Circularly polarised attosecond pulses: generation and applications

ABSTRACT

Molecular high-order harmonic generation(MHOHG) is simulated for H⁺₂ in the nonlinear nonperturbative regime of laser-molecule interactions with ultrashort intense circularly polarised laser pulses. It is shown that combinations of co-rotating or counter-rotating pulses produce laser-induced Coriolis forces with electron-parent ion recollisions, thus enhancing circularly polarised MHOHG, the source of circularly polarised attosecond pulses. Such pulses can be used to induce electron attosecond currents for the generation of attosecond magnetic field pulses, new tools for molecular attomagnetism.     

Generation of lower and higher harmonics in different plasma media with small <Emphasis Type="Italic">Z</Emphasis>

The generation of lower (third) and higher harmonics of femtosecond laser radiation in plasmas produced by laser ablation of different targets with a small atomic number Z (B, Be, Li) has been investigated. The high (10⁻³) efficiency of third-harmonic generation was observed in plasma produced on the boron surface. Efficient third-harmonic generation was also observed in beryllium plasma using femtosecond pulses of Ti:sapphire laser radiation (λ = 790 nm) and its second harmonic (395 nm). We could tune the higher harmonics generation spectrum by tuning the crystal converter when using 395-nm radiation to be converted. It is shown that, in plasmas formed on targets with small Z, the conversion efficiency and limiting generated harmonic order depend on the delay between the ablation pulse and the pulse to be converted.     

Broadly wavelength- and pulse width-tunable high-repetition rate light pulses from soliton self-frequency shifting photonic crystal fiber integrated with a frequency doubling crystal

Soliton self-frequency shift (SSFS) in a photonic crystal fiber (PCF) pumped by a long-cavity mode-locked Cr:forsterite laser is integrated with second harmonic generation (SHG) in a nonlinear crystal to generate ultrashort light pulses tunable within the range of wavelengths from 680 to 1800?nm at a repetition rate of 20?MHz. The pulse width of the second harmonic output is tuned from 70 to 600?fs by varying the thickness of the nonlinear crystal, beam-focusing geometry, and the wavelength of the soliton PCF output. Wavelength-tunable pulses generated through a combination of SSFS and SHG are ideally suited for coherent Raman microspectroscopy at high repetition rates, as verified by experiments on synthetic diamond and polystyrene films.     

Second Harmonic Generation in Microstructured Barium Titanate

We investigate the second harmonic generation under femtosecond pulse-periodic laser radiation in barium titanate in the form of ceramics, in pores of a globular photonic crystal, and in a water colloidal suspension. We measure the dependence of the second harmonic radiation intensity on the incident laser power. Excitation of the second harmonic was carried out by powerful (10⁸ W) pulses of a solid-state Yb:KGW laser (wavelength, 1,026 nm) operating at 200 kHz. We estimate the efficiency of the second harmonic generation in various microstructured phases of barium titanate and show that the threshold of plasma formation in a suspension of barium titanate microparticles in water is substantially higher than in ceramics and in the ferroelectric photonic crystal. The second-harmonicgeneration power can be significantly increased in a water suspension of barium titanate microparticles.     

Harmonic generation in bismuth triborate (BiB3O6)

We report a study of second- and third-harmonic generation in BiB₃O₆ (BiBO). The effective nonlinearity, phase-matching angle, acceptance bandwidth, and walk-off are calculated and analyzed within the principal planes of the optical indicatrix. In the experiment, the phase-matched harmonic generation is investigated within the xz and yz planes. Also, the temperature dependence of the noncritical phase matching for laser radiation propagating along the z axis is measured for second-harmonic generation (SHG) at crystal temperatures of 25–265^∘C. The corresponding wavelengths of the laser radiation are in the range of 1.16 to 1.34μm. In addition, SHG of 1342-nm radiation of a q-switched Nd:YVO₄ laser system is investigated for noncritical and critical phase matching. The achieved conversion efficiencies are 59% and 20%, respectively. Besides SHG, third-harmonic generation (THG) of 1064-nm, ns laser pulses is investigated. The measured conversion efficiency is as high as 34%. For THG the properties of BiBO are compared with those of BBO and LBO.     

Sensitivity of Narrow-Band Intracavity Laser Spectroscopy in Generation of the Second Harmonic

We carried out an analysis of the sensitivity of the method of intracavity laser spectroscopy with intracavity generation of the second harmonic to small frequency-independent losses evaluated by measuring the energies of laser-radiation pulses. We consider laser behavior with a constant and modulated quality factor of the cavity resonator. It is shown that the sensitivity of the method may be improved by an order of magnitude or higher by transforming the frequency of radiation and selecting the optimal parameters of the active medium pumping, nonlinear crystal, Q-factor of the cavity, and the means of its modulation. Measurement of the radiation power at the frequency of the second harmonic expands the range of laser-operation time regimes in which an increase in the sensitivity of the method is ensured.     

Nonlinear photoionization and laser-induced damage in silicate glasses by infrared ultrashort laser pulses

We show that photoionization of wide band gap silicate glasses by infrared ultrashort laser pulses can occur without laser-induced damage. Two glasses are studied, fused silica and a multi-component silicate photo-thermo-refractive (PTR) glass. Experiments are performed by low numerical aperture focusing of ultrashort laser pulses (100 fsec<τ<1.5 psec) at the wavelengths 780 nm, 1430 nm, and 1550 nm. Filaments form inside both glasses and are visibly observable due to intrinsic luminescence. Keldysh’s theory of nonlinear photoionization is used to model the formation of filaments and values of about 10¹³ W cm⁻² for the laser intensity and 10¹⁹ cm⁻³ for the free electron density are estimated for stable filaments to arise. Laser-induced damage is studied by the generation of a third harmonic from an interface created between a damage site and the surrounding glass matrix. It is found that third harmonic generation occurs only after several thousands of laser shots indicating that damage is not a single-shot phenomena. The ability to photoionize PTR glass without damage by ultrashort laser pulses offers a new approach for fabricating diffractive optical elements in photosensitive glass.     

The nonlinear optical coefficient,phasematching, and optical damage in the chalcopyrite AgGaSe2

We have made a direct measurement of the absolute nonlinear coefficient for AgGaSe₂ by phasematched second harmonic generation. The measured value is d₃₆ = (3.24 ± 0.50) × 10^?11 m/V. For CO and Co₂ lasers the observed phasematching angles for second harmonic generation and frequency mixing are within one degree of the values calculated by fitting the reported index of refraction data to Sellmeier equations. At 1.06 μm the optical damage threshold depends on the number of incident laser pulses. For 1000 pulses damage occurs at 11 MW/cm². The samples were cut from crack-free single crystal boules with absorption coefficient smaller than 0.1 cm^? at 10.6 μm.     

Characterization of laser-diode end-pumped intracavity frequency doubled, passively Q-switched and mode-locked Nd:YVO4 laser

Simultaneous Q-switching and mode-locking in a laser-diode end-pumped intracavity frequency doubled Nd:YVO₄/KTP green laser using Cr⁴⁺:YAG saturable absorber is experimentally demonstrated. The influence of the initial transmission (T₀) of the Cr⁴⁺:YAG crystal on the Q-switched mode-locked green pulses as well as on the average green power is characterized by using Cr⁴⁺:YAG crystal with various T₀. The effect of T₀ on the pulse build-up time in intracavity second harmonic configuration is theoretically investigated. It was found that the depth of modulation for the mode-locked pulses is greatly improved at the second harmonic wavelength as compared to that for the fundamental wavelength. The average pulse duration of the individual mode-locked pulse for the second harmonic beam measured to be less than 500 ps with a repetition rate of 400 MHz.     

Frequency doubling of phase-modulated femtosecond laser pulses in periodically poled and chirped nonlinear crystals

The second harmonic generation (SHG) at a wavelength of 0.8 μm by 50-and 10-fs pulses with and without phase modulation (PM) was systematically studied in LiNbO₃ crystals with regular domain structure and linearly varied domain thickness. The main results were obtained by numerical method, taking into account the difference between group velocities of interacting pulses and the group-velocity dispersion. In the approximation of the given field of the fundamental radiation, an analytical expression was derived for the spectral density of the second harmonic in the periodically poled nonlinear crystal (PPNC) under nonstationary excitation conditions. It was numerically found that the conversion efficiency of about 90% can be achieved by doubling the frequency of 50-fs laser pulses without PM in the LiNbO₃ PPNC. The maximum conversion efficiency for the SHG by PM pulses is achieved at a certain optimum chirp step in the crystal domain length, which depends on both the value and sign of frequency modulation.     

晶体环境下高次谐波谱的截止频率分析

通过数值求解中红外飞秒光脉冲与一维单电子多阱势相互作用的含时薛定谔方程, 研究了晶体环境下的高次谐波发射光谱, 发现了晶体谐波谱的截止位置公式.研究发现, 不同于气体环境下的谐波谱截止频率规律, 晶体谐波谱的截止频率与激光电场的峰值振幅及晶格参数成线性关系. 鉴于准经典力学的三步模型对于气体谐波截止频率的解释, 进一步采用准经典力学方法验证了晶体谐波截止位置规律的正确性. 关键词： 中红外飞秒光脉冲 晶体 高次谐波 截止频率     

Absorption and second harmonic emission from interaction of femtosecond laser pulses with microspherical droplets

In this paper, the interaction of femtosecond laser pulses with droplets microplasma at the intensity of 10¹⁶ W/cm² is theoretically studied. Laser absorption, suprathermal electron generation, and second harmonic generation are discussed. Using an analytical model and a 2D particle-in-cell code, we find that the dominated mechanism is resonant absorption in the interaction of femtosecond laser pulses with droplets for the misrospherical geometry.     

Double-pulse laser ablation applied to reactive PLD method for synthesis of carbon nitride film: A second laser shot delay

Carbon nitride films were deposited using ablation of graphite target by second harmonic radiation of Nd:YAG laser in nitrogen atmosphere. To produce high hardness films, the deposited particles should have sufficient kinetic energy to provide their efficient diffusion on a substrate surface for formation of crystal structure. However, a shock wave is arisen in ambient gas as a consequence of laser plasma explosive formation. This shock wave reflected from the substrate interacts with plume particles produced by the first laser pulse and decreases their kinetic energy. This results in decrease of film crystallinity. To improve film quality, two successive laser pulses was proposed to be used. At adjusting time delay, the particles induced by the second pulse wilt serve as a piston, which will push forward both stopped particles ablated by the first pulse and arisen from chemical reactions in ambient gas. An X-ray photoelectron spectroscopy (XPS) analysis of deposited films has shown an increase of content of sp ³ carbon atoms corresponding to crystalline phase, if double-pulse configuration is employed. The luminescence of excited C₂ and CN molecules in laser plume at different distances from the target was studied to optimize the delay between laser pulses.     

Relativistic high harmonics and (sub-)attosecond pulses: relativistic spikes and relativistic mirror

Using particle-in-cell simulations, we study high harmonic generation from overdense plasmas in the relativistic regime. Different incidence angles as well as different laser polarizations are considered and scalings are recovered. It is shown that the theory of relativistic spikes and the BGP power-law spectra [Phys. Rev. E 74, 046404 (2006)] describes well the normal incidence and s-polarized obliquely incident laser pulses. In the case of p-polarized laser pulses, exceptions from the BGP theory can appear when the quasi-static vector potential build-up at the plasma boundary becomes equal to that of the laser. In this case, the spectrum flattens significantly and has a lower cutoff.     

Efficient phase-matched third harmonic light generation in hexafluoroisopropanol solutions of a pyrimidonecarbocyanine dye

The phase-matched collinear third harmonic generation of picosecond laser pulses in a 0.0825 molar hexafluoroisopropanol solution of a pyrimidonecarbocyanine dye is studied. The fundamental pulses are generated in a passively mode-locked Nd-phosphate glass laser. The saturation of third harmonic generation at high intensities is investigated. The influences of two-photon absorption, excited-state absorption, and amplified spontaneous emission are discussed. For input peak intensities above 10¹¹ W/cm² a third harmonic energy conversion of about 2×10^–4 is achieved.     

Generation of tunable picosecond pulses in the ultraviolet region down to 197 nm

Tunable picosecond pulses in the ultraviolet region down to 197 nm with ? 20 kW peak power are generated by the sum frequency mixing of fourth or third harmonic pulses of a mode-locked YAG laser with tunable pulses produced by a LiNbO₃ parametric oscillator pumped by second harmonic pulses of the YAG laser by using a KB5 or KDP crystal.     

Passive Q-switching of the diode-pumped Er:YAG laser cavity with the Q-switch based on the Fe<Superscript>2+</Superscript>:ZnSe crystal

Repetitive-pulse generation of the diode-pumped Er:YAG laser (λ = 2.94 μm) in the free mode and in the mode of cavity passive Q-switching was achieved using a Q-switch based on the Fe²⁺:ZnSe crystal. When using pump pulses 3 ms long, the pulse-average output power of the Er:YAG laser in the free generation mode was 0.5W. In the passive Q-switching mode, giant pulses 180 ns long with an energy of 3 μJ were obtained.     

Third harmonic generation of CO2 laser radiation in AgGaSe2 crystal

Generation of third harmonic of CO₂ laser radiation has been obtained in a type-II, ϑ=57° cut 9 mm thick AgGaSe₂ crystal for the first time by sum-frequency-mixing of the fundamental with its second harmonic, the latter being obtained using another type-I, ϑ=55° cut 11 mm thick AgGaSe₂ crystal. The energy conversion efficiencies obtained for second harmonic and third harmonic generations are 6.3% and 2.4% respectively with the input fundamental pump power density of 5.9 MW/cm² only. The wavelength of the fundamental CO₂ laser radiation used for the generation of harmonics is 10.6 μm, P(20) line. A compact TEA CO₂ laser source has been built in the laboratory.     

Laser radiation tunable within the range of 4.35–5.45 <Emphasis Type="Italic">μ</Emphasis>m in a ZnTe crystal doped with Fe<Superscript>2+</Superscript> ions

We realized laser generation on a Fe²⁺:ZnTe crystal for first time. The crystal was pumped at room temperature by 40 ns pulses of an Er:YAG laser operating at a wavelength of 2.94 μm in the Q-switching mode. The output energy of the Fe²⁺:ZnTe laser was 0.18 mJ at a slope efficiency of 2.4% with respect to absorbed pumping energy. We achieved tuning of the Fe²⁺:ZnTe laser generation wavelength within the range of 4.35–5.45 μm using a prism-dispersion cavity.     

Ellipticity dependence of atomic and molecular high harmonic generation

High harmonic generation is compared in the dependence on the ellipticity of the fundamental laser radiation for an atomic and a molecular system. In particular argon and nitrogen are compared employing molecular beams and intense ( 3×10¹⁴ W/cm²) and ultrashort (80 fs) 800 nm laser pulses. It turns out that for all the harmonics under investigation (H5, H13 and H21) the harmonic yield decreases slower with the ellipticity for the molecule than for the atom. This indicates differences in atomic and molecular high harmonic generation. Received 24 April 2002 Published online 24 September 2002