Surface topography (nano-sized hillocks) and particle emission of metals, dielectrics and semiconductors during ultra-short-laser ablation: Towards a coherent understanding of relevant processes

By combining new studies of the surface topography and the emission characteristics of particles during interaction of ultra-short-laser radiation with surfaces, in particular during laser ablation, three different types of general processes (sub 100 fs electronic processes like Coulomb explosion (CE) or field ion emission by surface optical rectification (SOR), processes related to electronic plasma (FEP) formation (typically a few hundred fs time scale) and thermal ablation (TA)) could be identified to explain ultra-short-laser ablation of matter at laser intensities around the ablation threshold. In particular, the identification of the unique appearance of individual, localized nano-hillocks, typically a few nm in height and with a diameter below typically 50 nm, can be regarded as characteristic for a strong localized potential energy deposition to the electronic system resulting in CE or SOR. The observation and possibility of CE even on metals has implications beyond the field of laser ablation. A remarkable result observed concerns the similarities between laser ablation and sputtering with highly charged ions.     

Radiation-pressure acceleration of ion beams from nanofoil targets: the leaky light-sail regime

A new ion radiation-pressure acceleration regime, the "leaky light sail," is proposed which uses sub-skin-depth nanometer foils irradiated by circularly polarized laser pulses. In the regime, the foil is partially transparent, continuously leaking electrons out along with the transmitted laser field. This feature can be exploited by a multispecies nanofoil configuration to stabilize the acceleration of the light ion component, supplementing the latter with an excess of electrons leaked from those associated with the heavy ions to avoid Coulomb explosion. It is shown by 2D particle-in-cell simulations that a monoenergetic proton beam with energy 18 MeV is produced by circularly polarized lasers at intensities of just 101? W/cm2. 100 MeV proton beams are obtained by increasing the intensities to 2 × 102? W/cm2.     

Identification of ultra-fast electronic and thermal processes during femtosecond laser ablation of Si

Ultra-fast electronic and thermal processes for the energy deposition mechanism during femtosecond laser ablation of Si have been identified by means of atomic force microscopy and Raman scattering techniques. For this purpose, Si targets were exposed with 800-nm, 25-fs Ti:sapphire laser pulses for different laser fluencies in air and under UHV (ultra high vacuum) conditions. Various nano- and microstructures on the surface of the irradiated samples are revealed by a detailed surface topography analysis. Ultra-fast electronic processes are dominant in the lower-fluence regime. Therefore, by starting from the ablation threshold three different fluence regimes have been chosen: a lower-fluence regime (0.06–0.5 J?cm^?2 single-shot irradiation under UHV condition and 0.25–2.5 J?cm^?2 single-shot irradiation in ambient condition), a moderate-fluence regime (0.25–1.5 J?cm^?2 multiple-shot irradiation), and a higher-fluence regime (2.5–3.5 J?cm^?2 multiple-shot irradiation). Around the ablation threshold fluence, most significant features identified at the Si surface are nanohillock-like structures. The appearance of these nanohillocks is regarded as typical features for fast electronic processes (correlated with existence of hot electrons) and is explained on the basis of Coulomb explosion. The growth of these typical features (nanohillocks) by femtosecond laser irradiation is an element of novelty. At moderate irradiation fluence, a ring-shaped ablation with larger bumps and periodic surface structures is observed and is considered as a footprint of ultra-fast melting. Further increase in the laser fluence, i.e. a higher-fluence regime, resulted in strong enhancement of the thermal process with the appearance of larger islands. The change in surface topography provides an innovative clue to differentiate between ultra-fast electronic processes, i.e. Coulomb explosion (sub-100 fs) at a lower-fluence regime and ultra-fast melting (hundreds of fs) at a moderate-fluence regime, and slow thermal processes (ps time scale) at a higher-fluence regime. These fast electronic and thermal processes are well correlated to structural and crystallographic alterations, inferred from Raman spectroscopy.     

Double-pulse femtosecond laser ablation of the surface of stainless steel with variable interpulse delays

Spectral studies of optical emission from plumes produced via ablation of the surface of stainless steel in the phase explosion regime at different incident fluences by a pair of collinear degenerate femtosecond laser pulses, separated by variable delay time of 0.01–1.5 ns, demonstrate a drastic decrease in atomic emission intensities in a subnanosecond range. This effect was related to “bulk” absorption of the second pump pulse in ablative plumes with near-critical density, achieved during their hydrodynamic expansion on a subnanosecond timescale.     

Identification of non-thermal and thermal processes in femtosecond laser-ablated aluminum

Non-thermal and thermal processes due to femtosecond laser ablation of aluminum (Al) at low, moderate, and high-fluence regimes are identified by Atomic Force Microscope (AFM) surface topography investigations. For this purpose, surface modifications of Al by employing 25 fs Ti: sapphire laser pulses at the central wavelength of 800 nm have been performed to explore different nano- and microscale features such as hillocks, bumps, pores, and craters. The mechanism for the formation of these diverse kinds of structures is discussed in the scenario of three ablation regimes. Ultrafast electronic and non-thermal processes are dominant in the lower fluence regime, whereas slow thermal processes are dominant at the higher fluence regime. Therefore, by starting from the ablation threshold three different fluence regimes have been chosen: a lower fluence regime (0.06–0.5 J cm^?2 single-shot irradiation under ultrahigh vacuum condition and 0.25–2.5 J cm^?2 single-shot irradiation in ambient condition), a moderate-fluence regime (0.25–1.5 J cm^?2 multiple-shot irradiation), and a high-fluence regime 2.5–3.5 J cm^?2 multiple-shot irradiation. For the lower fluence (gentle ablation) regime, around the ablation threshold, the unique appearance of individual, localized Nano hillocks typically a few nanometers in height and less than 100 nm in diameter are identified. These Nano hillock-like features can be regarded as a nonthermal, electronically induced phase transition process due to localized energy deposition as a result of Coulomb explosion or field ion emission by surface optical rectification. At a moderate-fluence regime, slightly higher than ablation threshold multiple-pulse irradiation produces bump-formation and is attributed to ultrafast melting (plasma formation). The high-fluence regime results in greater rates of material removal with highly disturbed and chaotic surface of Al with an appearance of larger protrusions at laser fluence well above the ablation threshold. These nonsymmetrical shapes due to inhomogeneous nucleation, cluster formation, and resolidification of a metallic surface after melting are attributable to slow thermal processes (ps time scale).     

Theoretical studies of ultrafast ablation of metal targets dominated by phase explosion

Ultrashort pulse laser ablation of metallic targets is investigated theoretically through establishing a modified two-temperature model that takes into account both the temperature dependent electron–lattice coupling and the electron–electron-collision dominated electron diffusion processes for higher electron temperature regime. The electron–lattice energy coupling rate is found to reduce only slowly with increasing pulse duration, but grow rapidly with laser fluence, implying that the melting time of metallic materials decreases as the laser intensity increases. By taking phase explosion as the primary ablation mechanism, the predicted dependences of ablation rates on laser energy fluences for different laser pulse widths match very well with the experimental data. It is also found that during phase explosion the ablation rate is almost independent of the pulse width, whereas the ablation threshold fluence increases with the pulse duration even for femtosecond pulses. These theoretical results should be useful in having proper understanding of the ablation physics of ultrafast micromachining of metal targets. PACS 52.50.Jm; 61.80.Az; 72.15.Cz; 79.20.Ap; 79.20.Ds     

Dominance of radiation pressure in ion acceleration with linearly polarized pulses at intensities of 10(21) W cm(-2)

A novel regime is proposed where, by employing linearly polarized laser pulses at intensities 10(21) W cm(-2) (2 orders of magnitude lower than discussed in previous work [T. Esirkepov et al., Phys. Rev. Lett. 92, 175003 (2004)]), ions are dominantly accelerated from ultrathin foils by the radiation pressure and have monoenergetic spectra. In this regime, ions accelerated from the hole-boring process quickly catch up with the ions accelerated by target normal sheath acceleration, and they then join in a single bunch, undergoing a hybrid light-sail-target normal sheath acceleration. Under an appropriate coupling condition between foil thickness, laser intensity, and pulse duration, laser radiation pressure can be dominant in this hybrid acceleration. Two-dimensional particle-in-cell simulations show that 1.26 GeV quasimonoenergetic C(6+) beams are obtained by linearly polarized laser pulses at intensities of 10(21) W cm(-2).     

Sub–damage–threshold femtosecond laser ablation from crystalline Si: surface nanostructures and phase transformation

Surface structures and structural transformations are investigated upon femtosecond laser ablation (800 nm, 120 fs) from crystalline silicon (100) targets placed under ultra-high vacuum. After repetitive illumination with several thousand laser pulses at intensities below the single shot damage threshold, at normal incidence, the crater morphology indicates the development of periodic structures at the crater bottom, with the orientation depending on the laser beam polarization. Periods of 200 nm and 600–700 nm, respectively, are shorter than the laser wavelength and appear as a result of surface instability. The ablation dynamics monitored by time-of-flight mass spectrometry shows the emission of positive silicon ions and clusters with kinetic energies of about 7 eV. Raman spectroscopy reveals phase transformations in the irradiated spot from Si-I to the polymorphs Si-III, Si-IV, Si-XII, and amorphous silicon as well as a stable, uncommon phase of hexagonal Si-wurzite. PACS 61.80 Ba; 81.05 Cy; 82.80.Rt; 81.65.Cf; 78.30 Am     

Laser ablation of dental materials using a microsecond Nd:YAG laser

The action of microsecond laser pulses with a wavelength of 1064 nm on dental tissues (enamel and dentin) and various dental materials used for tooth replacement and filling (ceramics, metal alloys, and composites) is studied. It is demonstrated that the ablation thresholds of all of the dental materials are significantly lower than the threshold laser fluences for the dental tissue (E _thr = 200–300 J/cm²). At the laser fluences that do not allow ablation and damage of the dental tissues, the dental materials are effectively removed at a rate of no greater than 40 μm per pulse. It is shown that the laser ablation of the materials under study involves two processes (evaporation and volume explosion) depending on the optical density. The results obtained indicate that the laser radiation with a wavelength of 1064 nm and the microsecond pulse duration is promising for dental applications, since it allows effective cleaning of the tooth surface from various dental materials in the absence of the damages of dental tissues.     

Electronic mechanism of ion expulsion under UV nanosecond laser excitation of silicon: Experiment and modeling

We present experimental and modeling studies of UV nanosecond pulsed laser desorption and ablation of (111) bulk silicon. The results involve a new approach to the analysis of plume formation dynamics under high-energy photon irradiation of the semiconductor surface. Non-thermal, photo-induced desorption has been observed at low laser fluence, well below the melting threshold. Under ablation conditions, the non-thermal ions also have a high concentration. The origin of these ions is discussed on the basis of electronic excitation of Si surface states associated with the Coulomb explosion mechanism. We present a model describing dynamics of silicon target excitation, heating and charge-carrier transport. PACS 52.38.Mf; 68.34.Tj; 68.35.Rh; 79.20.Ds     

Thermodynamic evolution of materials during laser ablation under pico and femtosecond pulses

Using molecular-dynamics, we study the thermodynamic evolution of a simple two-dimensional Lennard–Jones system during laser ablation for pulse durations ranging from 200 fs to 400 ps. We briefly review results previously obtained for fs pulses where the evolution of the material was shown to be solely a function of the locally absorbed energy (provided that only thermal effects are important), i.e., is adiabatic. For longer pulses (100 and 400 ps) the situation becomes more complex, as the relaxation path also depends on the position in the target and on the timescale on which expansion occurs. We show that, in contrast to fs pulses, the material ejected following ps laser irradiation does not enter the liquid–vapor metastable region before ablation occurs, hence showing that phase explosion is not the dominant mechanism in this regime. Following on from previous work, we propose that trivial fragmentation is the main ablation mechanism. PACS 79.20.Ds; 79.20.Ap; 61.80.Az     

准分子激光轰击Y-Ba-Cu-O高温超导靶的空间分辨光谱研究

采用WP4-光学多道分析仪对准分子激光轰击Y_1Ba_2Cu_3O_x超导靶产生的等离子体辐射进行了空间分辨测量和研究。实验结果表明,在靶面的邻近区(d<0.4mm),等离子体辐射为较强的连续谱,并迭加有Y、Ba原子和Y~+、Ba~+离子基态电子跃迁的自吸收线。Y、Ba、Cu原子和相应的一价离子以及金属氧化物分子激发态的发射谱线仅在距靶面为0.4mm以外的区域出现。光谱的测量结果支持靶面表层发生爆炸、出射分子簇团和固体微粒的激光烧蚀沉积动力学机制解释。     

Comparison of the laser ablation process on Zn and Ti using pulsed digital holographic interferometry

Pulsed digital holographic interferometry has been used to compare the laser ablation process of a Q-switched Nd-YAG laser pulse (wavelength 1064 nm, pulse duration 12 ns) on two different metals (Zn and Ti) under atmospheric air pressure. Digital holograms were recorded for different time delays using collimated laser light (532 nm) passed through the volume along the target. Numerical data of the integrated refractive index field were calculated and presented as phase maps. Intensity maps were calculated from the recorded digital holograms and are used to calculate the attenuation of the probing laser beam by the ablated plume. The different structures of the plume, namely streaks normal to the surface for Zn in contrast to absorbing regions for Ti, indicates that different mechanisms of laser ablation could happen for different metals for the same laser settings and surrounding gas. At a laser fluence of 5 J/cm², phase explosion appears to be the ablation mechanism in case of Zn, while for Ti normal vaporization seems to be the dominant mechanism.     

Interface kinetics during pulsed laser ablation

This work investigates evaporation kinetics -- the relation between the surface temperature and pressure during excimer laser ablation. Nickel targets are ablated by excimer laser pulses in a laser fluence range between 1 and 6 J/cm², with the upper limit exceeding the threshold of phase explosion (5 J/cm²). The surface pressure is determined with a polyvinylidene fluoride (PVDF) piezoelectric transducer. When phase explosion occurs, the surface temperature is known to be near the thermodynamic critical temperature, therefore, by measuring the surface pressure, the surface temperature-pressure relation is determined at the threshold fluence of phase explosion. The surface temperature and the threshold fluence of phase explosion are also estimated from the measured velocity of the vapor plume and gas dynamics calculations. It is shown that, during excimer laser ablation, the temperature and pressure relation deviates significantly from the equilibrium kinetic relation.     

Optical transmission and reflection of aluminum film irradiated by nanosecond laser beam and experimental studying of phase-explosion

In this paper we present evidence for a phase explosion during the laser-induced ablation process by studying the optical reflectivity of the ablated plume. The ablation was produced by irradiating thin film aluminum coated on a quartz substrate with a single pulse laser beam in ambient air. The laser pulse was provided by the second harmonic of a Q-switched Nd:YAG laser with ∼10 ns pulse duration. The transmission of a low power He–Ne laser beam through the hot ablated material plume and its reflection (from the front surface, and rear surface of aluminum film) were also monitored during the duration of the ablation event. The results show that the front surface reflectivity is enhanced at an early time of ablation which is described as strong evidence for the creation of a phase explosion in this process.     

Laser ablation of carbon at the threshold of plasma formation

The ionization of laser-ablated vapours with lasers producing ns duration pulses at various wavelengths has been studied in order to understand the mechanisms of the vapour-plasma transition. It has been established that there are several regimes characterizing the laser-target interaction which depend on laser intensity, wavelength, and pulse duration. The range of laser intensities for optimal laser evaporation is determined by the condition of transparent vapours. The intensity range is upper-limited by the opaque plasma formation due to vapour optical breakdown. Results are given for laser evaporation of graphite with Nd:YAG laser (1.064 7m), KrF laser (248 nm) and ArF laser (193 nm). For the UV laser wavelength the regime of skin-effect interaction was proposed as the mechanism of ion acceleration, and the range of validity of the skin-effect mode was established. With UV lasers the interaction has a bimodal nature: the interaction may proceed initially in the skin effect regime, resulting in a few high-energy ions, until hydrodynamic expansion begins at a later stage. The skin-effect interaction at the initial stage of the UV laser pulse gives the first, to our knowledge, explanation for the acceleration of ions up to ~100 eV at low laser intensities of 10⁸-10⁹ W/cm² and ns-range pulse duration.     

Near QED regime of laser interaction with overdense plasmas

Interaction of laser plulses with intensities up to 10²⁵?W/cm² with overdense plasma targets is investigated via three-dimensional particle-in-cell simulations. At these intensities, radiation of electrons in the laser field becomes important. Electrons transfer a significant fraction of their energy to γ-photons and obtain strong feedbacks due to radiation reaction (RR) force. The RR effect on the distribution of laser energies among three main species: electrons, ions and photons is studied. The RR and electron-positron pair creation are implemented by a QED model. As the laser intensity inreases, the ratio of laser energy coupled to electrons drops while the one for γ-photons reaches up to 35%. Two distinctive plasma density regimes of the high-density carbon target and low-density solid hydrogen target are identified from the laser energy partitions and angular distributions of photons. The power-laws of absorption efficiency versus laser intensity and the transition of photon divergence are revealed. These show enhanced generation of γ-photon beams with improved collimation in the relativistically transparent regime. A new effect of transverse trapping of electrons inside the laser field caused by the RR force is observed: electrons can be unexpectedly confined by the intense laser field when the RR force is comparable to the Lorentz force. Finally, the RR effect and different regions of photon emission in laser-foil interactions are clarified.     

Impact of the lasr wavelength and fluence on the ablation rate of aluminium

The dependence of the ablation rate of aluminium on the fluence of nanosecond laser pulses with wavelengths of 532 nm and respectively 1064 nm is investigated in atmospheric air. The fluence of the pulses is varied by changing the diameter of the irradiated area at the target surface, and the wavelength is varied by using the fundamental and the second harmonic of a Q-switched Nd-YAG laser system. The results indicate an approximately logarithmic increase of the ablation rate with the fluence for ablation rates smaller than ∼6 μm/pulse at 532 nm, and 0.3 μm/pulse at 1064 nm wavelength. The significantly smaller ablation rate at 1064 nm is due to the small optical absorptivity, the strong oxidation of the aluminium target, and to the strong attenuation of the pulses into the plasma plume at this wavelength. A jump of the ablation rate is observed at the fluence threshold value, which is ∼50 J/cm² for the second harmonic, and ∼15 J/cm² for the fundamental pulses. Further increasing the fluence leads to a steep increase of the ablation rate at both wavelengths, the increase of the ablation rate being approximately exponential in the case of visible pulses. The jump of the ablation rate at the threshold fluence value is due to the transition from a normal vaporization regime to a phase explosion regime, and to the change of the dimensionality of the hydrodynamics of the plasma-plume.