Study on nonlinear optical absorption properties of [(CH3)4N]2[Cu(dmit)2] by Z-scan technique

The third-order optical nonlinearities of an organo-metallic compound, [(CH₃)₄N]₂[Cu(dmit)₂] (dmit²⁻=4,5-dithiolate-1,3-dithiole-2-thione), abbreviated as MeCu, dissolved in acetone are characterized by Z-scan technique with picosecond and nanosecond laser pulses in the near-infrared region. Two-photon absorption has been found when the sample solution is irradiated by 40 ps pulse width at 1064 nm and the two-photon absorption (TPA) coefficient β_TPA is 4×10⁻¹³ m/W. While excited by 15 ns laser pulses at 1053 nm, the Z-scan spectra reveal strong reverse saturable absorption (RSA) and the nonlinear absorption coefficient β_RSA is estimated to be as high as 7.07×10⁻¹¹ m/W which is much larger than β_TPA. An explanation for this enhancement is given. All the results suggest that MeCu may be a promising candidate for the application to optical limiting in the near-infrared region.     

A comparative study of the ionic keV X-ray line emission from plasma produced by the femtosecond,picosecond and nanosecond duration laser pulses

We report here an experimental study of the ionic keV X-ray line emission from magnesium plasma produced by laser pulses of three widely different pulse durations (FWHM) of 45 fs, 25 ps and 3 ns, at a constant laser fluence of ∼1.5 × 10⁴ J cm^− 2. It is observed that the X-ray yield of the resonance lines from the higher ionization states such as H- and He-like ions decreases on decreasing the laser pulse duration, even though the peak laser intensities of 3.5 × 10¹⁷ W cm^− 2 for the 45 fs pulses and 6.2 × 10¹⁴ W cm^− 2 for the 25 ps pulses are much higher than 5 × 10¹² W cm^− 2 for the 3 ns laser pulse. The results were explained in terms of the ionization equilibrium time for different ionization states in the heated plasma. The study can be useful to make optimum choice of the laser pulse duration to produce short pulse intense X-ray line emission from the plasma and to get the knowledge of the degree of ionization in the plasma.     

Stacking chirped pulse optical parametric amplification

Stacking chirped pulse optical parametric amplification based on a home-built Yb³⁺-doped mode-locked fiber laser and an all-fiber pulse stacker has been demonstrated. Energic 11 mJ shaped pulses with pulse duration of 2.3 ns and a net total gain of higher than 1.1 × 10⁷ at fluctuation less than 2% rms are achieved by optical parametric amplification pumped by a Q-switched Nd:YAG frequency-doubled laser, which provides a simple and efficient amplification scheme for temporally shaped pulses by stacking chirped pulse.     

Generation of synchronized signal and pump pulses for an optical parametric chirped pulse amplification based multi-terawatt Nd:glass laser system

Synchronized signal (650 ps) and pump (1.3 ns) pulses were generated using 4-pass geometry in a grating pair based pulse stretcher unit. The pump pulse has been further amplified in a high gain regenerative amplifier. This amplified pulse was used as the pump in an optical parametric chirped pulse amplification based Nd:glass laser system. As the chirped signal pulse and the pump pulse originated from the same oscillator, the time jitter between the pump pulse and the signal pulse can be <50 ps.     

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.     

Characterization of excimer laser ablation generated pepsin particles using multi-wavelength photoacoustic instrument

Preparation of organic thin layers on various special substrates using the pulsed laser deposition (PLD) technique is an important task from the point of view of bioengineering and biosensor technologies. Earlier studies demonstrated that particle ejection starts during the ablating laser pulse resulting in significant shielding effects which can influence the real fluence on the target surface and consequently the efficiency of layer preparation. In this study, we introduce a photoacoustic absorption measurement technique for in-situ characterization of ablated particles during PLD experiments. A KrF excimer laser beam (λ=248 nm, FWHM=18 ns) was focused onto pepsin targets in a PLD chamber; the applied laser fluences were 440 and 660 mJ/cm². We determined the wavelength dependence of optical absorption and mass specific absorption coefficient of laser ablation generated pepsin aerosols in the UV–VIS–NIR range. On the basis of our measurements, we calculated the absorbance at the ablating laser wavelength, too. We demonstrated that when the laser ablation generated pepsin aerosols spread through the whole PLD chamber the effect of absorptivity is negligible for the subsequent pulses. However, the interaction of the laser pulse and the just formed particle cloud generated by the same pulse is more significant.     

Nanosecond and femtosecond ablation of La0.6Ca0.4CoO3: a comparison between plume dynamics and composition of the films

Thin films of La_0.6Ca_0.4CoO₃ were grown by pulsed laser ablation with nanosecond and femtosecond pulses. The films deposited with femtosecond pulses (248 nm, 500 fs pulse duration) exhibit a higher surface roughness and deficiency in the cobalt content compared to the films deposited with nanosecond pulses (248 nm, 20 ns pulse duration). The origin of these pronounced differences between the films grown by ns and fs ablation has been studied in detail by time-resolved optical emission spectroscopy and imaging. The plumes generated by nanosecond and femtosecond ablation were analyzed in vacuum and in a background pressure of 60 Pa of oxygen. The ns-induced plume in vacuum exhibits a spherical shape, while for femtosecond ablation the plume is more elongated along the expansion direction, but with similar velocities for ns and fs laser ablation. In the case of ablation in the background gas similar velocities of the plume species are observed for fs and ns laser ablation. The different film compositions are therefore not related to different kinetic energies and different distributions of various species in the plasma plume which has been identified as the origin of the deficiency of species for other materials.     

Ablation and analysis of small cell populations and single cells by consecutive laser pulses

Laser ablation of single cells through a sharpened optical fiber is used for the detection of metabolites by laser ablation electrospray ionization (LAESI) mass spectrometry (MS). Ablation of the same Allium cepa epidermal cell by consecutive pulses indicates the rupture of the cell wall by the second shot. Intracellular sucrose heterogeneity is detected by subsequent laser pulses pointing to rupturing the vacuolar membrane by the third exposure. Ion production by bursts of laser pulses shows that the drying of ruptured A. cepa cells occurs in ∼50 s at low pulse rates (10 pulses/s bursts) and significantly faster at high pulse rates (100 pulses/s bursts). These results point to the competing role of cytoplasm ejection and evaporative drying in diminishing the LAESI-MS signal in ∼50 s or 100 laser pulses, whichever occurs first.     

Co:LaMgAl11O19 saturable absorber Q-switch for a 1.319 μm Nd:YAG laser

Passively Q-switched output of a flashlamp-pumped 1.319 μm Nd:YAG laser is realized by using Co²⁺:LaMgAl₁₁O₁₉ (Co:LMA) as saturable absorber. When initial transmission of the saturable absorber T₀ is 78%, a Q-switched output pulse with pulse width (FWHM) 44.8 ns and pulse energy 17.4 mJ is obtained, corresponding to 19.3% of the free-running energy under the equal pumping energy of 45.4 J. The experimental results show that the higher T₀ will result in a lower pumping threshold of the laser, but lower T₀ can make the laser generate pulses with higher single-pulse energy, narrower pulse width, and accordingly higher peak power.     

Structure and optical properties of carbon films obtained by multipulse pulsed laser deposition

We have obtained carbon thin films on silicon and glass substrates with multipulse pulsed laser irradiation of graphite under vacuum (p ≈ 2.6 Pa) using a high-frequency series of nanosecond laser pulses (τ = 85 ns, λ = 1060 nm) with pulse repetition frequency f ≈ 10–20 kHz and laser power density q ≈ 15–40 MW/cm². We established the optimal laser power density and laser pulse repetition frequency for obtaining amorphous nanostructured diamond-like films.     

Nonlinear optical absorption studies of an organo-metallic complex by Z-scan technique

An organo-metallic complex, [(CH₃)₄N][Ni(dmit)₂] (dmit²⁻ = (1,3-dithiole-2-thione-4,5-dithiolate), abbreviated as MeNi, is synthesized. The nonlinear optical absorption properties of MeNi dissolved in acetone have been studied using the open-aperture Z-scan technique with 40 ps pulse width at 1064 nm and 1 ns, 15 ns pulse width at 1053 nm, respectively. Strong saturable absorption has been found when the sample solution is irradiated by 40 ps and 1 ns laser pulses. While irradiated with 15 ns laser pulse, a stronger reverse saturable absorption has been found. The nonlinear optical absorption coefficients are −1.03 × 10⁻¹¹ m/W, −1.85 × 10⁻¹¹ m/W and 3.84 × 10⁻¹⁰ m/W, respectively. The mechanism responsible for the difference between the results is analyzed. All the results suggest that this material may be a promising candidate for the application to laser pulse compression in the near-infrared waveband.     

Superradiative rare gas halide lasers excited by electric discharge

Nd_xLa_1−xP₅O₁₄ (0.25≦x≦1) single crystals, placed within a confocal optical resonator, were pumped with ruby laser fundamental and second-harmonic nanosecond pulses. In both cases laser oscillations at 1.05 μm exceeding in duration many times the pumping pulse were obtained.     

Tunable,sub-nanosecond KrF-Raman laser in the ultraviolet

A 0.5 cm^–1 bandwidth injection-locked KrF laser pumps a rare-gas Brillouin cell to produce a reflected pulse with a leading edge risetime of 1 ns, tunable from 248.1 to 248.7 nm. Consistent with Lamb theory of laser amplifiers, subsequent excimer amplification of this pulse produces an intense 500 ps spike on the pulse leading edge. Stimulated Raman scattering then separates the spike from the parent pulse, yielding a tunable short pulse at the first Stokes (S ₁) wavelength. Varying the Raman cell length results in a variable Raman threshold and an adjustable short pulse duration: 250 ps pulses at energies of 3–4 mJ at 268 nm with a 50 cm methane cell and 350 ps, 5 mJ pulses from a 100 cm cell are measured with a streak camera. First pass Raman conversion of the spike toS ₁ followed by second pass backward Raman amplification, where the parent 248 nm pulse serves as the pump beam for the reflectedS ₁ pulse, yields simultaneousS ₁ pulses of 20–25 mJ in the 800 ps range andS ₂ pulses of 550 ps at 5–6 mJ near 290 nm. This laser will avoid collision effects during laser excitation and enable quantitative, single pulse imaging of OH radicals in turbulent combustion because of its high pulse energy.     

Generation of long bursts of high-repetition-rate arbitrarily shaped optical pulses using time lens

A technique for the generation of long ultrahigh-speed bursts of optical pulses with arbitrary shapes is proposed. A laser pulse is temporally chirped by a time lens and then passes through a filter with a reconfigurable periodic spectral response, which produces time-delayed replicas of the chirped pulse and recombines them. As a result of the temporal interference between the replicas, the chirped pulse is broken up into short pulses with the shape determined by the chosen filter response. It is demonstrated that the filter acts on a long chirped optical pulse as a temporal modulator with a periodic modulation function. The modulation frequency and bandwidth of the modulator can be much higher than for commercially available high-frequency modulators. The additional advantage of this modulator is the arbitrary shape of the modulation function. A 2.4 ns burst of nearly flat-top pulses with a repetition rate of about 400 GHz is obtained in numerical simulations. In addition, the technique proposed can act as a pulse repetition rate multiplier and a pulse compressor. A repetition rate of 1.589 THz and an individual pulse width of 212 fs are achieved in simulations for a 9.7 ns sinusoidally phase modulated pulse burst.     

High-energy long-pulse Nd:YAG picosecond laser

A long train of actively mode-locked pulses is obtained from a negative feedback controlled Nd:YAG laser. The 70s pulse train contains up to 0.1 J energy and the duration of the picosecond pulses is 120 ps. The laser is operated at a repetition rate of 20 Hz. ActiveQ-control of the cavity generates a short pulse train of duration 50 to 70 ns. An excellent peak-to-background intensity ratio of the correlation function for the picosecond pulses in the train of 5×10³ is reported.     

Non-linear optical properties of (Pb<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Sr<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>)TiO<Subscript>3</Subscript> thin films

Thin films of (Pb_1−x Sr _x )TiO₃, x=0,0.5,1.0 have been prepared on glass substrates by the chemical-solution method using the spin-coating technique. The optical nonlinearity in the visible spectral region is investigated using short (5 ns) laser pulses at the off-resonant wavelength of 532 nm employing the open aperture z-scan technique. It is found that the third order nonlinear absorption is dependent on the lead content of the films, with the compositions x=0, 0.5 exhibiting large values (β∼10⁻⁷ m/W), thereby suggesting the possible use of these materials as optical limiters. No optical nonlinearity is observed for the composition with x=1.0.     

Picosecond laser ablation of thin copper films

The ablation process of thin copper films on fused silica by picosecond laser pulses is investigated. The ablation area is characterized using optical and scanning electron microscopy. The single-shot ablation threshold fluence for 40 ps laser pulses at 1053 nm has been determinated toF _thres = 172 mJ/cm². The ablation rate per pulse is measured as a function of intensity in the range of 5 × 10⁹ to 2 × 10¹¹ W/cm² and changes from 80 to 250 nm with increasing intensity. The experimental ablation rate per pulse is compared to heat-flow calculations based on the two-temperature model for ultrafast laser heating. Possible applications of picosecond laser radiation for microstructuring of different materials are discussed.     

High efficiency KTiOAsO4 optical parametric oscillator within a diode-side-pumped two-rod Nd:YAG laser

A high efficiency KTiOAsO₄(KTA) intracavity optical parametric oscillator (IOPO) is demonstrated within a diode-side-pumped acousto-optically (AO) Q-switched two-rod Nd:YAG laser. With a 25-mm-long X-cut KTA crystal, efficient parametric conversions to signal (1.54 μm) and idler (3.47 μm) waves are realized. The highest output power of 15.8 W including 12.7 W signal and 3.1 W idler power is obtained at a repetition rate of 7.5 kHz and a pump power of 208 W, corresponding to an optical-to-optical conversion efficiency of up to 7.6%. The signal pulse duration is 32 ns with a peak power of 53 kW. At a repetition rate of 12.5 kHz and the pump power of 208 W, the highest idler power of 3.4 W is obtained with a peak power of 14 kW and a pulse duration of 19 ns. And the beam quality factors (M ²) of the signal and idler waves are determined to be around 2 and 20, respectively.     

Table-top kHz hard X-ray source with ultrashort pulse duration for time-resolved X-ray diffraction

The interaction of ultrashort laser pulses with solid state targets is studied concerning the production of short X-ray pulses with photon energies up to about 10 keV. The influence of various parameters such as pulse energy, repetition rate of the laser system, focusing conditions, the application of prepulses, and the chirp of the laser pulses on the efficiency of this highly nonlinear process is examined. In order to increase the X-ray flux, the laser pulse energy is increased by a 2nd multipass amplifier from 750 μJ to 5 mJ. By applying up to 4 mJ of the pulse energy a X-ray flux of 4×10¹⁰ Fe K _α photons/s or 2.75×10¹⁰ Cu K _α photons/s are generated. The energy conversion efficiency is therefore calculated to η _Fe≈1.4×10⁻⁵ and η _Cu≈1.0×10⁻⁵. The X-ray source size is determined to 15×25 μm². By focusing the produced X-rays using a toroidally bent crystal a quasi-monochromatic X-ray point source with a diameter of 56 μm×70μm is produced containing ≈10⁴ Fe K _α1 photons/s which permits the investigation of lattice dynamics on a picosecond or even sub-picosecond time scale. The lattice movement of a GaAs(111) crystal is shown as a typical application.     

Short-pulse UV laser ablation of solid and liquid metals: indium

2 to 2.5 mJ/cm² when a 0.5 ps pulse is used instead of a 15 ns laser pulse. Measurements on liquid indium show a different behavior. With 15 ns laser pulses the threshold fluence is lowered by a factor of ∼3 from 100 mJ/cm² for solid indium to 30 mJ/cm² for liquid indium. In contrast, measurements with 0.5 ps laser pulses do not show any change in the ablation threshold and are independent of the phase of the metal at 2.5 mJ/cm². This behavior could be explained by thermal diffusion and heat conduction during the laser pulse and demonstrates in an independent way the energy lost into the material when long laser pulses are applied. Time-of-flight measurements to investigate the underlying ablation mechanism show thermal behavior of the ablated indium atoms for both ps and ns ablation and can be fitted to Maxwell-Boltzmann distributions. Received: 2 December 1996/Accepted: 11 December 1996