The influence of thermal diffusion on laser ablation of metal films

Single-shot ablation thresholds of nickel and gold films in the thickness range from 50 nm to 7 m have been measured for 14 ns laser pulses at 248 nm, using photoacoustic shock wave detection in air. The metal films were deposited on fused silica substrates. The ablation threshold was found to increase linearly with film thickness up to the thermal diffusion length of the film. Beyond this point it remains independent of film thickness. The proportionality between threshold fluence and thickness allows the prediction of ablation thresholds of metal films from the knowledge of their optical properties, evaporation enthalpies and thermal diffusivities. Physically it proves that ablation is driven by the energy density determined by the thermal diffusion length. A simple thermodynamic model describes the data well. Thermal diffusivities, an essential input for this model, were measured using the technique of transient thermal gratings. In addition, the substrate dependence of the ablation threshold was investigated for 150 nm Ni films.     

Carbon thin films through laser ablation

Thin carbon films were deposited on silicon substrates at room temperature using a 0.355 μm Nd:YAG laser wavelength at low irradiance in the presence of argon gas. Various techniques including scanning electron microscopy, X-ray diffraction and Raman spectroscopy were used to analyze the film quality. The influence of the argon gas pressure on the properties of the films is demonstrated and a correlation with the optical emission data is presented.     

Picosecond laser ablation of thin copper films

The ablation process of thin copper films on fused silica by picosecond laser pulses is investigated. The ablation area is characterized using optical and scanning electron microscopy. The single-shot ablation threshold fluence for 40 ps laser pulses at 1053 nm has been determinated toF _thres = 172 mJ/cm². The ablation rate per pulse is measured as a function of intensity in the range of 5 × 10⁹ to 2 × 10¹¹ W/cm² and changes from 80 to 250 nm with increasing intensity. The experimental ablation rate per pulse is compared to heat-flow calculations based on the two-temperature model for ultrafast laser heating. Possible applications of picosecond laser radiation for microstructuring of different materials are discussed.     

Porphyrin-sensitized laser swelling and ablation of polymer films

Laser-induced morphological changes of poly(methyl methacrylate), poly(N-vinylcarbazole), and gelatin films doped with porphyrins have been studied by etch depth measurement and scanning electron microscopy. An irreversible swelling of the irradiated surface was observed for all films in the case of low laser fluence. The swelling was replaced by ablation when the fluence was increased. The etch depth depends on the irradiation fluence and the dye concentration in the polymer. The observation of the irradiated surfaces suggests that the thermal effect is predominant both for swelling and ablation. The surface temperature at which swelling or ablation is initiated was estimated, assuming that these morphological changes take place at a certain temperature for any dye concentration in each polymer film.     

Laser-induced ablation dynamics and flight of thin polymer films

We investigated the ejection dynamics of triazene polymer layers in the thickness range of 40 nm to 600 nm upon nanosecond laser ablation at a wavelength of 532 nm. The ablation is due to laser-induced thermal degradation of a small part of the polymer in contact with the silicon substrate. The subsequent dynamics of the flying polymer layer are measured with sub-nanosecond time resolution. The evaluation of the initial velocity for different film thicknesses gives insight into the energy transfer process during the acceleration of the films.     

Pulsed laser ablation deposition of thin films on large substrates

We have designed and built an ultra-high vacuum chamber which allows thin film deposition on large area (up to 100 mm diameter) flat substrates and on three-dimensional substrates (e.g. 100 mm long, 50 mm diameter cylinders) by the pulsed laser deposition and reactive pulsed laser deposition techniques. Heating of substrates during and after film deposition is possible using either resistive heaters or a lamp array. Metal (Cu) and metal nitride (TiN) and carbide (TiC) films were deposited on Si wafers (60 and 100 mm diameter), three-dimensional steel substrates (steel cylinders and screws), Teflon plates, and paper sheets.     

Excimer laser ablation of thin titanium oxide films on glass

Thin titanium dioxide films are deposited on glass substrates by magnetron sputter deposition. They are irradiated in air, by means of a KrF excimer laser. The ablation rate is measured as a function of the laser fluence per pulse, F, and of the number of pulses, N. Above a fluence threshold, the films are partially ablated. The ablated thickness does not vary linearly with N. This is the signature of a negative feedback between the film thickness and the ablation rate. The origin of this negative feedback is shown to be due to either thermal or electronic effects, or both. At high F, the film detachs from the substrate.     

Influence of the plasma parameters on the properties of aluminum oxide thin films deposited by laser ablation

The plasma produced by the ablation of a high purity Al₂O₃ target, using the fundamental line (1064 nm) of a Nd:YAG laser, was characterized. The laser fluence was varied in order to study its effect on the characteristics of the produced plasma as well as on the properties of the material deposited. Optical emission spectroscopy (OES) was used to determine the type of excited species present in the plasma. The mean kinetic energy of the ions and the maximum plasma density were determined from the time of flight (TOF) curves, obtained with a planar Langmuir probe. The obtained results reveal that the fast peak in the probe curve could be attributed to Al III, while the slow peak corresponds to the Al II. Aluminum oxide thin films were then deposited under the same conditions of the diagnosed plasma, in an attempt to correlate the plasma parameters with the properties of the deposited material. It was found that when Al II ion energies are lower than 461.0 eV the films deposited have structural characteristics similar to that of α-Al₂O₃, whereas at ion energies greater than 461.0 eV amorphous material was obtained.     

Deposition of NbC thin films by pulsed laser ablation

Niobium carbide thin films were prepared by pulsed laser ablation of a stoichiometric NbC target. XeCl (308 nm, 30 ns) and Nd:YAG (266 nm, 5 ns) lasers operating at a repetition rate of 10 Hz were used. Films were deposited on Si (100) substrates at room temperature either in vacuum or in an argon atmosphere (2᎒^-1 mbar). Different laser fluences (2, 4 and 6 J/cm²) and different numbers of pulses (1᎒⁴, 2᎒⁴ and 4᎒⁴) were tested. For the first time, NbC films were prepared through a clean procedure without the addition of a hydrocarbon atmosphere. The phase constitution of the films, unit cell size, mean crystallite dimensions and preferred orientation are determined as a function of deposition conditions by X-ray diffraction. Complementary morphological and structural analysis of the films were performed by scanning electron microscopy, atomic force microscopy and Rutherford backscattering spectroscopy.     

Nanostructured silver thin films deposited by pulsed laser ablation

Nanostructured thin films were deposited by excimer laser ablation of silver targets in controlled atmospheres of He and Ar. The film structural properties were investigated by means of scanning electron microscope and transmission electron microscope imaging. The film growth mechanism was identified as the result of coalescence of nanometric clusters formed during plume flight. Cluster formation involves plume confinement as a consequence of the increased collisional rate among plasma species. Fast photography imaging of the laser-generated silver plasma allowed to identify plasma confinement, shock wave formation and plasma stopping.     

Yttrium nitride thin films grown by reactive laser ablation

Yttrium nitride thin films were grown on silicon substrates by laser ablating an yttrium target in molecular nitrogen environments. The composition and chemical state were determined with Auger electron, X-Ray photoelectron, and energy loss spectroscopies. The reaction between yttrium and nitrogen is very effective using this method. Ellipsometry measurements indicate that the films are metallic. We attribute this behavior to a small oxygen contamination. Each oxygen atom introduces two additional electrons to the unit cell, resulting in a complex semiconductor-ionic-metallic system. These results are corroborated by first principles total energy calculations of clean and oxygen doped YN.     

Properties of conductive polymer films deposited by infrared laser ablation

Thin films of the conducting polymer poly(3,4-ethylenedioxy-thiophene):poly(styrenesulfonate) (PEDOT:PSS) were deposited by resonant infrared laser vapor deposition (RIR-LVD). The PEDOT:PSS was frozen in various matrix solutions and deposited using a tunable, mid-infrared free-electron laser (FEL). The films so produced exhibited morphologies and conductivities that were highly dependent on the solvent matrix and laser irradiation wavelength used. When deposited from a native solution (1.3% by weight in water), as in matrix-assisted pulsed laser evaporation (MAPLE), films were rough and electrically insulating. When the matrix included other organic “co-matrices” that were doped into the solution prior to freezing, however, the resulting films were smooth and exhibited good electrical conductivity (0.2 S/cm), but only when irradiated at certain wavelengths. These results highlight the importance of the matrix/solute and matrix/laser interactions in the ablation process.     

脉冲激光制备薄膜材料的烧蚀机理

研究了脉冲激光烧蚀靶材的整个过程.从包含热源项的导热方程出发，利用适当的动态边界条件，详细研究了靶材在熔融前后的温度分布规律，并且给出了熔融后的固、液分界面的变化规律.熔融后的温度演化规律和固液相界面均以解析表达式的形式给出.还根据能量平衡原理给出烧蚀面位置随时间的变化规律.以硅靶材为例计算模拟了激光烧蚀的整个过程，与实验结果符合较好. 关键词： 脉冲激光 烧蚀面 熔融 温度演化     

Depth profiling of copper thin films by resonant laser ablation

In Resonant Laser Ablation (RLA), material is related and selectively ionized by a low-energy pulse from a tunable laser. The selectivity and efficiency allow detection and quantitation at very low concentrations. We demonstrate that RLA has potential use in profiling thin layer and multilayer structures. Quantitative results are reported on the analysis of 20 and 100 Å copper thin films on Si(110) surfaces. Removal rates range from 10^–3 to 10^–2 Å/shot. Prospects for interrogation of dopants and impurities are also evaluated.     

Numerical simulation of the ablation of thin molybdenum films under laser irradiation

Laser irradiation of a molybdenum film on a quartz substrate is numerically studied. The simulated results prove the experimental effect lying in a threefold decrease in the size of the ablation region in comparison with the focal spot. The numerical experiment proves the hypothesis on the two-stage ablation of metal film with the primary formation of oxide phase. It is demonstrated that oxidation leads to a selective decrease in the thermal resistance of the film along the vertical direction, so that the anisotropic character of the ablation is enhanced.     

Textured thin films grown at room temperature by laser ablation

Thin films of SrFe₁₂O₁₉, BaFe₁₂O₁₉, Pb_0.76La_{0.16 0.08}Zr_0.53Ti_0.47O₃and Sr_0.3Ba_0.7Nb₂O₆ were grown on monocrystalline silicon substrates by pulsed laser deposition using a 20-ns Nd:YAG laser (1064 nm). The deposited thin films were analyzed by X-ray diffraction in the grazing incidence configuration. The analysis showed evidence of textured growth even though the films were grown at room temperature. Emission spectroscopy was used to establish the time of flight of the species within the plasma plume. Velocities of the order of 10⁶ cm/s were obtained. The high kinetic energy of the species is thought to be responsible for the film texture, as it is released in the substrate–film system, favoring a preferential growth. For all the ablated ceramics, singly ionized species were shown to expand at higher velocities than neutrals. For ions, no consistency in the mass–speed relation was obtained, suggesting both the presence of electric fields during the plasma formation and an evaporation of the target that depends on the vapor pressure of the elements. In this way species that are firstly evaporated will be attracted strongly by fast electrons, allowing heavy ions to acquire higher velocities than lighter ones. PACS 81.15.Fg; 52.38.Mf; 68.55.Jk; 52.38.Kd; 52.70.Kz     

纳秒脉冲激光沉积薄膜过程中的烧蚀特性研究

研究了高能短脉冲激光薄膜制备的整个烧蚀过程.首先建立了基于超热理论的烧蚀模型，然 后利用较为符合实际的高斯分布表示脉冲激光输入能量密度，给出了考虑蒸发效应不同阶段 的烧蚀状态方程.结合适当的边界条件，以Si靶材为例，利用有限差分法得到了靶材在各个 阶段温度随时间和烧蚀深度的演化分布规律及表面蒸发速度与烧蚀深度在不同激光辐照强度 下随时间的演化规律.结果表明，在脉冲激光辐照阶段，靶材表面的蒸发效应使得靶材表面 温度上升显著放缓；在激光辐照强度接近相爆炸能量阈值时，蒸发速度与蒸发厚度的变化由 于逆流现象将显著放缓.还得到了考虑了熔融弛豫时间及蒸发效应的固-液界面随时间的演化 方程，这一结论较先前工作更具有普适性. 关键词： 脉冲激光烧蚀 热流方程 温度演化 有限差分法     

Resonant infrared pulsed laser deposition of thin biodegradable polymer films

Thin films of the biodegradable polymer poly(DL-lactide-co-glycolide) (PLGA) were deposited using resonant infrared pulsed laser deposition (RIR-PLD). The output of a free-electron laser was focused onto a solid target of the polymer, and the films were deposited using 2.90 (resonant with O-H stretch) and 3.40 (C-H) μm light at macropulse fluences of 7.8 and 6.7 J/cm², respectively. Under these conditions, a 0.5-μm thick film can be grown in less than 5 min. Film structure was determined from infrared absorbance measurements and gel permeation chromatography (GPC). While the infrared absorbance spectrum of the films is nearly identical with that of the native polymer, the average molecular weight of the films is a little less than half that of the starting material. Potential strategies for defeating this mass change are discussed. Received: 22 August 2001 / Accepted: 23 August 2001 / Published online: 17 October 2001     

Characterization of polymer thin films obtained by pulsed laser deposition

The development of laser techniques for the deposition of polymer and biomaterial thin films on solid surfaces in a controlled manner has attracted great attention during the last few years. Here we report the deposition of thin polymer films, namely Polyepichlorhydrin by pulsed laser deposition. Polyepichlorhydrin polymer was deposited on flat substrate (i.e. silicon) using an NdYAG laser (266 nm, 5 ns pulse duration and 10 Hz repetition rate).The obtained thin films have been characterized by atomic force microscopy, scanning electron microscopy, Fourier transform infrared spectroscopy and spectroscopic ellipsometry.It was found that for laser fluences up to 1.5 J/cm² the chemical structure of the deposited polyepichlorhydrin polymer thin layers resembles to the native polymer, whilst by increasing the laser fluence above 1.5 J/cm² the polyepichlorohydrin films present deviations from the bulk polymer.Morphological investigations (atomic force microscopy and scanning electron microscopy) reveal continuous polyepichlorhydrin thin films for a relatively narrow range of fluences (1-1.5 J/cm²).The wavelength dependence of the refractive index and extinction coefficient was determined by ellipsometry studies which lead to new insights about the material.The obtained results indicate that pulsed laser deposition method is potentially useful for the fabrication of polymer thin films to be used in applications including electronics, microsensor or bioengineering industries.