Dynamics of phase transitions induced by femtosecond laser pulse irradiation of indium phosphide

The structural transformation dynamics of single-crystalline indium phosphide (InP) irradiated with 150 fs laser pulses at 800 nm has been investigated by means of time-resolved reflectivity measurements covering a time window from 150 fs up to 500 ns. The results obtained show that for fluences above a threshold of 0.16 J/cm² thermal melting of the material occurs on the timescale of 1–2 ps. The evolution of the reflectivity on a longer timescale reveals the reflectivity of the liquid phase and shows resolidification times typically around 10–30 ns after which an amorphous layer several tens of nanometers thick is formed on the surface. This amorphous layer significantly alters the optical properties of the surface and finally leads to a reduced ablation threshold for subsequent laser pulses. Single-pulse ablation at higher fluences (>0.23 J/cm²) is preceded by an ultrafast phase transition (non-thermal melting) occurring within 400 fs after the arrival of the pulse to the surface. PACS 79.20.Ds; 78.47.+p; 64.70.-p     

Ultrafast two-color ablation of fused silica

Two ultrafast laser pulses at the fundamental Ti:sapphire laser wavelength of 800 nm and the second harmonic at 400 nm were used to study the temporal evolution of the transmissivity in fused silica and resulting material ablation. It was observed that there was a sharp drop in the transmissivity of the probe pulse at zero delay between the two pulses, indicating that there was enhanced absorption/reflection due to the creation of defect states or free electron plasma by the pump pulse. Subsequent atomic force microscopy measurements of the ablated holes revealed that the ablated volume increased by about 50% when the separations of the two pulses are within 300 fs. Two-color machining of channels at the surface also showed a similar increase in the machined depth and width when the pulses are overlapped in time. PACS 52.38.Mf; 78.47.+p; 79.20.Ds     

Glassy carbon layer formed in diamond-like carbon films with femtosecond laser pulses

We report the first observation, to our knowledge, of a glassy carbon (GC) layer modified from diamond-like carbon (DLC) films with femtosecond (fs) laser pulses. The GC layer, which is confirmed by Raman spectroscopy, is produced most efficiently at low laser fluence near the ablation threshold of the DLC films. This surface modification depends little on the laser polarization and wavelength used. The fs laser-induced GC layer should be a new thin-film material useful for a variety of engineering applications due to its characteristics similar to those of DLC and the additional properties inherent in GC. PACS 61.80.Ba; 79.20.Ds; 42.62.Cf     

Ultra-short laser ablation of metals and semiconductors: evidence of ultra-fast Coulomb explosion

We have studied ultra-fast laser ablation of Si and a metal via the neutral and ion yield, the energy distribution of emitted neutrals and the charge distribution as a function of the laser pulse width. Two processes, one leading to the ejection of fast (3–7 eV), the other to slow thermal particles, can be identified. The origin of the first process can be correlated with laser pulse widths (or pump–probe delays) and processes on a time scale below 100 fs. Results for Si confirm recent findings for Coulomb explosion (CE) and we show for the first time that CE exists as a mechanism of material removal from metals for ultra-short laser pulses. PACS 06.60.Jn; 79.20.Ds; 79.60.Bm; 42.62.Fi; 71.20.-b     

Mechanisms of femtosecond laser ablation of dielectrics revealed by double pump–probe experiment

We study experimentally the electronic excitation mechanisms involved in the breakdown and ablation of wide band gap dielectrics. A femtosecond pump–probe interferometry technique, with 100 fs temporal resolution, allows measuring the modification of refractive index induced by ultra-short intense laser pulses. To get more information in the complex process of excitation and relaxation mechanisms involved during and after the interaction, we use a sequence of two excitation pulses: a first short pulse at 400 nm excites a controlled density of carriers, and a second one at 800 nm with variable pulse duration, from 50 fs to 10 ps, reaches an excited solid. In Al₂O₃, we show that the total density of carriers never exceeds the sum of the densities excited by the two pulses sent independently. This means that the second pulse deposits further energy in the material by heating the previously excited carriers, and that no electronic multiplication occurs. On the other hand, in SiO₂, it is possible, under specific conditions, to observe an increase of carrier density due to impact ionization. All these results demonstrate that the avalanche process, which is often invoked in the laser breakdown literature, does not play a dominant role in optical breakdown induced by short pulses.     

Theoretical investigation of laser pulse width dependence in a thermal confinement regime

Previous molecular dynamics (MD) simulations of ultraviolet (UV) laser ablation demonstrate the distinct dependence of material ejection on laser fluence and laser pulse duration. In this paper, we examine the pulse width dependence when the laser pulse widths are appropriate for the thermal confinement regime. We perform MD simulations of laser ablation with a laser pulse duration of 1 ns and compare with a pulse width of 150 ps as in previous simulations. The simulations confirm that the pulse width in thermal confinement regime does not dramatically influence the molecular ejection mechanism. The simulations reveal differentiations, however, in plume composition and the ablation threshold value. PACS 02.70.Ns; 61.80.Az; 79.20.Ap     

Short-pulse laser ablation of solids: from phase explosion to fragmentation

The mechanisms of laser ablation in silicon are investigated close to the threshold energy for pulse durations of 500 fs and 50 ps. This is achieved using a unique model coupling carrier and atom dynamics within a unified Monte Carlo and molecular-dynamics scheme. Under femtosecond laser irradiation, isochoric heating and rapid adiabatic expansion of the material provide a natural pathway to phase explosion. This is not observed under slower, nonadiabatic cooling with picosecond pulses where fragmentation of the hot metallic fluid is the only relevant ablation mechanism.     

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     

Femtosecond laser pulse ablation of GaAs and InP: studies utilizing scanning and transmission electron microscopy

Single pulse laser ablation of GaAs and InP using 130 fs light pulses at 800 nm was studied with various techniques, in particular, scanning and transmission electron microscopies. The final state of the material near the laser-ablated region following femtosecond ablation was characterized in detail for selected laser fluences. Threshold ablation laser fluences were also obtained for both compounds. PACS 61.80.Ba; 64.60.-i; 79.20.Ds     

Laser drilling of high aspect ratio holes in copper with femtosecond,picosecond and nanosecond pulses

Deep laser holes were drilled in copper sheets using various pulse lengths and environments. By recording the intensity on a photodiode placed under the sample while drilling the holes, we obtained the number of pulses to drill through the sheet as a function of pulse length and energy. The entrance diameter of the holes was successfully predicted using a Gaussian approximation and a material removal fluence threshold of 0.39 J/cm² for a pulse length of 150 fs. From cross sections of the holes, the morphology of the inside walls was observed and shows an increase in the amount of molten material with pulse length. A transition pulse length is defined as the point at which the laser affected material goes from being mainly vaporized to mainly melted. This transition occurs near ∼10 ps, which corresponds approximately to the electron–phonon relaxation time for copper. PACS 62.20.Mk; 62.25.+g; 79.20.Ds     

超短脉冲激光烧蚀石墨产生的喷射物的时间分辨发射光谱研究

本文使用不同激光能流(18 J/cm²–115 J/cm²)和脉冲宽度(50 fs–4 ps)的超短脉冲激光在真空中(4×10^-4 Pa)烧蚀高定向热解石墨. 通过测量烧蚀喷射物的时间分辨发射光谱研究喷射物的超快时间演化. 在喷射物发射光谱中, 观察到了C₂基团的天鹅带光谱系统, 416 nm附近C₁₅基团的由电子能级¹Σ_u⁺ 和¹Σ_g⁺之间的振动跃迁产生的光谱峰以及连续谱. 50 fs, 115 J/cm²的脉冲激光烧蚀产生的喷射物的连续谱的强度衰减分为快速下降和慢速下降两个阶段(以20 ns时间延迟为分界). 这表明连续谱是由两种不同的组分贡献的. 快速下降阶段, 连续谱主要由碳等离子体通过韧致辐射产生; 慢速下降阶段, 连续谱主要由烧蚀后期产生的大颗粒碳簇的热辐射贡献. 实验结果还揭示了激光能流的提高, 会明显增加喷射物中碳等离子体和激发态C₂的含量, 但对质量稍大的C₁₅的影响较小; 此外, 50 fs脉冲激光烧蚀产生的连续谱的存在时间会随着激光能流的减小而增大, 这说明低能流更有利于在烧蚀后期产生碳簇. 脉宽主要影响喷射物连续谱的时间演化. 4 ps脉冲激光烧蚀产生的连续谱的整个时间演化过程明显慢于50 fs脉冲产生的连续谱.     

Femtosecond laser ablation of silicon–modification thresholds and morphology

We investigated the initial modification and ablation of crystalline silicon with single and multiple Ti:sapphire laser pulses of 5 to 400 fs duration. In accordance with earlier established models, we found the phenomena amorphization, melting, re-crystallization, nucleated vaporization, and ablation to occur with increasing laser fluence down to the shortest pulse durations. We noticed new morphological features (bubbles) as well as familiar ones (ripples, columns). A nearly constant ablation threshold fluence on the order of 0.2 J/cm² for all pulse durations and multiple-pulse irradiation was observed. For a duration of ≈100 fs, significant incubation can be observed, whereas for 5 fs pulses, the ablation threshold does not depend on the pulse number within the experimental error. For micromachining of silicon, a pulse duration of less than 500 fs is not advantageous. Received: 4 December 2000 / Revised version: 29 March 2001 / Published online: 20 June 2001     

Ad-hoc design of temporally shaped fs laser pulses based on plasma dynamics for deep ablation in fused silica

We have analyzed the ablation depth yield of fused silica irradiated with shaped pulse trains with a separation of 500 fs and increasing or decreasing intensity envelopes. This temporal separation value is extracted from previous studies on ablation dynamics upon irradiation with transform-limited 100 fs laser pulses. The use of decreasing intensity pulse trains leads to a strong increase of the induced ablation depth when compared to the behavior, at the same pulse fluence, of intensity increasing pulse trains. In addition, we have studied the material response under stretched (500 fs, FWHM) and transform-limited (100 fs, FWHM) pulses, for which avalanche or multiphoton ionization respectively dominates the carrier generation process. The comparison of the corresponding evolution of the ablated depth vs. fluence suggests that the use of pulse trains with decreasing intensity at high fluences should lead to enhanced single exposure ablation depths, beyond the limits corresponding to MPI- or AI-alone dominated processes.     

Femtosecond pulsed laser ablation of thin gold film

Laser micromachining on 1000 nm-thick gold film using femtosecond laser has been studied. The laser pulses that are used for this study are 400 nm in central wavelength, 150 fs in pulse duration, and the repetition rate is 1 kHz. Plano-concave lens with a focal length of 19 mm focuses the laser beam into a spot of 3 μm (1/e² diameter). The sample was translated at a linear speed of 400 μm/s during machining. Grooves were cut on gold thin film with laser pulses of various energies. The ablation depths were measured and plotted. There are two ablation regimes. In the first regime, the cutting is very shallow and the edges are free of molten material. While in the second regime, molten material appears and the cutting edges are contaminated. The results suggest that clean and precise microstructuring can be achieved with femtosecond pulsed laser by controlling the pulse energy in the first ablation regime.     

Machining of submicron structures on metals and semiconductors by ultrashort UV-laser pulses

Ablation of submicron structures on copper and silicon by short ultraviolet laser pulses (0.5–50 ps, 248 nm) is presented. Features like periodic line structures with a line-spacing below 400 nm, and holes with characteristic sizes well below 1 µm are produced on the sample surface by single laser shot exposure. The structures are projection printed by a Schwarzschild-objective (N.A.=0.4) in air environment. The morphology of ablation sites made with different pulse durations (0.5 ps, 5 ps, 50 ps) is discussed in terms of thermal diffusion effects.     

高温合金不同脉宽超快激光作用下多脉冲去除阈值

实验研究了激光脉冲宽度和脉冲个数对镍基高温合金材料去除阈值的影响,分别在290 fs,1 ps和7 ps脉宽的激光下,使用1,10,50,100,300,500和1000个不同能量的激光脉冲辐照高温合金样品表面。实验结果表明,烧蚀坑尺寸会随脉冲数的增加而增加,而脉冲宽度的增加会加大脉冲个数对烧蚀坑直径的影响。通过烧蚀坑直径的平方值与激光脉冲能量之间存在的对数关系,得到了不同脉冲宽度下镍基高温合金的多脉冲材料阈值。3种不同脉宽下的高温合金多脉冲去除阈值都存在显著的累积效应。根据去除阈值计算得到290 fs,1 ps和7 ps脉宽下的累积效应系数分别为0.88,0.86和0.78。     

Time-resolved dynamics analysis of nanoparticles applying dual femtosecond laser pulses

The evolution of a fs laser generated plume on copper was studied by dual laser pulses. The plume generated by the first pulse (620 nm) was excited by the second, delayed pulse (310 nm). The actual state of the plume was monitored by detecting the intensities of the emitted light and the reflected delayed pulse from the interaction range, i.e. 0–150 μm above the surface. Four peaks were observed in the 0–1400 ps time range and assigned to appearance of electrons, ions, atomic species and nanoparticles. Accordingly, the timing of the creation and ejection of these species was determined. By integrating the intensity of the nanoparticle peak, the production yield of the nanoparticles and its dependence on the ablating laser fluence was calculated. The ablation products were deposited on a Si substrate, too, and analyzed by atomic force microscopy and scanning electron microscopy. The results of the deposition and the dual-pulse experiments are in good agreement with the theory. PACS 52.38.Mf; 79.20.Ds; 61.80.Ba     

Femtosecond,picosecond and nanosecond laser ablation of solids

Laser ablation of solid targets by 0.2–5000 ps Ti: Sapphire laser pulses is studied. Theoretical models and qualitative explanations of experimental results are presented. Advantages of femtosecond lasers for precise material processing are discussed and demonstrated.     

Onset of crater formation during short pulse laser ablation

We report morphologic changes of metallic surfaces at the onset of ablation, starting from gentle ablation to the emergence of ablation craters. The evolution of both observed melting zones and of ablation craters therein are investigated in dependence of the ablation laser fluence for nanosecond ultraviolet laser pulses. Further, consequences of crater formation for cluster synthesis within the released atomic vapor are pointed out. PACS 52.38.Mf; 79.20.Ds; 65.40.De     

Transient reflectivity and transmission changes during plasma formation and ablation in fused silica induced by femtosecond laser pulses

We have studied the plasma formation and ablation dynamics in fused silica upon irradiation with a single 120 fs laser pulse at 800 nm by using fs-resolved pump-probe microscope. It allows recording images of the laser-excited surface at different time delays after the arrival of the pump pulse. This way, we can extract both the temporal evolution of the surface reflectivity and transmission, at 400 nm, for different spatial positions in the spots (and thus for different local fluences) from single series of images. At fluences well above the visible ablation threshold, a fast and large increase of the reflectivity is induced by the formation of a dense free-electron plasma. The maximum reflectivity value is reached within ≈1.5 ps, while the normalized transmission decreases within ≈400 fs. The subsequent temporal evolution of both transient reflectivity and transmission are consistent with the occurrence of surface ablation. In addition, the time-resolved images reveal the existence of a free-electron plasma distribution surrounding the visible ablation crater and thus formed at local fluences below the ablation threshold. The lifetime of this sub-ablation plasma is ≈50 ps, and its maximum electron density amounts to 5.5×10²² cm⁻³.