Time-resolved measurements during backside dry etching of fused silica

The laser-induced backside dry etching (LIBDE) investigated in this study makes use of a thin metal film deposited at the backside of a transparent sample to achieve etching of the sample surface. For the time-resolved measurements at LIBDE fused silica samples coated with 125 nm tin were used and the reflected and the transmitted laser intensities were recorded with a temporal resolution of about 1 ns during the etching with a ∼30 ns KrF excimer laser pulse. The laser beam absorption as well as characteristic changes of the reflection of the target surface was calculated in dependence on the laser fluence in the range of 250-2500 mJ/cm² and the pulse number from the temporal variations of the reflection and the transmission. The decrease of the time of a characteristic drop in the reflectivity, which can be explained by the ablation of the metal film, correlates with the developed thermal model. However, the very high absorption after the film ablation probably results in very high temperatures near the surface and presumably in the formation of an absorbing plasma. This plasma may contribute to the etching and the surface modification of the substrate. After the first pulse a remaining absorption of the sample was measured that can be discussed by the redeposition of portions of the ablated metal film or can come from the surface modification in the fused silica sample. These near-surface modifications permit laser etching with the second laser pulse, too.     

Microstructuring of fused silica by laser-induced backside wet etching using picosecond laser pulses

The laser-induced backside wet etching (LIBWE) is an advanced laser processing method used for structuring transparent materials. LIBWE with nanosecond laser pulses has been successfully demonstrated for various materials, e.g. oxides (fused silica, sapphire) or fluorides (CaF₂, MgF₂), and applied for the fabrication of microstructures. In the present study, LIBWE of fused silica with mode-locked picosecond (t_p = 10 ps) lasers at UV wavelengths (λ₁ = 355 nm and λ₂ = 266 nm) using a (pyrene) toluene solution was demonstrated for the first time. The influence of the experimental parameters, such as laser fluence, pulse number, and absorbing liquid, on the etch rate and the resulting surface morphology were investigated. The etch rate grew linearly with the laser fluence in the low and in the high fluence range with different slopes. Incubation at low pulse numbers as well as a nearly constant etch rate after a specific pulse number for example were observed. Additionally, the etch rate depended on the absorbing liquid used; whereas the higher absorption of the admixture of pyrene in the used toluene enhances the etch rate and decreases the threshold fluence. With a λ₁ = 266 nm laser set-up, an exceptionally smooth surface in the etch pits was achieved. For both wavelengths (λ₁ = 266 nm and λ₂ = 355 nm), LIPSS (laser-induced periodic surface structures) formation was observed, especially at laser fluences near the thresholds of 170 and 120 mJ/cm², respectively.     

Laser backside etching of fused silica with ultra-short pulses

Laser backside etching of transparent materials like fused silica at the interface to liquids with sub-picosecond UV laser pulses using a pyrene/toluene solution is achieved. For the experimental conditions applied, the etching effect is rather weak with measured rates of the order of 0.1 nm/pulse. A linear dependence of the etched volume upon the laser pulse energy or the pulse number was extracted from the experimental data obtained. At low pulse numbers the etched surface exhibits a feature-free, smooth morphology, while quasi-periodic ripple formation is observed for prolonged laser exposure. In addition, the etching process is accompanied by enhanced carbon deposition at and in the vicinity of the etched surface. The etching mechanism proposed comprises the primary interaction of the laser radiation with the liquid, a surface-modification phase, and the etching of the modified fused-silica surface. PACS 81.65.Cf; 81.05.Kf; 79.20.Ds; 61.80.Ba; 42.55.Lt; 68.45.Da     

Time-resolved transmission study of fused silica during laser-induced backside dry etching

Laser-induced backside dry etching (LIBDE) is a promising technique for micro- and nanomachining of transparent materials. Although several experiments have already proved the suitability and effectiveness of the technique, there are several open questions concerning the etching mechanism and the concomitant processes. In this paper time-resolved light transmission investigations of etching process of fused silica are presented. 125 nm thick silver coating was irradiated through the carrying 1 mm thick fused silica plate by single pulses of a nanosecond KrF excimer laser. The applied fluences were 0.38, 0.71 and 1 J/cm². During the etching process the irradiated spots were illuminated by an electronically delayed nitrogen laser pumped dye laser. The delay between the pump and probe pulses was varied in the range of 0 ns and 20 μs. It was found that the transmitted probe beam intensity strongly depends on the applied delays and fluences. Scanning electron microscopy and energy dispersive X-ray spectrometry of the etched surface showed the existence of silver droplets and fragments on the illuminated surfaces and silver atoms built into the treated surface layer influencing the transmission behavior of the studied samples.     

Laser backside etching of fused silica due to carbon layer ablation

The backside ablation of a absorbing carbon layer onto fused silica is studied in air and water confinement in comparison. The confinement influences the etch rate and the laser fluence dependence of the etch rate significantly while the threshold fluence is almost the same. The different confinement of the laser induced plasma results in the observed rate saturation in the case of air and in a linear growing rate in the case of water confinement at medium laser fluences. The less dense air confinement permits a faster plasma expansion of the laser plume than in the case of water confinement and effects consequently the interaction time and interaction strength of the laser plume with the fused silica surface. The differences in the laser-plasma-substrate interaction cause the observed rate saturation at weak interaction (air) and the growing etch rate at strong interaction (water). Thus, the confinement situation controls the interaction process in the case of backside ablation and should be considered in indirect material processing methods such as LIBWE and LESAL, too. PACS 81.65.C; 81.05.K; 79.20.D; 61.80.B; 42.55.L; 68.45.D     

Surface plasmon scattering on polymer-bimetal layer covered fused silica gratings generated by laser induced backside wet etching

Large amplitude fused silica gratings are prepared by combining the UV laser induced backside wet etching technique (LIBWE) and the two-beam interference method. The periodic patterning of fused silica surfaces is realized by s-polarized fourth harmonic beams of a Nd:YAG laser, applying saturated solution of naphthalene in methyl-methacrylate as liquid absorber. Atomic force microscopy is utilized to analyze how the modulation amplitude of the grating can be controlled by the fluence and number of laser pulses. Three types of plasmonic structures are prepared by a bottom-up method, post-evaporating the fused silica gratings by gold-silver bimetal layers, spin-coating the metal structures by thin polycarbonate films, and irradiating the multilayers by UV laser. The effect of the bimetal and polymer-coated bimetal gratings on the surface plasmon resonance is investigated in a modified Kretschmann arrangement allowing polar and azimuthal angle scans. It is demonstrated experimentally that scattering on rotated gratings results in additional minima on the resonance curves of plasmons excited by second harmonic beam of a continuous Nd:YAG laser. The azimuthal angle dependence proves that these additional minima originate from back-scattering. The analogous reflectivity minima were obtained by scattering matrix method calculations realized taking modulation depths measured on bimetal gratings into account.     

Effects of halogenated organic solvents on laser-induced backside wet etching of fused silica

Laser-induced backside wet etching of fused silica using a solution of pyrene dissolved in halogenated and non-halogenated solvents is presented. A significant influence of the solvent used on the etch rate and the etched surface appearance was ascertained. The etching of uniform and smooth surfaces with rates of ∼0.1 nm/pulse for laser fluences below 500 mJ/cm² is observed only for halogenated solvents. Furthermore, reduced threshold fluences, only small incubation effects, and a constant etch rate in dependence on the pulse number were found. The experimental data suggest an additional etch process at low laser fluences characterized by the very low etch rate and the smooth etching observed only with halogen-containing solvents. The generation of halogen radicals/compounds close to the heated surface due to the decomposition of the solvent causing the attack of the surface seems the most probable mechanism. PACS 81.65.Cf; 81.05.Kf; 79.20.Ds; 61.80.Ba; 42.55.Lt; 68.45.Da     

Fabrication of 550 nm gratings in fused silica by laser induced backside wet etching technique

A series of 550 nm spacing gratings were fabricated in fused silica by laser induced backside wet etching (LIBWE) method using the fourth harmonic of a Q-switched Nd:YAG laser (wavelength: λ = 266 nm; pulse duration: FWHM = 10 ns). During these experiments we used a traditional two-beam interference method: the spatially filtered laser beam was split into two parts, which were interfered at a certain incident angle (2θ = 28°) on the backside surface of the fused silica plate contacting with the liquid absorber (saturated solution of naphthalene-methyl-methacrylate c = 1.85 mol/dm³). We studied the dependence of the quality and the modulation depth of the prepared gratings on the applied laser fluence and the number of laser pulses. The surface of the etched gratings was characterized by atomic force microscope (AFM). The maximum modulation depth was found to be 180-200 nm. Our results proved that the LIBWE procedure is suitable for production of submicrometer sized structures in transparent materials.     

Backside laser etching of fused silica using liquid gallium

Laser-induced backside wet etching (LIBWE) that is regularly performed with hydrocarbon solutions is demonstrated with the liquid metal gallium as a new class of absorbers for the first time. Well-contoured square etch pits in fused silica with smooth bottoms and well-defined edges were achieved already with the first pulse from a 248 nm excimer laser. The etching is characterized by a threshold fluence of 1.3 J/cm² and a straight proportional etch rate growth with the fluence up to 8.2 J/cm². In addition, the etch depth increases linearly for onward pulsed laser irradiation and gives evidence for an only marginal incubation effect. The high fluences necessary for etching originate from the high reflection losses as well as the high thermal conductivity of the metallic absorber. The suggested etch mechanism comprises the heating of the fused silica up to or beyond the fused silica melting point by the laser heated gallium and the removing of the softened or molten fraction of the material by mechanical forces from shock waves, bubbles, high pressures, or stress fields. PACS 81.65.C; 81.05.J; 79.20.D; 61.80.B; 42.55.L     

104 nm period grating fabrication in fused silica by immersion two-beam interferometric laser induced backside wet etching technique

A substantial extension of the method of two-beam interferometric laser induced backside wet etching (TWIN-LIBWE), the immersion TWIN-LIBWE, is used to fabricate fused silica gratings with a 104 nm period. The spatially filtered fourth harmonic of Nd:YAG laser (λ=266 nm, τ_FWHM=8 ns) pulses were split into two parts which then interfered at the backside of the fused silica target in contact with a liquid absorber (naphthalene methyl methacrylate saturated solution with a concentration of 1.85 mol/dm³). The hypotenuse of a rectangular fused silica prism is attached to the fused silica target with the use of distilled water as the immersion liquid. On steering the beams through the sides of the prisms, the angle between the two laser beams has been substantially increased. The resulting period of 104 nm is the minimal grating constant achievable under such experimental conditions and, to our knowledge, the smallest laser generated grating period in fused silica at present. PACS 42.62; 42.79; 81.65     

Using Ion-beam etching to smooth fused silica surfaces

The roughness of fused silica, silicon, and sapphire substrates from different manufacturers is studied. Features of the substrates for imaging optics in the soft X-ray (SXR) and extreme UV (EUV) ranges are discussed. The first results from smoothing quartz substrates by etching with neutralized 50–500-eV argon beams are reported. Surface smoothing has been observed in the spatial-frequency range of 10^-1-10^-2 μm^-1.     

Indirect laser etching of fused silica: Towards high etching rate processing

The indirect laser processing approach (LIBWE) laser-induced backside wet etching allows defined microstructuring of transparent materials at low laser fluences with high quality. The optical and the thermal properties of the solid/liquid interface determine the temperatures and therefore the etching mechanism in conjunction with the dynamic processes at the interface due to the fast heating/cooling rates. The exploration of organic liquid solvents and solutions such as 0.5 M pyrene/toluene results in low etch rates (∼20 nm/pulse). By means of liquid metals as absorber here, demonstrated for gallium (Ga), etch rates up to 600 nm/pulse can be achieved. Regardless of the high etch rates a still smooth surface similar to etching with organic liquid solutions can be observed. A comparative study of the two kinds of absorbing liquids, organic and metallic, investigates the etch rates regarding the fluence and pulse quantity. Thereby, the effect of incubation processes as result of surface modification on the etching is discussed. In contrast to pyrene/toluene solution the metallic absorber cannot decompose and consequently no decomposition products can alter the solid/liquid interface to enhance the absorption for the laser radiation. Hence, incubation can be neglected in the case of the silica/gallium interface so that this system is a suitable model to investigate the primary processes of LIBWE. To prove the proposed thermal etch mechanism an analytical temperature model based on a solution of the heat equation is derived for laser absorption at the silica/gallium interface.     

Backside etching of fused silica with Nd:YAG laser

The laser-induced backside etching of fused silica with gallium as highly absorbing backside absorber using pulsed infrared Nd:YAG laser radiation is demonstrated for the first time. The influence of the laser fluence, the pulse number, and the pulse length on the etch rate and the etched surface topography was studied. The comparable high threshold fluences of about 3 and 7 J/cm² for 18 and 73 ns pulses, respectively, are caused by the high reflectivity of the fused silica-gallium interface and the high thermal conductivity of gallium. For the 18 and 73 ns long pulses the etch rate rises almost linearly with the laser fluence and reaches a value of 350 and 300 nm/pulse at a laser fluence of about 12 and 28 J/cm², respectively. Incubation processes are almost absent because etching is already observed with the first laser pulse at all etch conditions and the etch rate is constant up to 30 pulses.The etched grooves are Gaussian-curved and show well-defined edges and a smooth bottom. The roughness measured by interference microscopy was 1.5 nm rms at an etch depth of 0.6 μm. The laser-induced backside etching with gallium is a promising approach for the industrial application of the backside etching technique with IR Nd:YAG laser.     

超声波辅助酸蚀提高熔石英损伤阈值

为了提高熔石英元件表面抗激光损伤阈值,利用超声波辅助HF酸研究平滑光学元件表面缺陷形貌和去除刻蚀后残留物效果,通过扫描电子显微镜电镜和原子力显微镜记录表面形貌结构,以及单脉冲激光辐照测试抗损伤阈值确定实验参数。研究表明,超声波场的引入能催化HF酸的刻蚀速率、提高钝化效果并且更易剥离嵌入的亚μm级杂质粒子。经过实验测试,获得了熔石英类元件相匹配的超声辅助HF酸刻蚀实验参数,研究结果对应用超声波辅助HF酸研究熔石英表面抗激光损伤有重要意义。     

超声波辅助酸蚀提高熔石英损伤阈值

为了提高熔石英元件表面抗激光损伤阈值,利用超声波辅助HF酸研究平滑光学元件表面缺陷形貌和去除刻蚀后残留物效果,通过扫描电子显微镜电镜和原子力显微镜记录表面形貌结构,以及单脉冲激光辐照测试抗损伤阈值确定实验参数。研究表明,超声波场的引入能催化HF酸的刻蚀速率、提高钝化效果并且更易剥离嵌入的亚m级杂质粒子。经过实验测试,获得了熔石英类元件相匹配的超声辅助HF酸刻蚀实验参数,研究结果对应用超声波辅助HF酸研究熔石英表面抗激光损伤有重要意义。;     

Improvement of laser damage thresholds of fused silica by ultrasonic-assisted hydrofluoric acid etching

Polished fused silica samples were etched for different durations by using hydrofluoric(HF) acid solution with HF concentrations in an ultrasonic field. Surface and subsurface polishing residues and molecular structure parameters before and after the etching process were characterized by using a fluorescence microscope and infrared(IR) spectrometer, respectively. The laser induced damage thresholds(LIDTs) of the samples were measured by using pulsed nanosecond laser with wavelength of 355 nm. The results showed that surface and subsurface polishing residues can be effectively reduced by the acid etching process, and the LIDTs of fused silica are significantly improved. The etching effects increased with the increase of the HF concentration from 5 wt.% to 40 wt.%. The amount of polishing residues decreased with the increase of the etching duration and then kept stable. Simultaneously, with the increase of the etching time, the mechanical strength and molecular structure were improved.     

酸蚀与紫外激光预处理结合提高熔石英损伤阈值

采用HF酸刻蚀和紫外激光预处理相结合的方式提升熔石英元件的负载能力,用质量分数为1%的HF缓冲溶液对熔石英刻蚀1~100 min,综合透过率、粗糙度和损伤阈值测试结果,发现刻蚀时间为10min的熔石英抗损伤能力最佳。采用355 nm紫外激光对HF酸刻蚀10 min的熔石英进行预处理,结果表明:紫外预处理能量密度在熔石英零损伤阈值的60%以下时,激光损伤阈值单调递增;能量到达80%时,阈值反而低于原始样片的损伤阈值。适当地控制酸蚀时间和紫外激光预处理参数能有效提高熔石英的抗损伤能力。     

熔石英元件HF刻蚀的实验研究

为深入了解熔石英元件化学刻蚀过程,研究了HF刻蚀反应机理、HF刻蚀工艺参数以及刻蚀对表面质量的影响规律。通过控制变量法,获得刻蚀速率随HF浓度、刻蚀温度以及NH4F浓度的变化规律。对刻蚀不同深度后的元件表面粗糙度、形貌、杂质含量以及激光损伤阈值进行了检测,实验结果表明：刻蚀速率受多种因素共同影响,其中HF浓度的促进作用最为显著;刻蚀后的熔石英表面形貌复杂,有横向、纵向、拖尾等形式的划痕,以及坑点、杂质等缺陷,其中横向划痕和纵向划痕占据了缺陷部分的主体,主要杂质铈元素随刻蚀时间的增长不断减少;激光损伤阈值测量实验表明,通过HF刻蚀将元件损伤阈值提高了59.6%。     

酸蚀与紫外激光预处理结合提高熔石英损伤阈值

采用HF酸刻蚀和紫外激光预处理相结合的方式提升熔石英元件的负载能力,用质量分数为1%的HF缓冲溶液对熔石英刻蚀1~100 min,综合透过率、粗糙度和损伤阈值测试结果,发现刻蚀时间为10 min的熔石英抗损伤能力最佳。采用355 nm紫外激光对HF酸刻蚀10 min的熔石英进行预处理,结果表明：紫外预处理能量密度在熔石英零损伤阈值的60%以下时,激光损伤阈值单调递增;能量到达80%时,阈值反而低于原始样片的损伤阈值。适当地控制酸蚀时间和紫外激光预处理参数能有效提高熔石英的抗损伤能力。     

Subwavelength structures for high power laser antireflection application on fused silica by one-step reactive ion etching

In this paper we report a simple method to fabricate a novel subwavelength structure surface on fused silica substrate using one-step reactive ion etching with two-dimensional polystyrene colloidal crystals as masks. The etching process and the morphologies of the obtained structure are controlled. We show that the period of the obtained fused silica pillar-like arrays were determined by the initial polystyrene nanoparticle size. The height of pillar arrays can be adjusted by controlling the etching duration, which is proved to be of importance in tailoring the antireflection properties of subwavelength structures surface. The novel subwavelength structures surface exhibit excellent broadband antireflection properties, but the size of the pillar affects the antireflective properties in short wavelength region. We anticipate this method would offer a convenient and scalable way for inexpensive and high-efficiency high power laser field designs.