Ultrafast and nanosecond laser-induced desorption of positive ions from lithium fluoride single crystals

We compare desorption of positive ions from lithium fluoride single crystals following pulsed laser excitation using either femtosecond (180 fs, 265 nm) or nanosecond (3 ns, 266 nm) sources. Following optical excitation, desorbed ions are mass analyzed using standard time-of-flight techniques. Several important differences between nanosecond and femtosecond excitation are revealed. Femtosecond excitation produces higher kinetic energy Li⁺ than does nanosecond excitation (10 eV vs. 5 eV) while nanosecond excitation yields significant quantities of impurity ions Na⁺ and K⁺, in addition to efficient Li⁺ emission. The Li⁺ desorption threshold is similar for both laser sources. This similarity is a surprising result, as sub-bandgap nanosecond pulses are only likely to excite defect states efficiently (via linear excitation), while the ultrahigh peak-power femtosecond pulses could in principle induce multiphoton and avalanche excitation. Femtosecond excitation results in much less complicated time-of-flight spectra, as predominantly Li⁺ is detected with some H⁺ also observed. We have measured the Li⁺ yield as a function of time delay between two sub-threshold femtosecond laser pulses. We find that the majority of the Li⁺ yield decays rapidly, largely within the fs pulse duration. However, a weak but measurable decay component of approximately 2 ps is indicated.     

Femtosecond time-resolved interferometric microscopy

We describe optical interferometry with 100 fs time resolution and a spatial resolution of approximately one micrometer. Using a pump-probe scheme and a 2D-Fourier transformation algorithm, we are able to retrieve from the interferograms very small changes in the phase and the amplitude of the reflected probe pulses. The performance of the technique is illustrated by measurements of transient and permanent surface modifications of crystalline GaAs after exposure to intense femtosecond laser pulses with fluences near the ablation threshold. PACS 78.47.+p; 42.65.Re; 42.15.Eq; 68.35.Ja     

Electron and photon stimulated desorption of positive ions from alkali halide surfaces

We have observed desorption of positive ions from alkali halides stimulated by low energy electron and photon bombardment. Our experiments include the first measurements of electron stimulated desorption (ESD) of Na⁺ from NaCl and the first measurements of photon stimulated desorption (PSD) of positive ions from NaCl and LiF. The energy dependence data indicate that the initial onset for Na⁺ ejection by ESD occurs at the excitation threshold of the Cl(3s) core level. Similarly for the PSD of positive ions from NaCl and LiF we can relate incident photon beam energy dependent ion yields with the production of substrate core holes. The data provide insight into the mode of initial energy transfer to the solid which leads to desorption. ESD and PSD ion yields were measured to be on the order of 10^?7 ions per incident electron or photon.     

Femtosecond time-resolved energy transfer from CdSe nanoparticles to phthalocyanines

The first real-time observation of the early events during energy transfer from a photoexcited CdSe nanoparticle to an attached phthalocyanine molecule are presented in terms of a femtosecond spectroscopic pump–probe study of the energy transfer in conjugates of CdSe nanoparticles (NPs) and silicon phthalocyanines (Pcs) with 120 fs time resolution. Four different silicon phthalocyanines have been conjugated to CdSe NPs. All of these have proven potential for photodynamic therapy (PDT). In such NP-Pc conjugates efficient energy transfer (ET) from CdSe NPs to Pcs occurs upon selective photoexcitation of the NP moiety. Spectral analysis as well as time-resolved fluorescence up-conversion measurements revealed the structure and dynamics of the investigated conjugates. Femtosecond transient differential absorption (TDA) spectroscopy was used for the investigation of the non-radiative carrier and ET dynamics. The formation of excitons, trapped carriers states, as well as stimulated emission was monitored in the TDA spectra and the corresponding lifetimes of these states were recorded. The time component for energy transfer was found to be between 15 and 35 ps. The ET efficiencies are found to be 20-70% for the four Pc conjugates, according to fluorescence quenching experiments. Moreover, as a result of the conjugation between NP and the Pcs the photoluminescence efficiency of the Pc moieties in the conjugates do not strictly follow the quantum yields of the bare phthalocyanines. PACS 73.63.Bd     

Femtosecond time-resolved ERE-CARS of PM650

We utilize femtosecond time-resolved electronic resonance-enhanced coherent anti-Stokes Raman scattering (ERE-CARS) to investigate new information for pyrromethene 650 (PM650) dye molecules. For this purpose, the vibrational properties of PM650 are registered in diluted solutions of several organisms. We observe a strong Raman vibrational mode with a wavenumber difference of about 48 cm^? 1 in its organic solutions. This may be linked to the intramolecular electron transfer (ICT) process from the aromatic ring to the cyano group in PM650. The influence of the solvent effects on the vibrational dynamics of PM650 is also investigated. The vibrational properties of PM650 dye molecules diluted in polar organic solutions are light solvent-dependent.     

Femtosecond laser-induced damage in reflector

We have investigated the damage for ZrO₂/SiO₂ 800 nm 45° high-reflection mirror with femtosecond pulses. The damage morphologies and the evolution of ablation crater depths with laser fluences are dramatically different from that with pulse longer than a few tens of picoseconds. The ablation in multilayers occurs layer by layer, and not continuously as in the case of bulk single crystalline or amorphous materials. The weak point in damage is the interface between two layers. We also report its single-short damage thresholds for pulse durations ranging from 50 to 900 fs, which departs from the diffusion-dominated scaling. A developed avalanche model, including the production of conduction band electrons (CBE) and laser energy deposition, is applied to study the damage mechanisms. The theoretical results agree well with our measurements.     

Femtosecond laser induced desorption of water from silver nanoparticles

The photodesorption mechanism of H₂O from quartz-supported silver nanoparticles has been studied by femtosecond laser two-pulse correlation and fluence dependence measurements. With the laser wavelength close to the maximum of the (1,1) plasmon resonance of the nanoparticles, the desorption was found to be purely thermal, i.e., induced by coupling of the desorption coordinate to the nanoparticle lattice temperature, both in the low- and the high-coverage regimes. The lattice cooling times of the nanoparticles are in the range of several hundred ps, in accordance with recent time-resolved X-ray measurements. Also observed is a reversible red-shift of the nanoparticle plasmon modes with increasing H₂O coverage which is attributed to dielectric screening. PACS 78.67.-n; 82.53.-k; 65.80.+n     

Femtosecond laser-induced damage of gold films

Single- and multi-shot ablation thresholds of gold films in the thickness range of 31-1400 nm were determined employing a Ti:sapphire laser delivering pulses of 28 fs duration, 793 nm center wavelength at 1 kHz repetition rate. The gold layers were deposited on BK7 glass by an electron beam evaporation process and characterized by atomic force microscopy and ellipsometry. A linear dependence of the ablation threshold fluence F_th on the layer thickness d was found for d ≤ 180 nm. If a film thickness of about 180 nm was reached, the damage threshold remained constant at its bulk value. For different numbers of pulses per spot (N-on-1), bulk damage thresholds of ∼0.7 J cm⁻² (1-on-1), 0.5 J cm⁻² (10-on-1), 0.4 J cm⁻² (100-on-1), 0.25 J cm⁻² (1000-on-1), and 0.2 J cm⁻² (10000-on-1) were obtained experimentally indicating an incubation behavior. A characteristic layer thickness of L_c ≈ 180 nm can be defined which is a measure for the heat penetration depth within the electron gas before electron-phonon relaxation occurs. L_c is by more than an order of magnitude larger than the optical absorption length of α⁻¹ ≈ 12 nm at 793 nm wavelength.     

Femtosecond time-resolved exciton dynamics in CdSe

Transient behavior of the excitonic resonance in CdSe is investigated experimentally by femtosecond pump-probe reflectively measurements. The onset of screening by free carriers is observed to occur in less than 100 femtoseconds.     

Femtosecond laser-induced microstructure in Foturan glass

We report on the microstructure formation in Foturan glass, induced by 1~kHz, 120 femtosecond laser irradiation. It is found that the line-shaped filamentation, not void array tends to be formed in this glass. This is different from our previous experimental results in fused silica and BK7 glasses. A possible mechanism Ag$^+$ captures the free electrons generated by laser, is proposed to explain the observed phenomena.     

Femtosecond laser-induced formation of spikes on silicon

We find that silicon surfaces develop arrays of sharp conical spikes when irradiated with 500-fs laser pulses in SF₆. The height of the spikes decreases with increasing pulse duration or decreasing laser fluence, and scales nonlinearly with the average separation between spikes. The spikes have the same crystallographic orientation as bulk silicon and always point along the incident direction of laser pulses. The base of the spikes has an asymmetric shape and its orientation is determined by the laser polarization. Our data suggest that both laser ablation and laser-induced chemical etching of silicon are involved in the formation of the spikes. Received: 10 September 1999 / Accepted: 7 January 2000 / Published online: 8 March 2000     

Combination of temperature-programmed thermal desorption and laser-induced thermal desorption

The combination of temperature-programmed thermal desorption with heating rates of the order of 1 K s^–1 and laser-induced thermal desorption with of the order of 10¹⁰ K s^–1 has proved to be a suitable method to determine both the frequency factor v and the activation energy E _d of desorption. The systems Ni(110)/N₂ and Ni(110)/CO serve as examples.     

Femtosecond time-resolved measurements of weak localization of light

Time-resolved backscattering of coherent light from a disordered medium under weak localization conditions has been observed for the first time with femtosecond resolution using a light-gating technique based on second-harmonic generation. The time dependence of the observed enhanced backscattering is consistent with simple diffusion theory.     

飞秒激光诱导水光学击穿阈值

为了研究飞秒激光诱导水光学击穿阈值随激光脉冲参数的变化关系,采用四阶RungeKutta方法对飞秒激光诱导水光学击穿的椭球体模型进行了不同脉宽(40～540fs)、波长(400～1200nm)和光斑尺寸(0～200μm)下的数值模拟。通过控制变量法得出阈值光强与这些激光脉冲参数的关系曲线图,据此定性分析了阈值光强与激光脉冲参数的变化特征趋势。应用光强与功率、能量、辐照曝光量和电场强度之间的关系,得到了它们随激光脉冲参数脉宽、波长和光斑尺寸的动态关系,这为进一步研究飞秒激光与水和含水介质的相互作用提供了理论依据。     

飞秒激光诱导水光学击穿阈值

为了研究飞秒激光诱导水光学击穿阈值随激光脉冲参数的变化关系,采用四阶Runge-Kutta方法对飞秒激光诱导水光学击穿的椭球体模型进行了不同脉宽（40~540 fs）、波长(400~1 200 nm)和光斑尺寸（0~200 μm）下的数值模拟。通过控制变量法得出阈值光强与这些激光脉冲参数的关系曲线图,据此定性分析了阈值光强与激光脉冲参数的变化特征趋势。应用光强与功率、能量、辐照曝光量和电场强度之间的关系,得到了它们随激光脉冲参数脉宽、波长和光斑尺寸的动态关系,这为进一步研究飞秒激光与水和含水介质的相互作用提供了理论依据。     

Femtosecond laser-induced blazed periodic grooves on metals

In this Letter, we generate laser-induced periodic surface structures (LIPSSs) on platinum following femtosecond laser pulse irradiation. For the first time to our knowledge, we study the morphological profile of LIPSSs over a broad incident angular range, and find that the morphological profile of LIPSSs depends significantly on the incident angle of the laser beam. We show that LIPSS grooves become more asymmetric at a larger incident angle, and the morphological profile of LIPSSs formed at an incident angle over 55° eventually resembles that of a blazed grating. Our study suggests that the formation of the blazed groove structures is attributed to the selective ablation of grooves through the asymmetric periodic surface heating following femtosecond pulse irradiation. The blazed grooves are useful for controlling the diffraction efficiency of LIPSSs.     

Femtosecond laser-induced nanostructure-covered large-scale waves on metals

Through femtosecond (fs) laser pulse irradiation (pulse duration: 65 fs, central wavelength: 800 nm, and repetition rate: 250 Hz), we investigate the morphological evolution of fs laser-induced periodic surface structure on Au and Pt, called a nanostructure-covered large-scale wave (NC-LSW) with a period of tens of microns, densely covered by iterating stripe patterns of nanostructures and microstructures. We show that the surface morphology of NC-LSW crucially depends on the fluence of the laser, the number of irradiating pulses, and the incident beam angle. Our experimental observations allow us to establish a three-step model for the NC-LSW formation: the formation of laser-induced surface unevenness, inhomogeneous energy deposition due to the interference between the incident light and the scattered field, and nonuniform energy deposition due to shielding by the peaks of LSW.