Generation of nanospikes via laser ablation of metals in liquid environment and their activity in surface-enhanced Raman scattering of organic molecules

The formation of dense arrays of nanospikes occurs under laser ablation of bulk targets (Ag, Au, Ta, Ti) immersed in liquids such as water or ethanol. The average height of spikes is 50 nm and their density on the target amounts to 10¹⁰ cm⁻². The effect is observed with sufficiently short laser pulses. In particular, either a 350 ps or a 90 ps Nd:YAG lasers are used in their fundamental harmonics. The nanospikes are characterized by UV-Visible reflection spectrometry and atomic force microscopy. The oscillations of electrons within nanospikes result in a permanent coloration of the surface and a modification of the optical reflection spectra of the metal. Scanning the laser beam along the metal surface allows its nanostructuring over extended areas (∼1 cm²). The nanostructured Ag surface shows enhanced Raman scattering of acridine molecules at a concentration of 10⁻⁵ M/l, whereas the initial Ag targets do not show any signal within the accuracy of measurements.     

Optical absorption in early stage low temperature laser produced plasma

We describe a new technique to measure the UV/visible absorption spectrum of the ablated material during the laser pulse. The technique utilizes the continuum emission from one laser produced plasma as a light source to measure the absorption properties of a second laser produced plasma which is formed on a semi-transparent target with an array of 40 μm holes. A 6 ns, 1064 nm laser was used to ablate a Ag target and the plasma absorption was measured in the range 450–625 nm for a laser fluence of 1 J cm⁻². The total absorption cross-section is (0.5–1.5)×10⁻¹⁷ cm² in the range 450–540 nm. By comparing the measured absorption with a calculation using the plasma spectroscopy code FLYCHK it can be concluded that, in the wavelength region examined here, the absorption is mainly due to bound-bound transitions.     

Near IR laser light visualizators using nonlinear GaSe and other layered crystallites

Two methods of preparation of the devices for visualization of pulsed and continuous near-IR (near infrared) are described and the results of conversion of pulsed and continuous IR (800–1360 nm) laser radiation into the visible range of spectra (400–680 nm) by using a transparent substrate covered with the particles (including nanoparticles) of effective nonlinear materials of GaSe _x S_{1 − x} (0.2 ≤ x ≤ 0.8) are presented. Converted light can be detected in transmission or reflection geometry as a visible spot corresponding to the real size of the incident laser beam. Developed device structures can be used for checking if the laser is working or not, for optical adjustment, for visualization of distribution of laser radiation over the cross of the beam and for investigation of the content of the laser radiation. Low energy (power density) limit for visualization of the IR laser pulses with 2–3 ps duration for these device structures are: between 4.6–2.1 μJ (3 × 10⁻⁴−1 × 10⁻⁴ W/cm²) at 1200 nm; between 8.4–2.6 μJ (4.7 × 10⁻⁴−1.5 × 10⁻⁴ W/cm²) at 1300 nm; between 14.4–8.1 μJ (8.2 × 10⁻⁴–4.6 × 10⁻⁴ W/cm²) at 1360 nm. Threshold damage density is more than 10 MW/cm² at λ = 1060 nm, pulse duration τ = 35 ps. The results are compared with commercially existing laser light visualizators.     

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.     

Theoretical study of Ni-like Ag 13.9nm TCE x-ray laser driven by two picosecond pulses

The Ni-like Ag 13.9nm x-ray laser has been previously demonstrated that the higher gain near critical surface contributes little to the amplification of the x-ray laser because of severe refraction. In this paper, the transient collision excitation (TCE) Ni-like Ag 13.9nm x-ray laser is simulated, driven by two 3ps short pulse preceded by a 330ps long prepulse, optimization of the peak to peak delay time of the two short pulses is made to get the best results. Simulation indicates that by producing lowly ionized preplasma with smoothly varying electron density, it is possible to decrease electron density gradient in higher density region, and thus higher gains near this region could be utilized, and if the main short pulse is delayed by 900ps, local gains where electron density larger than ～ 4×10²⁰cm^-3 could be utilized.     

Influence of laser pulse width on absolute EUV-yield from Xe-clusters

Using 50 fs ( ∼ 2×10¹⁸ W/cm²) and 2 ps ( ∼ 5×10¹⁶ W/cm²) pulses from a Ti:Sa multi-TW laser at 800 nm wavelength large Xe-clusters ( 10⁵...10⁶ atoms per cluster) have been excited. Absolute yield measurements of EUV-emission in a wavelength range between 10 nm and 15 nm in combination with cluster target variation were carried out. The ps-laser pulse has resulted in about 30% enhanced and spatially more uniform EUV-emission compared to fs-laser excitation. Circularly polarized laser light instead of linear polarization results in enhanced emission which is probably caused by electrons gaining higher energies by the polarization dependent optical field ionization process. An absolute emission efficiency at 13.4 nm of up to 0.8% in 2π sr and 2.2% bandwidth has been obtained. Received 11 January 2001 and Received in final form 27 March 2001     

Photodesorption from ultra-thin metal films – a comparison of SO<Subscript>2</Subscript> and NO<Subscript>2</Subscript> on Ag/Si(100)

The photochemistry of SO₂ on thin epitaxial Ag films (5–60 nm) deposited on Si(100) has been studied using laser light with the wavelengths of 266, 355, and 532 nm. SO₂ desorbs with cross sections of 1.7×10^-19,1.7×10^-20 and 2.9×10^-21 cm², respectively. The average translation energy, 〈E_trans/2k〉, is 440 K for 266 and 355 nm light, and 270 K for 532 nm light. Cross sections for a 60 nm thick Ag film are practically identical to the ones for Ag(111) as the substrate. An increase by a factor of ∼3.5 is observed when the film thickness is reduced to 5 nm for 266 and 355 nm light. No significant change is observed for 532 nm excitation. The film thickness has no significant influence on the translational energy of the photodesorbed molecules. The data are discussed in connection with the change of absorptivity of the metal film–semiconductor system. A model is put forward which takes into account the light absorption in the Si substrate and the reduced relaxation of excited electrons in Si. Modelling indicates that electrons excited in the Si substrate with energies and parallel momenta not allowed in Ag contribute to the surface chemistry after crossing the gap in the projected band structure of Ag(111). PACS 82.45.MP; 73.63.-b; 82.50.Bc     

Synthesis of ZnO thin films by 40 ps @ 532 nm laser pulses

The synthesis by pulsed laser deposition of ZnO thin films with a Nd:YAG laser system delivering pulses of 40 ps @ 532 nm is reported. The laser beam irradiated the target placed inside a vacuum chamber evacuated down to 1.33×10⁻¹ Pa. The incident laser fluence was of 28 J/cm² in a spot of 0.1 mm². The ablated material was collected onto double face polished (111) Si or quartz wafers placed parallel at a separation distance of 7 mm. The AFM, SEM, UV-Vis, FT-IR and absorption ellipsometry results indicated that we obtained pure ZnO films with a rather uniform surface, having an average roughness of 37 nm. We observed by SEM that particulates are present on ZnO film surface or embedded into bulk. Their density and dimension were intermediary between particulates observed on similar structures deposited with fs or ns laser pulses. We noticed that the density of the particulates is increasing while their average size is decreasing when passing from ns to ps and fs laser pulses. The average transmission in the UV-Vis spectral region was found to be higher than 85%.     

激光等离子体自发电流

本文研究了脉宽为200ps(FWHM),输出能量为0.1～4J,波长为1.06μm的激光束辐照Rh,Ag和Cu靶激光等离子体发射的自发电流.实验结果发现,激光辐照的焦斑中心位置,峰值电流密度高达10⁷A/cm²。 关键词：     

The effect of screening in an erosion flare on the recoil momentum and on the measurement of the reflection coefficient

Experimental investigations have been carried out to measure the transmission coefficient of laser light through an erosion flare, the coefficient of reflection from the irradiated solid surface, and the recoil momentum of insulating and metal targets in the range of pulsed laser intensities from 10⁶ to 10⁷ W/cm² with variation in the pressure of the surrounding medium from 10⁻² to 10⁵ Pa. An analysis is made of how the screening properties of the erosion flare affect the recoil momentum, and it is found necessary to take into account absorption of the radiation in the flare in determining the coefficient of reflection of the radiation from the surface. Zh. Tekh. Fiz. 67, 58–62 (March 1997)     

Nonthermal desorption of molecular ions of polyatomic molecules induced by uv laser radiation

The paper presents the results of studies into ion desorption from the surface of adenine and anthracene molecular crystals and anthracene molecules adsorbed on a metal as the surface is irradiated by an uv laser at λ=249, 308, and 337 nm. A sharp increase in molecular ion yield has been revealed with a decrease in radiation wavelength down to 249 nm. At this wavelength the effect of molecular ion desorption is observed at the radiation intensity of 20∶50 kW/cm² and pulse duration of 20 ns, it cannot be explained by thermal mechanisms. The initial velocity distribution of photoions is nonthermal by character, with maximum velocity of 2·10⁵ cm/s in case of adenine. The mechanisms responsible for the effect observed are discussed.     

Structural transitions in silicon induced by a femtosecond laser pulse: The role of an electron-hole plasma and phonon-phonon anharmonicity

It is shown by the methods of time-resolved self-reflection and linear reflection that irradiation of a silicon target by a 100-fs laser pulse induces successive structural transitions of the target material to new crystal and liquid metal phases, which can occur during the laser pulse or 0.1–10³ ps after the pulse termination, depending on the excitation conditions. The thresholds of these structural transitions are determined, and “’soft” phonon modes involved in them are identified, which represent “hot” short-wavelength LA modes. The dynamics of the structural transitions in silicon in the time interval from 0.1 to 10³ ps is described using the model of instability of phonon modes caused by an electron-hole plasma and intra-and intermode phonon-phonon anharmonic interactions     

Engineering of hydrophilic and plasmonic properties of Ag thin film by atom beam irradiation

Hydrophilic Ag nanostructures were synthesized by physical vapour deposition of 5 nm Ag thin films followed by irradiation with 1.5 keV Ar atoms. Optical absorbance measurements show a characteristic surface plasmon resonance absorption band in visible region. A blue-shift in absorbance from 532 to 450 nm is observed with increasing fluence from 1 × 10¹⁶ to 3 × 10¹⁶ atoms/cm². Atomic force microscopy was performed for the pristine and irradiated samples to study the surface morphology. The atom beam irradiation induced sputtering and surface diffusion lead to the formation of plasmonic surface. Rutherford backscattering spectroscopy of the pristine and irradiated film indicates that metal content in the film decreases with ion fluence, which is attributed to the sputtering of Ag by Ar atoms. The contact angle measurement demonstrates the possibility of engineering the hydrophilicity by atom beam irradiation.     

Parametric generation of shortened,narrow-band picosecond pulses using a Yag-pump laser

Using a single path parametric system pumped by a YAG laser, shortened pulses are produced at various frequencies. Starting with a duration of the pump pulse of 21 ps at 9400 cm^?1 we achieve a duration of 4 ps between 2700 cm^?1 and 6700 cm^?1, of 8 ps between 13 500 cm^?1 and 16 100 cm^?1, and of 8 ps between 27 000 cm^?1 and 32 000 cm^?1. Typical bandwidths are 10 cm^?1 in the infrared, 4 cm^?1 in the visible, and 5 cm^?1 in the ultraviolet.     

Optimization of nickel-like collisional soft-X-ray lasers at low pump power

We report on the experimental demonstration of saturated X-ray laser output from collisionally pumped Ni-like Pd, Ag, and Sn at wavelengths of 14.7, 14.0, and 12.0 nm, respectively. Using a 100 ps drive pulse irradiation and a `twin-0.25%' prepulse configuration on flat slab targets, gain-length products >16 were obtained for the three elements. The drive power required for saturation was only 250 GW in a 100 ps pulse (25 J), corresponding to an irradiance of 10 TW/cm².     

Selective ablation of thin SiO<Subscript>2</Subscript> layers on silicon substrates by femto- and picosecond laser pulses

The selective ablation of thin (∼100 nm) SiO₂ layers from silicon wafers has been investigated by applying ultra-short laser pulses at a wavelength of 800 nm with pulse durations in the range from 50 to 2000 fs. We found a strong, monotonic decrease of the laser fluence needed for complete ablation of the dielectric layer with decreasing pulse duration. The threshold fluence for 100% ablation probability decreased from 750 mJ/cm² at 2 ps to 480 mJ/cm² at 50 fs. Significant corruption of the opened Si surface has been observed above ∼1200 mJ/cm², independent of pulse duration. By a detailed analysis of the experimental series the values for melting and breaking thresholds are obtained; the physical mechanisms responsible for the significant dependence on the laser pulse duration are discussed.     

Silver nanoparticles produced by PLD in vacuum: role of the laser wavelength used

In this work we report the results of investigation of silver (Ag) nanoparticles prepared on a silica substrate by laser ablation. Our attention was focused on the mean diameter, size distribution and optical absorption properties of nanoparticles prepared in vacuum by using different laser wavelengths. The fundamental wavelength and the second, third, and fourth harmonics of a nanosecond Nd:YAG laser were used for nanoparticles fabrication. The corresponding values of the laser fluence for each wavelength were: 0.6 J/cm² at 266 nm, 0.8 J/cm² at 355 nm, 2.8 J/cm² at 532 nm, and 2 J/cm² at 1064 nm. The Ag nanoparticles produced have mean diameters in the range from 2 nm to 12 nm as the nanoparticles’ size decreases with the decrease of the wavelength used. The presence of the Ag nanoparticles was also evidenced by the appearance of a strong optical absorption band in the measured UV-VIS spectra associated with surface plasmon resonance (SPR). A redshift and widening of the absorption peak were observed as the laser wavelength was increased. Some additional investigations were performed in order to clarify the structure of the Ag nanoparticles.     

Experimental investigation into polycrystalline and single-crystal diamonds under negative pressures formed by picosecond laser pulses

Results of the experimental investigation of the spallation phenomenon in polycrystalline and single-crystal synthetic diamond are presented. The shock-wave action on the target was formed by a laser pulse with a duration of 70 ps using a Kamerton-T installation. To attain the ablation pressure of 0.66 TPa on the face surface of the target, the laser radiation of the Nd:glass laser (second harmonics λ = 527 nm, the pulse energy is 2.5 J) was used at intensity up to 2 × 10¹³ W/cm². The attained maximal spall strength of diamond σ* ～ 16.5 GPa is 24% of the theoretical ultimate strength. The Raman scattering indicates that a small amount of crystalline diamond is graphitized in the spall region on the back target side.     

Laser-assisted generation of self-assembled microstructures on stainless steel

Utilising a Nd:YVO₄ laser (wavelength of 532 nm, pulse duration of 8 ns, repetition rate of 30 kHz) and a Nd:YAG laser (wavelength of 1064 nm, pulse duration of 7 ns, repetition rate of 25 kHz), it was found that during the pulsed laser ablation of metal targets, such as stainless steel, periodic nodular microstructures (microcones) with average periods ranging from ∼30 to ∼50 μm were formed. This period depends on the number of accumulated laser pulses and is independent of the laser wavelength. It was found that the formation of microcones could occur after as little as 1500 pulses/spot (a lower number than previously reported) are fired onto a target surface location at laser fluence of ∼12 J/cm², intensity of ∼1.5 GW/cm². The initial feedback mechanism required for the formation of structures is attributed to the hydrodynamic instabilities of the melt. In addition to this, it has been shown that the structures grow along the optical axis of the incoming laser radiation. We demonstrate that highly regular structures can be produced at various angles, something not satisfactorily presented on metallic surfaces previously. The affecting factors such as incident angle of the laser beam and the structures that can be formed when varying the manner in which the laser beam is scanned over the target surface have also been investigated.     

Femtosecond Fourier interferometry of a nonideal plasma

Experimental diagnostic methods based on the measurement of the reflectance of a plasma are considered. The application of Fourier interferometry for measuring the dynamics of variation of the amplitude and phase of the complex reflectance of the Au plasma for various delay times in intervals shorter than 1 ps relative to the pumping laser pulse with a femtosecond time resolution is described in detail in the intensity range ∼10¹³–10¹⁴ W/cm². The variation of the complex refractive index of the heated Au target for a pump pulse intensity of ∼10¹²–10¹³ W/cm² is analyzed on the basis of experimental data using the Fresnel formulas.