Surface modifications of crystalline silicon created by high intensity 1064 nm picosecond Nd:YAG laser pulses

A study of silicon modification induced by a high intensity picosecond Nd:YAG laser, emitting at 1064 nm, is presented. It is shown that laser intensities in the range of 5 × 10¹⁰-0.7 × 10¹² W cm⁻² drastically modified the silicon surface. The main modifications and effects can be considered as the appearance of a crater, hydrodynamic/deposition features, plasma, etc. The highest intensity of ∼0.7 × 10¹² W cm⁻² leads to the burning through a 500 μm thick sample. At these intensities, the surface morphology exhibits the transpiring of the explosive boiling/phase explosion (EB) in the interaction area. The picosecond Nd:YAG laser-silicon interaction was typically accompanied by massive ejection of target material in the surrounding environment. The threshold for the explosive boiling/phase explosion (TEB) was estimated to be in the interval 1.0 × 10¹⁰ W cm⁻² < TEB ≤ 3.8 × 10¹⁰ W cm⁻².     

High contrast optical switching in vanadium dioxide thin films

Thermochromic vanadium dioxide thin films prepared by radio-frequency sputtering exhibit controllable transmittance at 1550 nm with a dynamic range exceeding 10³. Efficient optical control with a laser beam at 532 nm is demonstrated with intensities as low as 3 W/cm². Optical switch-on times as short as 100 μs are reported.     

The nonlinear refraction and nonlinear absorption in 4-(4,6-diaminopyrimidin-2-ylthio) substituted double-decker Lu(III) phthalocyanine

A 4-(4,6-diaminopyrimidin-2-ylthio) substituted double-decker Lu(III) phthalocyanines (4) have been prepared and characterized by elemental analysis, IR, UV-vis and ¹H NMR spectroscopies. The nonlinear refractive index, nonlinear absorption and the optical limiting (OL) performance of the compound 4 in a 0.5 mm spectroscopic cell in DMF solution were investigated by using 4 ns pulse laser at 532 nm. Z-scan experiments have been conducted between 0.24 and 2.39 GW/cm² peak intensities for 10 Hz repetition rate and also between 2.39 and 23.89 GW/cm² peak intensities for 1 Hz repetition rate. The thermal effect contributes to the nonlinear response of the material higher than 0.72 GW/cm² peak intensity at 10 Hz. We measured the effective nonlinear refractive index of the material as 1.2×10⁻¹¹ esu at 3.5×10⁻⁴ M concentration with the peak intensity less than 0.72 GW/cm² and we found that nonlinear absorption was very small. On the other hand, when concentration is increased to 2.4×10⁻³ M material's nonlinear absorption becomes dominant mechanism for the nonlinear response and the compound 4 indicates OL behavior at 2.4×10⁻³ M concentration.     

Effects of electron relaxation on multiple harmonic generation from metal surfaces with femtosecond laser pulses

Calculations are presented for the first four (odd and even) harmonics of an 800 nm laser from a gold surface, with pulse widths ranging from 100 down to 14 fs. For peak laser intensities above 1 GW/cm² the harmonics are enhanced because of a partial depletion of the initial electron states. At 10¹¹ W/cm² of peak laser intensity the calculated conversion efficiency for 2nd-harmonic generation is 3 × 10⁻⁹, while for the 5th-harmonic it is 10⁻¹⁰. The generated harmonic pulses are broadened and delayed relative to the laser pulse because of the finite relaxation times of the excited electronic states. The finite electron relaxation times cause also the broadening of the autocorrelations of the laser pulses obtained from surface harmonic generation by two time-delayed identical pulses. Comparison with recent experimental results shows that the response time of an autocorrelator using nonlinear optical processes in a gold surface is shorter than the electron relaxation times. This seems to indicate that for laser pulses shorter than ∼30 fs, the fast nonresonant channel for multiphoton excitation via continuum-continuum transitions in metals becomes important as the resonant channel becomes slow (relative to the laser pulse) and less efficient.     

Resonantly enhanced three-photon excitation spectra of lithium

We present the first measurement on the resonantly enhanced three-photon excitation spectra of natural lithium using a Nd:YAG laser pumped dye laser in conjunction with a thermionic diode ion detector. Exploiting the linear and circular polarizations, the np ²P_3/2(8 ? n ? 11) and nf  ²F_7/2 (8 ? n ? 38) series have been observed via three-photon excitation from the ground state. The measured level energies reveal a dynamic shift from calculated values, which increases with an increase of the principal quantum number n. The ac stark shift and line broadening mechanisms are studied as a function of laser intensity. It is noted that the width increases and the line center shifts towards the higher energy side as the laser intensity is increased. The maximum observed shift for the 12f ²F_7/2 line is 0.33 cm⁻¹ corresponding to the laser intensity variation from 1.34 × 10¹² W/m² to 1.03 × 10¹³ W/m², whereas its width increases from 0.36 cm⁻¹ to 0.82 cm⁻¹.     

Pulsed Nd:YAP laser at 1432 nm pumped with high power laser diode

LD end pumped Nd:YAP laser operation in the eye safe spectrum region at 1432 nm is reported. With pump energy of 256 mJ, maximum linearly polarized output of 26 mJ is obtained. The optical-to-optical overall efficiency is around 10%, and the slope efficiency is around 18%. The laser beam operates with spiking mode with a total emission period of less than 300 µs at 10 Hz. The stimulated emission cross section is estimated at around 0.85 × 10^− 20 cm².     

Indium tin oxide sol-gel precursor conversion process using the third harmonics of Nd:YAG laser

We use the third harmonics of Nd:YAG laser (λ = 355 nm) for simultaneous precursor conversion and dopant activation on sol-gel ITO thin films at a laser fluence range of 700-1000 mJ/cm². A minimum resistivity of 5.37 × 10⁻² Ω-cm with a corresponding carrier concentration of 6 × 10¹⁹ cm⁻³ is achieved at laser irradiation fluence of 900 mJ/cm². X-ray photoelectron analysis reveals that extremely high tin concentration of 19.4 at.% and above is presented in the laser-cured ITO thin films compared with 8.7 at.% in the 500 °C thermally cured counterpart. These excess tin-ions form complex defects, which contribute no free carriers but act as scattering centers, causing inferior electrical properties of the laser-cured films in comparison with the thermally cured ones.     

Generation of tunable infrared radiation in rubidium titanyl phosphate crystal for the optical measurement of number density, absorption cross-section of methane gas

Tunable near-infrared radiation has been generated in a rubidium titany1 phosphate (RTP) crystal by employing non-collinear difference-frequency mixing (DFM) technique. The input radiation sources are Nd:YAG laser radiation and its second harmonic pumped dye laser radiation. For the generation of 2.0 radiation, the maximum value of the conversion efficiency (quantum) obtained in the process is 49% from the dye (0.6945 μm) to the infrared (2.0 μm) radiation in the 7.9-mm-long crystal. The generated tunable mid-infrared radiation has been used to measure the number density, absorption cross-section and minimum detectable concentration of methane gas in its 2ν₃ band in a multi-pass cell at 30.075 Torr pressure. The number density and column density of the methane molecules are found to be 1.068×10¹⁸ cm⁻³ and 3.02×10²¹ cm⁻², respectively, whereas the minimum still-detectable concentration at 1.658 μm wavelength is estimated to be 4.523×10¹⁷/cm³.     

Femtosecond pulsed laser deposition of diamond-like carbon films: The effect of double laser pulses

The bonding structure of carbon films prepared by pulsed laser deposition is determined by the plasma properties especially the change of the kinetic energy. Using double laser pulses the ablation process and the characteristics of the generated plasma can be controlled by the setting of the delay between the pulses. In our experiments, amorphous carbon films have been deposited in vacuum onto Si substrates by double pulses from a Ti:sapphire laser (180 fs, λ = 800 nm, at 1 kHz) and a KrF laser system (500 fs, λ = 248 nm, at 5 Hz). The intensities have been varied in the range of 3.4 × 10¹² to 2 × 10¹³ W/cm². The morphology and the main properties of the thin layers were investigated as a function of the time delay between the two ablating pulses (0-116.8 ps) and as a function of the irradiated area on the target surface. Atomic force microscopy, spectroscopic ellipsometry and Raman-spectroscopy were used to characterize the films. It was demonstrated that the change of the delay and the spot size results in the modification of the thickness distribution of the layers, and the carbon sp²/sp³ bonding ratio.     

The absorption spectrum of water between 13 540 and 14 070 cm: ICLAS detection of weak lines and a complete line list

The absorption spectrum of water vapor has been investigated by Intracavity Laser Absorption Spectroscopy (ICLAS) between 13 540 and 14 070 cm⁻¹. This spectrum is dominated by relatively strong transitions of the 4δ polyad of vibrational states. The achieved sensitivity - on the order of α_min ∼ 10⁻⁹ cm⁻¹ - has allowed one to newly measure 222 very weak transitions with intensities down to 5 × 10⁻²⁸ cm/molecule at 296 K. Fifty new or corrected H₂¹⁶O energy levels belonging to a total of 13 vibrational states could be determined from the rovibrational analysis based on variational calculations by Schwenke and Partridge. The previous investigations in the region by Fourier Transform Spectroscopy were critically evaluated and used to construct the best to date set of energy levels accessed by transitions in the considered region. All the rovibrational transitions reaching these upper energy levels and having intensities larger than 4.0 × 10⁻²⁸ cm/mol were calculated. In the resulting line list, the positions at the level of experimental accuracy were augmented with variational intensities leading to the most complete line list for water in normal isotopic abundance in the 13 500-14 100 cm⁻¹ region.     

Continuous-wave broadly tunable Cr:ZnSe laser pumped by a thulium fiber laser

We describe a compact, broadly tunable, continuous-wave (cw) Cr²⁺:ZnSe laser pumped by a thulium fiber laser at 1800 nm. In the experiments, a polycrystalline ZnSe sample with a chromium concentration of 9.5 × 10¹⁸ cm⁻³ was used. Free-running laser output was around 2500 nm. Output couplers with transmissions of 3%, 6%, and 15% were used to characterize the power performance of the laser. Best power performance was obtained with a 15% transmitting output coupler. In this case, as high as 640 mW of output power was obtained with 2.5 W of pump power at a wavelength of 2480 nm. The stimulated emission cross-section values determined from laser threshold data and emission measurements were in good agreement. Finally, broad, continuous tuning of the laser was demonstrated between 2240 and 2900 nm by using an intracavity Brewster cut MgF₂ prism and a single set of optics.     

Line intensity measurements in N2O and their treatment using the effective dipole moment approach.II. The 5400-11 000 cm region

The absorption spectrum of N₂O, at room temperature, was recorded in the 5400-11 000 cm^-1 region at resolutions ranging from 0.008 cm^-1 near 5400 to 0.023 cm^-1 near 11 000 cm^-1 using a Bruker IFS120HR Fourier transform spectrometer. Sample pressure/absorption path length products ranging from 200 to 4700 mbar×m were used. More than 6000 absolute line intensities have been measured in 64 different bands of ¹⁴N₂¹⁶O. Using wavefunctions previously determined from a global fit of an effective Hamiltonian to more than 18 000 line positions [Tashkun SA, Perevalov VI, and Teffo JL, to be published], the experimental intensities measured in this work and by Toth [J Mol Spectrosc 1999;197:158-87] were fit using 62 parameters of a corresponding effective dipole moment, with residuals very close to the experimental uncertainty.     

Investigation on upconversion photoluminescence of Bi3TiNbO9:Er:Yb thin films

Bi₃TiNbO₉:Er³⁺:Yb³⁺ (BTNEY) thin films were fabricated on fused silica by pulsed laser deposition. It was demonstrated that different laser fluence and substrate temperature during growth of BTNEY upconversion photoluminescence (UC-PL) samples control the film’s grain size and hence influences the UC-PL properties. The average grain size of BTNEY thin films deposited on fused silica substrates with laser fluence 4, 5, 6, and 7 J/cm² are 30.8, 35.9, 40.6, and 43.4 nm, respectively. The 525 nm emission intensities increase with the deposition laser fluence and the emission intensities of BTNEY thin film deposited under 700 and 600 °C are almost 24 and 4 times, respectively, as strong as those of samples under 500 °C. The grain size of BTNEY thin film increases with the increasing temperature. UC-PL of BTNEY films is enhanced by increasing grain size of the films.     

Empirical line parameters of methane from 1.1 to 2.1 μm

To provide line parameters for the near-infrared methane spectrum, 35,306 line positions and intensities at room temperature were retrieved between 6180 and 9200 cm⁻¹, along with 4936 lines between 4800 and 5500 cm⁻¹. For this, laboratory absorption spectra were recorded at 0.010-0.022 cm⁻¹ resolution using the McMath-Pierce Fourier Transform Spectrometer located on Kitt Peak in Arizona. Positions were calibrated using CO transitions at 2.3 and 1.6 μm and H₂O lines at 1.9 and 1.3 μm. The minimum line intensity included was 3.7×10⁻²⁶ cm⁻¹/(molecule cm⁻²), and the combined sum of the intensities in these two intervals was 7.085×10⁻²⁰ cm⁻¹/(molecule cm⁻²) at 296 (±4) K. Quantum assignments from the literature were matched for 1% of the features, and a new methane database was compiled for the near-infrared.     

Electro-optic Q-switched intracavity optical parametric oscillator at 1.53 μm based on KTiOAsO4

An eye-safe, high peak power optical parameter oscillator (OPO) intracavity pumped by electro-optic Q-switched Nd:YAG laser is presented. This OPO is based on a 20 mm length KTiOAsO₄ crystal with non-critical phase matching (θ = 90°, ?=0°) cut. An aperture ∅3 mm acted as limiting diaphragm to get good beam quality of pumping laser. The output energy of 25 mJ at the signal wavelength 1.53 μm was obtained with repetition rate of 1 Hz. The highest peak power intensity was up to 88 MW/cm² with pulse width of 4 ns. Without diaphragm, the maximum output energy of 90 mJ was achieved with area of light spot (∅6 mm) four times larger, but the peak power intensity was lower.     

Studies of craters’ dimension for long-pulse laser ablation of metal targets at various experimental conditions

Long pulse laser shots of the PALS iodine laser in Prague have been used to obtain metal target ablation at various experimental conditions. Attention is paid mainly to the dependencies of the crater diameter on the position of minimum laser-focus spot with regard to the target surface, by using different laser wavelengths and laser energies. Not only a single one, but two minima, independently of the wavelength, of the target irradiation angle and of the target material, were recorded. Significant asymmetries, ascribed to the non-linear effects of intense laser beam with pre-formed plasma, were found, too. Estimations of ejected mass per laser pulse are reported and used to calculate the efficiency of laser-driven loading. Results on metal target ablation and crater formation at high intensities (from 2 × 10¹³ to 3 × 10¹⁶ W/cm²) are presented and compared. Crater depth, crater diameter and etching yield are reported versus the laser energy, in order to evaluate the ablation threshold fluence.     

ICLAS of weak transitions of water between 11 300 and 12 850 cm: Comparison with FTS databases

Very weak water vapor absorption lines have been investigated by intracavity laser absorption spectroscopy (ICLAS) in the 11 335-11 947 and 12 336-12 843 cm⁻¹ spectral regions dominated by the ν₁ + 3ν₂ + ν₃ and ν₂ + 3ν₃ bands, respectively. A detectivity on the order of α_min ∼ 10⁻⁹ cm⁻¹ was achieved with an ICLAS spectrometer based on a Ti: Sapphire laser. It allowed detecting transitions with an intensity down to 5 × 10⁻²⁸ cm/molecule which is about 10 times lower than the weakest line intensities previously detected in the considered region. A line list corresponding to 1281 transitions with intensity lower than 5 × 10⁻²⁶ cm/molecule has been generated. A detailed comparison with the line lists provided by the HITRAN database and by recent investigations by Fourier transform spectroscopy associated with very long multi pass cell is presented. The rovibrational assignment performed on the basis of the ab initio calculations of Schwenke and Partridge, has allowed for determining 176 new energy levels belonging to a total of 16 vibrational states.     

Flexible gratings fabricated in polymeric plate using femtosecond laser irradiation

Flexible gratings embedded in poly-dimethlysiloxane (PDMS) were fabricated using femtosecond laser pulses. Photo-induced gratings in a flexible PDMS plate were directly written by a high-intensity femtosecond (130 fs) Ti: Sapphire laser (λ_p=800 nm). Refractive index modifications with 4 μm diameters were photo-induced after irradiation of the femtosecond pulses with peak intensities of more than 1×10¹¹ W/cm². The graded refractive index profile was fabricated to be symmetric around the center of the focal point. The diffraction efficiency of the grating samples is measured by an He-Ne laser. The maximum value of refractive index change (Δn) in the laser-modified regions was estimated to be approximately 3.17×10⁻³.     

Empirical low energy values for methane transitions in the 5852-6181 cm region by absorption spectroscopy at 81 K

The high resolution absorption spectrum of methane has been recorded at liquid nitrogen temperature by direct absorption spectroscopy between 1.62 and 1.71 μm (5852-6181 cm⁻¹) using a newly developed cryogenic cell and a series of distributed feedback (DFB) laser diodes. The minimum value of the measured line intensities is on the order of 3 × 10⁻²⁶ cm/molecule The investigated spectral range corresponds to the high energy part of the tetradecad dominated by the 2ν₃ band for which a theoretical treatment is not yet available. The positions and strengths at 81 K of 2187 transitions were obtained from the spectrum analysis. From the values of the line strength at liquid nitrogen and room temperatures, the low energy values of 845 transitions could be determined. The obtained results are discussed in relation with the previous work of Margolis and compared to the line list provided by the HITRAN database.     

Mid-infrared polarization spectroscopy of C2H2: Non-intrusive spatial-resolved measurements of polyatomic hydrocarbon molecules for combustion diagnostics

Polarization spectroscopy in the mid-infrared (IRPS) has been applied to the detection of acetylene molecules making use of the asymmetric C-H stretching vibration at around 3 μm. The infrared laser pulses were produced through difference frequency generation in a LiNbO₃ crystal pumped by a Nd:YAG and dye laser system. By directly probing the ro-vibrational transitions with IRPS, sensitive detection of molecules with otherwise inaccessible electronic states was realized with high temporal and spatial resolution by using a pulsed laser and a cross-beam geometry. Detection sensitivities of 2 × 10¹³ molecules/cm³ (10 ppm in 70 mbar gas mixture) of C₂H₂ were achieved using the P(1 1) line of the (0 1 0(1 1)⁰)-(0 0 0 0⁰ 0⁰) band. The dependence of the IRPS signal on the pump laser fluence, acetylene mole fraction, and buffer gas pressure of Ar, N₂, H₂, and CO₂ has been studied experimentally. The investigation demonstrates the quantitative nature of IRPS for sensitive detection of polyatomic IR active molecules. In order to fully demonstrate the technique for combustion applications, nascent acetylene molecules were measured in a low pressure methane/oxygen flame.