大气环境下飞秒激光对铝靶烧蚀过程的研究

利用时间分辨的光阴影成像技术研究了在大气环境下飞秒激光烧蚀铝靶的动态过程. 在入射激光能量为4 mJ, 激光光斑超过1 mm时, 激光烧蚀区表面物质以近似平面冲击波形式向外喷射; 在同样激光能量下、激光光斑较小时(约0.6 mm), 激光烧蚀区以近似半球型冲击波形式向外喷射. 当激光能量比较大时(7 mJ), 发现空气的电离对于激光烧蚀靶材有着重要影响. 在光轴附近烧蚀产生的喷射物具有额外的柱状和半圆型的结构, 叠加在平面冲击波结构上.     

Fluence dependence of femtosecond-laser-induced nanostructure formed on TiN and CrN

The fluence dependence of the nanostructure formation, which has been observed in our recent experiments on femtosecond (fs)-laser ablation, was examined in detail for hard thin films of TiN and CrN. The size D of the periodic fine structure formed with fs-laser pulses can be divided into two regions that depend on the laser fluence F, i.e. the region I where D increases rapidly with increasing F near the ablation threshold, and the region II where D increases slowly with an increase in F and almost saturates. The nanostructure has been observed only in the region I with a narrow width of F. The region II produces a periodic ripple structure whose size is 1/2–4/5 of the wavelength used. The effects of the thermal process and material composition on the nanostructure formation are discussed. PACS 61.80.Ba; 79.20.Ds; 42.62.Cf     

Optodynamic study of multiple pulses micro drilling

This paper describes an analysis of pulsed lasers micro-drilling of different metals. Study focuses to an optodynamic phenomenon which appears as thermal effects induced by laser light pulses and leads to dynamic process manifested as ultrasonic shock waves propagating into the sample material. The shock waves are detected by a non-contact optical method by using arm compensated Michelson. Monitoring of the main parameters of the micro drilling such as material ablation rate and efficiency was realized by analysis of the optodynamic signals. The process is characterized by decreasing ablation rate that leads to the finite hole depth. The experimental part of study comprehends a comparison between various metals. In order to describe decreasing ablation rate a theoretical model based on the energy balance is proposed. It considers the energy/heat transfer from the laser beam to the material and predicts a decreasing drilling rate with an increasing number of successive laser pulses. According to the proposed model, the finite depth of the hole appears as a consequence of the increasing surface area through which the energy of the laser beam is conducted away to the material around the processed area. Decreasing ablation rate and the finite hole depth predicted by model were in good agreement with the experimental results.     

Direct observation of the temperature field during ablation of materials by multiple femtosecond laser pulses

We report a direct observation of the temperature field on a steel specimen during ablation by multiple femtosecond laser pulses using an infrared thermography technique. From the experimental results and simulation study of the temperature field, we quantified the deposited thermal power into the specimen during the ablation process. We found that more than two thirds of the incident laser power was deposited in the steel specimen when ablated by multiple femtosecond laser pulses. This result provides further understanding of the heating effect in materials processing by ultrashort laser pulses.     

Non-Thermal Laser Ablation Model for Micro-Surgical Applications

We have developed a non-thermal laser ablation model which may reduce thermal damage to neighboring structures. Based on this model, the three critical parameters for a well controlled non-thermal microsurgery are (1) the laser wavelength with its photon energy matching closely the bond dissociation energy, (2) the energy fluence must be above threshold to avoid thermal process due to non-radiative relaxation from the excited electronic states to vibrational, (3) ultra short laser pulses (few fs) to completely eliminate thermal and direct biomolecular reactions. In this model the UV laser photon dissociates the molecular bonds which leads to the splitting of longer polymer chains into small fragments. The excess energy if any may appear as kinetic energy in the polymer-fragments. The extreme rapidity of the bond breaking process reduces heat conduction. The model establishes a relationship between ablation depth per pulse, the absorption coefficient, the incident laser energy fluence, and the threshold energy fluence. The ablation depths per pulse were calculated for the polymers Polymethyl methacrylate (PMMA) and polyimide for various commercially available UV lasers. It has been found that the minimum ablations depth occurs at 193 nm for both PMMA and polyimide. This assures a well defined incision with minimal thermal damage to the surrounding structures at this wavelength. There exists a definite threshold energy fluence for non-thermal ablation for any given biomolecule and below the threshold the non-radiative relaxation process may cause thermal ablation. New ultra fast lasers (few femtoseconds) (fs) will completely eliminate thermal diffusion as well as direct biomolecular reactions.     

Picosecond pulse laser ablation of yttria-stabilized zirconia from kilohertz to megahertz repetition rates

Thin films of yttria stabilized zirconia were deposited onto silicon substrates using high repetition rate picosecond pulse lasers. The applied lasers covered the repetition rate range from 10 kHz to 4 MHz. We found that the laser pulse overlapping which results from increased repetition rates led to considerable changes in the ablation process. Defect formation and local heating lead to lower ablation thresholds and, with sufficiently high repetition rates, to melting of the target and even to thermal evaporation. We found that yttria-stabilized zirconia (YSZ) films deposited with picosecond pulses at 1064 nm wavelength below repetition rates of 2 MHz have rough, nanostructured morphology and the same atomic ratio of yttrium and zirconium as the target. Films deposited with 2 MHz and higher repetition rates with high number of overlapping pulses are very smooth, but are yttrium deficient, providing evidence of the importance of the thermal processes.     

Minimization of cavitation effects in pulsed laser ablation illustrated on laser angioplasty

Cavitation effects in pulsed laser ablation can cause severe deformation of tissue near the ablation site. In angioplasty, they result in a harmful dilatation and invagination of the vessel walls. We suggest to reduce cavitation effects by dividing the laser pulse energy into a pre-pulse with low and an ablation pulse with high energy. The pre-pulse creates a small cavitation bubble which can be filled by the ablation products of the main pulse. For suitable energy ratios between the pulses, this bubble will not be enlarged by the ablation products, and the maximal bubble size remains much smaller than after a single ablation pulse. The concept was analyzed by numerical calculations based on the Gilmore model of cavitation dynamics and by high-speed photography of the effects of single and double pulses performed with a silicone tube as vessel model. The use of double pulses prevents the deformation of the vessel walls. The concept works with an energy ratio of up to about 1:30 between the pulses. For the calculated optimal ratio of 1:14.6, the bubble volume is reduced by a factor of 17.7. The ablation pulse is best applied when the pre-pulse bubble is maximally expanded, but the timing is not very critical.     

纳秒紫外重复脉冲激光烧蚀单晶硅的热力学过程研究

采用波长为355 nm的纳秒紫外重复脉冲激光对单晶硅片进行了盲孔加工实验, 观测了随脉冲增加激光烧蚀硅片的外观形貌和盲孔孔深、孔径的变化规律, 并对紫外激光辐照硅片的热力学过程进行了分析. 研究结果表明:紫外激光加工硅盲孔是基于热、力效应共同作用的结果, 热效应会使得硅材料熔化、气化甚至发生电离产生激光等离子体,为材料的去除提供条件;激光等离子体冲击波以及高温气态物向外膨胀会对熔化材料产生压力致使其向外喷射,为重复脉冲的进一步烧蚀提供了条件;力效应主要沿着激光传输的方向,垂直于硅表面,使得去除部位主要集中在孔的深度方向,达到较高的孔径比,实验观察孔径比可达8:1;此外,激光等离子体的产生也阻止了激光对靶面的作用,加之随孔深的增加激光发生散焦,使得烧蚀深度有一定的限制,实验观察烧蚀脉冲个数在前100个时加工效率较高.     

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     

铁磁薄膜中圆偏振光感应的瞬态磁光Kerr峰的物理起源

使用飞秒时间分辨抽运-探测磁光Kerr光谱技术,实验研究了圆偏振光抽运面内磁化FePt和垂直磁化GdFeCo薄膜的磁化演化动力学,发现在时间延迟零点处均出现瞬态Kerr峰.分析了此Kerr峰的起源,指出此瞬态Kerr峰与铁磁性无关,可能起源于自由电子的顺磁磁化,而顺磁磁化的外磁场来自圆偏振抽运光的逆Faraday效应.基于顺磁磁化模型的计算结果支持此观点.基于此观点,逆Faraday效应感应的磁场脉冲宽度应该与激光脉冲宽度一致.     

Few‐optical‐cycle light pulses with passive carrier‐envelope phase stabilization

One of the most advanced frontiers of ultrafast optics is the control of carrier‐envelope phase (CEP) ϕ of light pulses, which enables the generation of optical waveforms with reproducible electric field profile. Such control is important for pulses with few‐optical‐cycle duration, for which a CEP variation produces a strong change in the waveform, so that strongly nonlinear optical phenomena, such as multiphoton absorption, above‐threshold ionization and high‐harmonic generation become CEP‐dependent. In particular, CEP control is the prerequisite for the production of isolated attosecond pulses. Standard laser systems generate pulses that are CEP unstable; the CEP can be stabilized using either active or passive methods. Passive, all‐optical schemes rely on difference‐frequency generation (DFG) between two pulses sharing the same CEP: in this process the phases of the two pulses add up with opposite signs, leading to cancellation of the shot‐to‐shot CEP fluctuations. This paper presents an overview of passive CEP stabilization schemes, starting from the basic concepts and progressing to the details of the practical implementations of the idea. The passive approach allows the generation of CEP‐controlled few‐optical‐cycle pulses covering a very broad range of parameters in terms of carrier frequency (from visible to mid‐IR), energy (up to several mJs) and repetition rate (up to hundreds of kHz)     

Pulse-width influence on the laser-induced structuring of CaF2 (111)

We have investigated the morphology of CaF₂ (111) irradiated by 780 nm laser pulses of varying pulse width (200 fs-8 ns) with fluences above the damage threshold. Large differences can be observed which we relate to the mechanisms and dynamics of defect production in this wide band gap material. The best defined and most controllable ablation is obtained for laser pulse widths of a few picoseconds. For nanosecond and femtosecond pulses strong fracturing of the crystal is observed with damage outside the laser irradiated zone. This has a thermal origin for nanosecond pulses but a non-thermal origin for pulse widths below approximately 1 ps.     

Early stage of the material removal during ArF laser ablation of graphite

Material removal during ArF excimer laser ablation of graphite at atmospheric pressure was investigated by two independent methods; 1) by observation of the propagating properties of the shock wave generated by the carbonaceous ejecta and 2) by in situ measurement of the size distribution of carbon nanoparticles condensing in the ablation plume. This latter was carried out by a scanning mobility particle sizer system based on a differential mobility analyser. The performed measurements indicate that the material removal during ArF laser ablation consists of two steps at fluences above the threshold fluence. First, a thin layer of carbon (of the order of 1 nm) is removed by a quick desorption process, leading to shockwave formation. This process takes place in a ns time scale, and desorption rate estimations reveal that this can not be explained by thermal surface evaporation. Since to our knowledge there is no thermal process that could account for the estimated desorption rate, it is argued that this is a fast photochemical (i.e. non-thermal) process. The size distribution of the condensed nanoparticles related to this step shows a rising edge at diameters below 10 nm. At fluences above the ablation threshold, the majority of the material is ejected in the second phase, resulting in condensation of carbon nanoparticles, peaking at 50 nm diameters in the size spectrum. Both shockwave formation and material removal are also detected well below the ablation threshold fluence, which is attributed to the photochemical process. PACS 61.46.+w; 81.16.Mk     

Energy‐dispersive diffraction with synchrotron radiation and a germanium detector

The response of an intrinsic Ge detector in energy‐dispersive diffraction measurements with synchrotron radiation is studied with model calculations and diffraction from perfect Si single‐crystal samples. The high intensity and time‐structure of the synchrotron radiation beam leads to pile‐up of the output pulses, and the energy distribution of the pile‐up pulses is characteristic of the fill pattern of the storage ring. The pile‐up distribution has a single peak and long tail when the interval of the radiation bunches is small, as in the uniform fill pattern, but there are many pile‐up peaks when the bunch distance is a sizable fraction of the length of the shaping amplifier output pulse. A model for the detecting chain response is used to resolve the diffraction spectrum from a perfect Si crystal wafer in the symmetrical Laue case. In the 16‐bunch fill pattern of the ESRF storage ring the spectrum includes a large number of `extra reflections' owing to pile‐up, and the model parameters are refined by a fit to the observed energy spectrum. The model is used to correct for the effects of pile‐up in a measurement with the 1/3 fill pattern of the storage ring. Si reflections (2h,2h,0) are resolved up to h = 7. The pile‐up corrections are very large, but a perfect agreement with the integrated intensities calculated from dynamical diffraction theory is achieved after the corrections. The result also demonstrates the convergence of kinematical and dynamical theories at the limit where the extinction length is much larger than the effective thickness of the perfect crystal. The model is applied to powder diffraction using different fill patterns in simulations of the diffraction pattern, and it is demonstrated that the regularly spaced pile‐up peaks might be misinterpreted to arise from superlattices or phase transitions. The use of energy‐dispersive diffraction in strain mapping in polycrystalline materials is discussed, and it is shown that low count rates but still good statistical accuracy are needed for reliable results.     

Anisotropic distribution of quantum‐vacuum momentum density in a moving electromagnetic medium

An isotropic electromagnetic medium becomes gyrotropically anisotropic when it moves, and an anisotropic electromagnetic environment can then be created in this motion‐induced anisotropic medium. One of the most remarkable features is that the quantum vacuum in the anisotropic electromagnetic environment exhibits a nonzero electromagnetic momentum density, since the universal symmetry of the vacuum fluctuation field is broken, and the anisotropic quantum vacuum mode structure is produced because of the symmetry breaking. This would give rise to a noncompensation effect among the four vacuum eigenmodes (i.e., the forward and backward propagating modes as well as their respective mutually perpendicular polarized components), and leads to an anisotropic correction to the vacuum momentum in the moving medium. The physical significance and the potential applications of the anisotropic quantum vacuum are discussed. This quantum‐vacuum effect may be used to develop sensitive sensor techniques and to design new quantum optical and photonic devices.     

Acoustic wave monitoring of the excimer laser ablation of YBCO high-Tc superconductor

Monitoring the amplitude and the delay of arrival of the pressure waves generated during the interaction of laser pulses with YBCO in air, we can determine the vaporization and the ablation thresholds, the etching rate, the change of the acoustic wave velocity and the effect of plasma shielding on the etching rate. The steep increase of the amplitude and the order-of-magnitude increase of the etching rate above the ablation threshold, suggest that the laser–target coupling mechanism changes from (thermal) vaporization below threshold to a rapid solid-to-gas phase transition. The dumping of the acoustic waves following the ablation with successive laser pulses correlates with the evolution of the YBCO high-T_c superconductor surface morphology, which is known to relate to the deposition rate and the surface morphology of pulsed-laser-deposited high-T_c thin films. Received: 7 January 2000 / Accepted: 9 October 2000 / Published online: 25 July 2001     

Rotor synchronization of radiofrequency and gradient pulses in high-resolution magic angle spinning NMR

We have investigated the extent to which rotor synchronization of radiofrequency pulses leads to spectral improvement in high-resolution magic angle spinning NMR experiments. Several pulse sequences were tested, and the effect was found to be maximal in homonuclear TOCSY spectra. The physicochemical nature of the sample plays a role in the phenomenon, as rotor synchronization allows the refocusing of residual anisotropic interactions. However, even in a liquid sample the effects were visible. Radial inhomogeneities of the radiofrequency field were identified as an important source of the problem.     

Aggregation and chimney formation during the solidification of ammonium chloride

Experiments study large-scale pattern formation during the growth of ammonium chloride (NH4Cl) from solution in a thin (Hele-Shaw) geometry. In particular a solid-liquid mixture ("mushy layer") forms in which growing solid NH4Cl crystals form a solid network interspersed with liquid. There are different ways that the mushy layer can be formed, however. If the cell is heated from below and cooled from above, thermal convection generates large-scale recirculating flows that carry seed crystals from the upper (cold) boundary to the (warmer) side and bottom boundaries. Ballistic deposition of these seed crystals leads to aggregation patterns with significant voids (filled with liquid) with a wide range of length scales. If the cell is cooled from below with a warm environment, the solid NH4Cl grows dendritically without deposition, resulting in a compact mushy layer. Plume convection within this mushy layer produces one or two well-defined "chimneys." If the environment is cool (comparable to the liquidus temperature of the solution), the mushy layer forms by a combination of dendritic growth and ballistic deposition, resulting in a more permeable mushy layer and enhanced chimney formation. The effects of ballistic deposition are enhanced if the cell is tipped, in which case the voids reappear. Plume convection and chimney formation are dramatically enhanced in this case. Additional experiments are done in which fluid flows in the system are enhanced artificially to verify that enhancements in chimney formation are due primarily to the aggregation process, and not to the increases in fluid flows due to thermal and compositional convection.     

Anisotropy enhanced X‐ray scattering from solvated transition metal complexes

Time‐resolved X‐ray scattering patterns from photoexcited molecules in solution are in many cases anisotropic at the ultrafast time scales accessible at X‐ray free‐electron lasers (XFELs). This anisotropy arises from the interaction of a linearly polarized UV–Vis pump laser pulse with the sample, which induces anisotropic structural changes that can be captured by femtosecond X‐ray pulses. In this work, a method for quantitative analysis of the anisotropic scattering signal arising from an ensemble of molecules is described, and it is demonstrated how its use can enhance the structural sensitivity of the time‐resolved X‐ray scattering experiment. This method is applied on time‐resolved X‐ray scattering patterns measured upon photoexcitation of a solvated di‐platinum complex at an XFEL, and the key parameters involved are explored. It is shown that a combined analysis of the anisotropic and isotropic difference scattering signals in this experiment allows a more precise determination of the main photoinduced structural change in the solute, i.e. the change in Pt—Pt bond length, and yields more information on the excitation channels than the analysis of the isotropic scattering only. Finally, it is discussed how the anisotropic transient response of the solvent can enable the determination of key experimental parameters such as the instrument response function.