG laser profile measurement, metal thin film ablation and thermal simulation

Laser ablation of nickel, gold and copper thin film on glass substrates has been investigated using a nanosecond pulsed Nd:YAG laser operating at 355 nm in air with a Gaussian intensity profile. The exact beam profile was measured through mechanical scanning with a photodiode. A small beam defect was observed, which can affect the machining performance at higher pulse energies. The ablation thresholds of the films were calculated from the crater diameter values. The effect of the pulse repetition rate and the film thickness was also studied. At high pulse repetition rates heat accumulation was observed and the ablation threshold decreased with the film thickness. Both cases resulted in higher diameters.     

Comparison of the transmission behavior of a triazeno-polymer with a theoretical model

The threshold fluence,F _Th, of ablation of a triazeno-polymer was measured in the low fluence range for thin films using conventional UV-spectroscopy. It was found that there is a clearly definedF _Th for 308 nm irradiation between 20 and 25 mJ cm^–2. In the case of 248 nm irradiation, a threshold fluence range between 16 and 32 MJ cm^–2 was found. The ablation rate for both irradiation wavelengths depends on film-thickness. For the XeCl excimer-laser, the point at which the rate becomes independent of thickness was observed to lie at a value which did not correspond to the calculated laser penetration depth, whereas for the KrF laser the independence was not reached within the applied thickness range (up to 0.35 m). Additional transmission measurements have been performed showing that the target transmission at 248 nm increases only slightly, whereas for 308 nm the transmission increases by a factor of approximately 4. This result shows that dynamic target absorption properties are very important for describing the ablation process. The results derived from the transmission studies and etch rates were analyzed theoretically with a two-level model of chromophore absorption. For 248 nm irradiation this model can describe the transmission behavior and the ablation rate. In the case of 308 nm irradiation, it was only possible to match one data set. A good agreement with the experimental transmission ratio does not match the ablation rate and vice versa.     

Single-shot ablation threshold of chromium using UV femtosecond laser pulses

Single-shot ablation threshold for thin chromium film was studied using 266 nm, femtosecond laser pulses. Chromium is a useful material in the nanotechnology industry and information on ablation threshold using UV femtosecond pulses would help in precise micromachining of the material. The ablation threshold was determined by measuring the ablation crater diameters as a function of incident laser pulse energy. Absorption of 266 nm light on the chromium film was also measured under our experimental conditions, and the absorbed energy single-shot ablation threshold fluence was \(46 \pm 5\)  mJ/cm². The experimental ablation threshold fluence value was compared to time-dependent heat flow calculations based on the two temperature model for ultrafast laser pulses. The model predicts a value of 31.6 mJ/cm² which is qualitatively consistent with the experimentally obtained value, given the simplicity of the model.     

Enhancement and band distortion of the IR absorption spectra of a methanol on silver evaporated thin films in UHV-ATR configuration

Enhanced infrared absorption spectra of methanol adsorbed on evaporated silver films were measured using Kretschmanns ATR configuration. Whereas the enhanced spectra were recordable using p-polarized radiation alone when the metal film was continuous, it was obtainable using both the p-polarized and s-polarized radiations from island films. Band distortion was also measured for changing incident angle and metal thickness. Furthermore, when film with silver of intermediate thickness was used, great distortion of the absorption band was observed. The relation between the anomalous absorption by the silver film and the band distortion was indicated.     

Femtosecond laser interaction with pulsed-laser deposited carbon thin films of nanoscale thickness

The dependence of optical, electronic and thermal penetration zones on the thickness of nanoscale layers grown on silicon wafers is reported. Tetrahedral amorphous carbon (ta-C) and amorphous carbon nitride (a-C_xN_y) films were prepared by inverse pulsed laser deposition (IPLD). Single-pulse modification thresholds for femtosecond laser processing proved to be dependent on the actual film thickness below 60 nm for ta-C and 90 nm for a-C_xN_y. The modification behaviour was governed by multiphoton processes. An effective penetration depth of the laser radiation in a-C_xN_y was of ca. 110 nm in accordance with two-photon absorption. Both the emergence length of ballistic hot electrons and the heat diffusion length are negligible in these thin film materials. The lower bulk value of the threshold fluence of the a-C_xN_y films as compared to ta-C is mainly controlled by optical contributions due to nitrogen-related defects.     

Incubation effect and its influence on laser patterning of ITO thin film

Results are presented on the surface damage thresholds of ITO thin films induced by single- and multi-pulse laser irradiation at a pulse duration of 10 ps and a wavelength of 1064 nm. For multi-pulse ablation the incubation effect results in a reduction of the damage threshold, especially apparent at low pulse numbers and very small film thicknesses. The incubation effect attributes to the accumulation of defect sites and/or the storage of thermal stress-strain energy induced by the incident laser pulses. An incubation coefficient of S=0.82 has been obtained which is independent on the film thickness in the range of 10–100 nm. In practical applications, the incubation effect determines the laser patterning structure of ITO films while increasing the pulse overlapping rate. The width of the patterned line can be predicted by the proposed model involving the laser fluence, the overlapping rate and the incubation coefficient.     

Nanometer-microscopy of the electron transmission through an ultrathin (3–22 nm) Au film and of the Au-Si schottky barrier height

Direct imaging with nanometer scale resolution of the Schottky barrier height and of the ballistic transmission of electrons through an ultrathin metal film is demonstrated for the first time. The images are obtained by applying a new pixel-by-pixel evaluation method to the ballistic electron emission spectroscopy (BEES). We find a laterally uniform Schottky barrier height _B=0.88 eV for ultrathin (3–22 nm) Au films evaporated on Si. The transmission coefficient is strongly correlated with the island structure of the Au film. A transmission decay length =14 nm is determined by a statistical analysis of the transmission coefficient with variation of the film thickness.     

Nanosecond surface interferometry measurements on designed and commercial polymers

The effect of the ablation mechanism on surface morphology changes during an ablation process was studied by comparing three different polymers: a triazene polymer, a polyimide and poly(methylmethacrylate) (PMMA) with nanosecond surface interferometry. The triazene polymer, for which only indications for a photochemical ablation mechanism had been detected in previous studies, revealed no surface swelling, which could be attributed to a thermal ablation mechanism. For polyimide, a photothermal ablation mechanism is usually used to describe the ablation process at irradiation wavelengths 248 nm. However, the interferometric measurements do not show any surface swelling, which would be a clear indication for a thermal ablation mechanism. A surface swelling was only detected for PMMA with irradiation at 248 nm and fluences below the threshold of permanent surface modification. The detected phase shift, which is proportional to the change of the film thickness and the refractive index, can be explained by the opposite signs of the thermal expansion coefficient and the thermal refractive-index coefficient. PACS 52.38.Mf; 42.87.Bg; 71.20.Rv     

Electrical and switching properties of the Se90Te10−xAgx (0?x?6) films

Amorphous Se₉₀Te_10−xAg_x (0?x?6) films are obtained by thermal evaporation technique under vacuum from the synthesized bulk materials on pyrographite and glass substrates. X-ray analysis shows the amorphous nature of the obtained films. The dc electrical conductivity was studied for different thicknesses (165-711 nm) as a function of temperature in the range (298-323 K) below the corresponding T_g for the studied films. The obtained results show that the conduction activation energy has a single value through the investigated range of temperature which can be explained in accordance with Mott and Davis model. The I-V characteristic curves for the film compositions are found to be typical for a memory switch. The mean value of the threshold voltage increases linearly with increasing film thickness (165-711 nm), while it decreases exponentially with increasing temperature in the investigated range for the studied compositions. The results are explained in accordance with the electrothermal model for the switching process. The effect of Ag on the studied parameters is also investigated.     

Effect of physical ageing in thin glassy polymer films

We have studied the effect of physical ageing in thin supported glassy polystyrene films by using ellipsometry to detect overshooting in the expansivity-temperature curve upon heating of aged samples. Films with thickness 10-200 nm have been aged at 70^° C and 80^° C (below the bulk glass transition temperature). We observe clear relaxation peaks in the expansivity-temperature curve for films thicker than 18 nm but not for the 10 nm film. The intensity of the relaxation peak is inversely proportional to the film thickness, while the temperatures characteristic to the relaxation peak are almost independent of the film thickness. These observations are successfully interpreted by the idea that the surface layer of the order of 10 nm has liquid-like thermal properties. Received 28 October 2002 / Published online: 1 April 2003 RID="a" ID="a"Present address: Yokohama Research Center, Mitsubishi Chemical Corporation, 1000 Kamoshida-chou, Aoba-ku, Yokohama 227-8502, Japan; e-mail: kawana@rc.m-kagaku.co.jp     

1 064 nm激光对氧化铟锡薄膜的损伤研究

 液晶光学器件在激光光束精密控制上具有重要应用前景,氧化铟锡（ITO）薄膜作为液晶光学器件的透明导电电极,是液晶器件激光损伤的薄弱环节。为此,建立了ITO薄膜激光热损伤物理模型。理论计算结果表明：1 064 nm激光对ITO薄膜的损伤主要为热应力损伤;连续激光辐照下,薄膜损伤始于靠近界面的玻璃基底内;脉冲激光辐照下,温升主要发生在光斑范围内的膜层,薄膜损伤从表面开始。利用泵浦探测技术,研究了ITO薄膜的损伤情况,测量了不同功率密度激光辐照后薄膜的方块电阻,结合1-on-1法测定了ITO薄膜的50%损伤几率阈值。实验结果表明：薄膜越厚,方块电阻越小,激光损伤阈值越低;薄膜未完全损伤前,方块电阻随激光功率密度的增加而增大。理论计算与实验结果吻合较好。设计液晶光学器件中的ITO薄膜电极厚度时,应综合考虑激光损伤、透光率及薄膜电阻的影响。     

Processing of W/Si and Si/W bilayers and multilayers with single and multiple excimer-laser pulses

Interdiffusion phenomena, thermal damage and ablation of W/Si and Si/W bilayers and multilayers under XeCl-excimer laser (=308 nm) irradiation at fluences of 0.15, 0.3 and 0.6 J/cm² were studied. Samples were prepared by UHV e-beam evaporation onto oxidized Si. The thickness of W and Si layers and the total thickness of the structures were 1–20 nm and 40–100 nm, respectively. 1 to 300 laser pulses were directed to the same irradiation site. At 0.6 J/cm² the samples were damaged even by a single laser pulse. At 0.3 J/cm² WSi₂ silicide formation, surface roughening and ablation were observed. The threshold for significant changes depends on the number of pulses: it was between 3–10 pulses and 10–30 pulses for bilayers with W and Si surfaces, respectively, and more than 100 pulses for multilayers with the same total thickness of tungsten. At 0.15 J/cm² the periodicity of the multilayers was preserved. Temperature profiles in layered structures were obtained by numerical simulations. The observed differences of the resistance of various bilayers and multilayers against UV irradiation are discussed.     

Optical properties of nickel(II)-azo complexes thin films for potential application as high-density recordable optical recording media

Smooth thin films of three kinds of nickel(II)-azo complexes were prepared by the spin-coating method. Absorption spectra of the thin films on K9 glass substrate in the 300-600 nm wavelength region were measured. Optical constants (complex refractive index ) and thickness of the thin films prepared on single-crystal silicon substrate in the 300-600 nm wavelength region were investigated on rotating analyzer-polarizer type of scanning ellipsometer, and dielectric constants , absorption coefficients α as well as reflectance R of thin films were then calculated at 405 nm. In addition, in order to examine the possible use of nickel(II)-azo complex thin film as an optical recording medium, one of the nickel(II)-azo complex thin film prepared on K9 glass substrate with an Ag reflective layer was also studied by atomic force microscopy and static optical recording. The results show that the nickel(II)-azo complex thin film is smooth and has a root mean square surface roughness of 2.25 nm, and the recording marks on the nickel(II)-azo complex thin film are very clear and circular, and their size can reach 200 nm or less.     

Threshold behavior in polyimide photoablation: Single-shot rate measurements and surface-temperature modeling

The ablation rate of Kapton-type polyimide has been measured as a function of incident fluence and excimer laser wavelength using a sensitive quartz-crystal microbalance (QCM). The experiments were performed such that the fluence and the ablated depth were known for each laser pulse, avoiding the need to average rate and fluence data over many pulses. By limiting the investigations to the low-fluence regimes near ablation threshold, high precision and detailed curve shapes were obtained. It was found that the ablation rate increases smoothly and exponentially with increasing fluence for 248, 308, and 351 nm wavelengths. This exponential behavior was modeled using an Arrheniustype thermal rate equation. In contrast, the 193 nm curve is linear in fluence, displays a sharp threshold, and is consistent with a possible photochemical ablation mechanism. Using a sophisticated surface temperature modeling code, the maximum laser induced surface temperature at the fluence at which ablation can first be detected is found to be the same, 850° C, for all four wavelengths. This ablation temperature is significantly higher than the approximately 500° C temperature at which Kapton starts to degrade under isothermal heating conditions.     

Thermal diffusivity measurements of thin films with a pyroelectric calorimeter

The use of pyroelectric polyvinylidene fluoride calorimeters for the measurement of thermal diffusivities of thin films is described. The potential of this detection scheme combined with photothermal excitation is demonstrated on polymer films with thickness in the 1 m range.     

Direct observation of laser-induced crystallization of a-C:H films

The post-growth modification of diamond-like amorphous hydrogenated carbon a-C:H films by laser treatment has been studied by transmission electron microscopy and Raman spectroscopy. a-C:H films grown on Si substrates by benzene decomposition in a rf glow discharge were irradiated with 15 ns pulses of a KrF-excimer laser with fluences in the range of E=50–700 mJ/cm². At fluences below 100 mJ/cm² an increase in the number of graphitic clusters and in their ordering was evidenced from Raman spectra, while the film structure remained amorphous according to electron microscopy and electron diffraction observations. At higher fluences the appearance of diamond particles of 2–7 nm size, embedded into the lower crystallized graphitic matrix, was observed and simultaneously a progressive growth of graphite nanocrystals with dimensions from 2 nm to 4 nm was deduced from Raman measurements. The maximum thickness of the crystallized surface layer (400 nm) and the degree of laser annealing are limited by the film ablation which starts at E>250 mJ/cm². The laser-treated areas lose their chemical inertness. In particular, chemical etching in chromium acid becomes possible, which may be used for patterning the highly inert carbon films.