Properties of nanoparticles generated during femtosecond laser machining in air and water

Femtosecond laser ablation is used to generate nanoparticle aerosols and colloids from solid targets of various materials (Ti, Ag, Au, Co, etc.) in air and water ambience. We determine the influence of different laser parameters (pulse energy, pulse overlap) and properties of media (air, airbrush, water) on the rate of production and size distribution of the laser-generated nanoparticles. It is shown that the pulse overlap and laser fluence are the parameters determining the nanoparticle size. At optimum conditions the nanoparticle productivity can be increased by 150–300%. The generation of multimaterial nanoparticle dispersions is demonstrated. Being free of toxic impurities, the laser-produced nanoparticles may be promising for biomedical applications. PACS 79.20.Ds; 81.16.Mk; 81.16.-c; 52.38.Ph; 06.60.Jn     

Critical parameters of a micro-hotspot model of the laser-pulse initiation of the explosive decomposition of energetic materials

The work continues a series of studies of the micro-hotspot model a thermal explosion. The dependences of the critical energy fluence and the temperature of the reaction kernel in pentaerythritol tetranitrate (PETN) on the radius of aluminum nanoparticles at half-maximum pulse durations of 10 to 150 ns are calculated. For each pulse duration, there is an optimal nanoparticle radius at which the critical energy fluence is minimal. The dependences of these parameters on the pulse duration are derived. It is shown that there is a universal relationship, independent of the pulse duration, between the normalized critical energy fluence and the nanoparticle radius.     

Evolution of terahertz conductivity in ZnSe nanocrystal investigated with optical-pump terahertz-probe spectroscopy

The unique optical properties of nanoparticles are highly sensitive in respect to particle shapes, sizes, and localization on a sample. This demands for a fully controlled fabrication process. The use of femtosecond laser pulses to generate and transfer nanoparticles from a bulk target towards a collector substrate is a promising approach. This process allows a controlled fabrication of spherical nanoparticles with a very smooth surface. Several process parameters can be varied to achieve the desired nanoparticle characteristics. In this paper, the influence of two of these parameters, i.e. the applied pulse energy and the laser beam shape, on the generation of Si nanoparticles from a bulk Si target are studied in detail. By changing the laser intensity distribution on the target surface one can influence the dynamics of molten material inducing its flow to the edges or to the center of the focal spot. Due to this dynamics of molten material, a single femtosecond laser pulse with a Gaussian beam shape generates multiple spherical nanoparticles from a bulk Si target. The statistical properties of this process, with respect to number of generated nanoparticles and laser pulse energy are investigated. We demonstrate for the first time that a ring-shaped intensity distribution on the target surface results in the generation of a single silicon nanoparticle with a controllable size. Furthermore, the generated silicon nanoparticles presented in this paper show strong electric and magnetic dipole resonances in the visible and near-infrared spectral range. Theoretical simulations as well as optical scattering measurements of single silicon nanoparticles are discussed and compared.     

In situ bioconjugation—Novel laser based approach to pure nanoparticle-conjugates

The generation and characterization of nanoparticulate carrier systems is important for drug delivery, biosensing and in vivo or in vitro diagnostics. Conventional nanoparticle generation is based on chemical synthesis methods requiring time intensive reaction and additive design for each material. Successive purification and surface functionalisation is often required after the nanoparticle generation to achieve pure nanoparticle-bioconjugates. We established a novel single step method, which allows the generation of pure nanoparticles and their in situ conjugation with biomolecules bearing electron donating moieties using pulsed laser ablation in liquids. For comparison between unspecific binding and binding through strong dative bonds (here: S-Au), we applied this preparation method to the conjugation of gold nanoparticles with unmodified and thiolated oligonucleotides. In order to determine optimal parameters (laser pulse energy, focus diameter), the influence on productivity of nanoparticle generation and their interaction with oligonucleotides is studied. We report quenching of nanoparticle growth and modification of the surface plasmon resonance as evidence of a successful functionalisation. Their stability in ionic solutions is evidenced with relevance to biological and medical assays. Negligible differences between the two model bioconjugations evidence the universality of the established in situ bioconjugation method.     

Simulation of rippled structure adjustments based on localized transient electron dynamics control by femtosecond laser pulse trains

This study investigates the effects of pulse energy distributions on subwavelength ripple structures (the ablation shapes and subwavelength ripples) using the plasma model with the consideration of laser particle–wave duality. In the case studies, the laser pulse (800 nm, 50 fs) trains consist of double pulses within a train with the energy ratios of 1:2, 1:1, and 2:1. Localized transient electron densities, material optical properties, and surface plasmon generation are strongly affected by the energy distributions. Hence, the adjustment of the ablation shape and subwavelength ripples can be achieved based on localized transient electron dynamics control during femtosecond laser pulse train processing of dielectrics. The simulation results show that better, more uniform structures, in terms of ablation shapes and subwavelength ripples, can be easily formed at a lower fluence or subpulse energy ratio of 1:1 with a fixed fluence. It is also found that pulse trains at a 1:1 energy ratio are preferred for drilling high-aspect-ratio microholes or microchannels.     

High-energy femtosecond Yb-doped fiber laser operating in the anomalous dispersion regime

We report on high-energy ultrashort pulse generation from a passively mode-locked ytterbium-doped large-mode-area photonic crystal fiber oscillator operating in the anomalous dispersion regime. In the single-pulse regime, the laser directly generates 880 mW of average power of sub-500 fs pulses at a repetition rate of 53.33 MHz, corresponding to a pulse energy of 16.5 nJ. Stable and self-starting operation is obtained by adapting the spot size at the saturable absorber mirror to the pulse evolution in the low-nonlinearity fiber. The approach presented demonstrates the scaling potential of fiber based short pulse oscillators towards the microJ-level.     

Dynamics of femtosecond laser-produced plasma ions

We investigated the ion laser-produced plasma plume generated during ultrafast laser ablation of copper and silicon targets in high vacuum. The ablation plasma was induced by ≈50 fs, 800 nm Ti:Sa laser pulses irradiating the target surface at an angle of 45°. An ion probe was used to investigate the time-of-flight profiles of the emitted ions in a laser fluence range from the ablation threshold up to ≈10 J/cm². The angular distribution of the ion flux and average velocity of the produced ions were studied by moving the ion probe on a circle around the ablation spot. The angular distribution of the ion flux is well described by an adiabatic and isentropic model of expansion of a plume produced by laser ablation of solid targets. The angular distribution of the ion flux narrows as the laser pulse fluence increases. Moreover, the ion average velocity reaches values of several tens of km/s, evidencing the presence of ions with kinetic energy of several hundred eV. Finally, the ion flux energy is confined in a narrow angular region around the target normal.     

Pulse laser ablation at water–air interface

We studied a new pulse laser ablation phenomenon on a liquid surface layer, which is caused by the difference between the refractive indices of the two materials involved. The present study was motivated by our previous study, which showed that laser ablation can occur at the interface between a transparent material and a gas or liquid medium when the laser pulse is focused through the transparent material. In this case, the ablation threshold fluence is reduced remarkably. In the present study, experiments were conducted in water and air in order to confirm this phenomenon for a combination of two fluid media with different refractive indices. This phenomenon was observed in detail by pulse laser shadowgraphy. A high-resolution film was used to record the phenomenon with a Nd:YAG pulse laser with 10-ns duration as a light source. The laser ablation phenomenon on the liquid surface layer caused by a focused Nd:YAG laser pulse with 1064-nm wavelength was found to be followed by the splashing of the liquid surface, inducing a liquid jet with many ligaments. The liquid jet extension velocity was around 1000 m/s in a typical case. The liquid jet decelerated drastically due to rapid atomization at the tips of the ligaments. The liquid jet phenomenon was found to depend on the pulse laser parameters such as the laser fluence on the liquid surface, laser energy, and laser beam pattern. The threshold laser fluence for the generation of a liquid jet was 20 J/cm². By increasing the incident laser energy with a fixed laser fluence, the laser focused area increased, which eventually led to an increase in the size of the plasma column. The larger the laser energy, the larger the jet size and the longer the temporal behavior. The laser beam pattern was found to have significant effects on the liquid jet’s velocity, shape, and history.     

Effect of laser spot size on fusion neutron yield in laser--deuterium cluster interactions

The effect of the laser spot size on the neutron yield of table-top nuclear fusion from explosions of a femtosecond intense laser pulse heated deuterium clusters is investigated by using a simplified model, in which the cluster size distribution and the energy attenuation of the laser as it propagates through the cluster jet are taken into account. It has been found that there exists a proper laser spot size for the maximum fusion neutron yield for a given laser pulse and a specific deuterium gas cluster jet. The proper spot size, which is dependent on the laser parameters and the cluster jet parameters, has been calculated and compared with the available experimental data. A reasonable agreement between the calculated results and the published experimental results is found.     

Optimization of laser printing of nanoparticle suspensions for microelectronic applications

Digital printing of interconnects for electronic devices requires processes capable of delivering controlled amounts of conductive inks in a fast and accurate way. Laser-induced forward transfer (LIFT) is an emerging technology that enables controlled printing of voxels of a wide range of inks with micrometer resolution. Its use with high solids content nanoparticle suspensions results in the deposition of voxels shaped as the impinging laser beam. This allows higher processing speeds, increasing the throughput of the technique. However, the optimum conditions for printing spot-like voxels have not been determined, yet. In this work, we perform a systematic study of the main experimental parameters, including laser pulse energy, laser beam dimensions, and gap distance, in order to understand the role that these parameters play in laser printing. Based on these results, we find that there is a narrow fluence range at distances close to the receiving substrate where spot-like voxels are deposited. We also provide a detailed discussion of the possible mechanisms that may lead to the observed features.     

90% pump depletion and good beam quality in a pulse-injection-seeded nanosecond optical parametric oscillator

We measured 90% pump depletion in a singly resonant image-rotating nanosecond optical parametric oscillator that was pulse-injection seeded by a self-generated signal pulse. The oscillator was pumped by an 8 ns duration single-frequency 532 nm pulse from an injection-seeded Q-switched Nd:YAG laser and resonated an 803 nm signal. The pump and pulsed-seed beams had flat-topped spatial fluence profiles with diameters of approximately 6 mm, giving a cavity Fresnel number at 803 nm approaching 400. The beam cleanup effects of the image-rotating cavity produce a far-field signal spatial fluence profile with approximately 60% of its energy falling within the diffraction-limited spot size.     

Micro-ablation on silicon by femtosecond laser pulses focused with an axicon assisted with a lens

Micro-ablation of crystalline silicon was performed by irradiating a silicon substrate with femtosecond laser pulses of wavelengths 786 nm or 393 nm focused using a conical axicon assisted with a convex lens. Focusing the laser beam close to the tip of the axicon by means of the lens significantly improved the efficiency of concentration of laser pulse energy at the central spot of the resulting Bessel-Gaussian intensity distribution. As a result, micron-sized holes were formed with the diameter determined by the ablation threshold in the calculated fluence profile. It is possible to predict hole size from the laser pulse energy and the wavelength. Crystalline particles, a few tens of nanometers in size, were formed near the ablated zone.     

激光脉冲宽度对有质动力加速电子的影响

基于真空中单电子运动模型,编程计算得到了高斯激光脉冲与初始位于激光传播轴上电子的相互作用结果。不同激光参鼍条件下,得到了电子的能量增益与激光强度、焦斑大小和脉冲宽度关系。结果表明,高斯激光脉冲焦斑较大时,电子没有明显的能量增益,高斯激光脉冲焦斑太小时,电子也没有明显的能量增益。电子的能量增益有一个最佳焦斑大小。在相同激光强度下,电子能量增益的最佳焦斑大小随脉冲宽度的增大而增大,但最佳焦斑大小与脉冲宽度的比值基本上是不变的。     

大口径衍射光栅10 ps激光损伤阈值测量（英）

在采用啁啾脉冲放大技术的高功率短脉冲激光装置中,终端衍射光栅的损伤阈值是限制装置输出能力的瓶颈之一。提出了测量大口径光栅损伤阈值的方法。该方法通过在线监测采集大口径光斑的同发近场光强分布情况和相应的光栅损伤图像,并经过一系列后期图像数据处理,建立起能量与损伤点的对应关系,经过一个测试光斑便可获得所有通量下的光栅损伤特性。该测量方法对光斑均匀性没有硬性要求,为损伤测量装置中难以解决的光斑均匀性问题提出了新的应对思路和方法。     

复杂激光脉冲波形的整形

介绍了用时空变换的方法对激光脉冲整形的原理；提出了由于硬边光通量调制器引入的动态的光脉冲强度空间分布的不一致性及其克服的方法，理论上用二维快速傅里叶变换（ＦＦＴ）进行了验证；最后计算了系统光强透过率和光束焦斑大小，调制狭缝宽度的关系，为了显示本系统的复杂脉冲整形能力，在实验上获得了惯性约束核聚变（ＩＣＦ）感兴趣的复杂激光脉冲波形。     

Size distribution control of metal nanoparticles using femtosecond laser pulse train: a molecular dynamics simulation

Microscopic mechanisms and optimization of metal nanoparticle size distribution control using femtosecond laser pulse trains are studied by molecular dynamics simulations combined with the two-temperature model. Various pulse train designs, including subpulse numbers, separations, and energy distributions are compared, which demonstrate that the minimal mean nanoparticle sizes are achieved at the maximal subpulse numbers with uniform energy distributions. Femtosecond laser pulse trains significantly alter the film thermodynamical properties, adjust the film phase change mechanisms, and hence control the nanoparticle size distributions. As subpulse numbers and separations increase, alternation of film thermodynamical properties suppresses phase explosion, favors critical point phase separation, and significantly reduces mean nanoparticle size distributions. Correspondingly, the relative ratio of two phase change mechanisms causes two distinct nanoparticle size control regimes, where phase explosion leads to strong nanoparticle size control, and increasing ratio of critical point phase separation leads to gentle nanoparticles size control.     

合肥光源逐圈束流位置监测系统中的定时系统

定时系统是合肥光源逐圈束流位置监测和相空间测量系统中的重要组成部分，其主要目的是为数据采集卡提供与环内电子束团同步的时钟信号。该系统包含高速ECL时钟成形、分频电路、程控延时电路、控制模块等部分。可实现延时范围0～220ns，最小延时步距0.5ns，调整精度0.1ns，时钟抖动小于200ps。系统控制软件基于客户/服务器结构，操作灵活、方便。     

Study on the effect of laser parameters on wakefield excitation in femtosecond pulsed laser–plasma interaction using PIC method

Propagation of an intense short laser pulse through under-dense plasma can produce huge amplitude plasma wake field. A 3D particle in cell (PIC) method was used to simulate the wakefield generation for different laser parameters such as intensity, pulse duration, spot size and temporal pulse shape. Our study shows that the amplitude of wakefield is increased with laser intensity, but it is decreased with spot size. The results for pulse shape and pulse duration depend on their optimum values.     

On determining the spot size for laser fluence measurements

Energy fluence, defined as pulse energy over irradiated area, is a key parameter of pulsed laser processing. Nevertheless, most of the authors using this term routinely do not realize the problems related to the accurate measurement of the spot size. In the present paper we are aiming to approach this problem by ablating crystalline Si wafers with pulses of a commercial KrF excimer laser (λ = 248 nm, τ = 15 ns) both in vacuum and at ambient atmosphere. For any pulse energy, the size of the ablated area monotonously increases with increasing number of pulses. The difference in the ablated area could be as high as a factor of three when 2000 consecutive pulses impinge on the surface. The existence and extent of the gradual lowering of multi-pulse ablation threshold queries the applicability of routinely used procedure of dividing the pulse energy with the size of the ablated area exposed into either carbon-paper or a piece of Si with one or a few pulses when determining the fluence. A more quantitative way is proposed allowing comparison of results originating from different laboratories.     

Local near field assisted ablation of fused silica

In this contribution we present recent experimental and theoretical results on local near-field assisted laser ablation. Along these lines, we have generated sub-diffraction sized nanostructures on fused silica substrates, exploiting the local near fields of highly ordered triangular gold nanoparticle arrays generated by nanosphere lithography. After preparation, the nanoparticle arrays were irradiated with a single 35 fs long laser pulse with a central wavelength of λ=790 nm. The pulse energy was set to E=3.9 μJ, resulting in a fluence well below the ablation threshold of the fused silica substrates. In addition, 3D electromagnetic simulations using a finite integration technique in time domain have been performed. The simulations demonstrate that indeed the local field in the vicinity of the tips of the triangular nanoparticles overcome the ablation threshold and easily explain the generated nanostructures. Most importantly, the simulations show, that higher order modes contribute to the ablation process. These modes cause ablation along the side edges of the nanoparticles. Finally, we demonstrate, that the optical properties of the triangular nanoparticles, which can be tuned by their morphology, are crucial parameters for the generation of the ablation structures.