Tunable light sources based on high harmonics generation for time-resolved VUV spectroscopy

The project of set-up for time resolved femtosecond VUV spectroscopy, which is based on a high harmonic generation source and a VUV monochromator is presented. We discuss the generation conditions of quasi-continuous VUV spectrum via HHG in Ar using the intense chirped IR fundamental pulse and the relatively weak second harmonic of IR fundamental. The desired narrow VUV spectral range is selected by time compensated double monochromator with concave spherical diffraction gratings. PACS 42.65.Ky; 42.79.Dj; 78.47.+p; 39.30.+w     

Phase matching and focussing effects in noncollinear sum frequency mixing in the near VUV region

We demonstrate that focussing effects are extremely important in determining the bandwidth in sum frequency mixing of ultrashort pulses in the near VUV region. This effect is demonstrated with noncollinear sum frequency mixing performed between the fundamental and the third harmonic subpicosecond pulses of a Ti:sapphire laser. The spectrum of the generated fourth harmonic radiation is significantly broader (by 33%) than the theoretical spectrum obtained if focussing is not taken into account. We have developed a method of calculating the output bandwidth for sum frequency mixing of broadband spectral envelopes whose bandwidths correspond to ultrashort optical pulses, including focussing. The calculated and the measured spectra show excellent agreement.     

基于空间啁啾的宽带激光倍频技术

提出一种新型的宽带倍频方案，利用时空耦合效应将宽带的时间啁啾光转换成空间啁啾光，采用多块晶体并联、各晶体独立调谐的技术途径对空间啁啾光进行谐波转换，因此倍频效率与窄带激光倍频相当。理论研究表明，采用KDP晶体I类位相匹配，对中心波长为1 053 nm的宽带基频光实现了带宽约30 nm、转换效率大于60%的高效率宽带二倍频。而且倍频光仍为线性啁啾宽带光，具备可压缩性。     

High-energy, high-contrast, multiterawatt laser pulses by optical parametric chirped-pulse amplification

We describe a compact, reliable, high-power, and high-contrast noncollinear optical parametric chirped-pulse amplifier system. With a broadband Ti:sapphire oscillator and grating-based stretching and compression, the chirped pulses are amplified from 0.1 nJ to 122 mJ in type I beta-barium borate optical parametric chirped-pulse amplifiers with a total gain of over 10(9) at 10 Hz repetition rate. Pulse compression down to 19-fs duration achieved after amplification indicates a peak power of 3.2 TW at an average power of 0.62 W. The prepulse contrast is measured to be less than 10(-8) on picosecond time scales.     

Generation of femtosecond vacuum-ultraviolet pulses

High power femtosecond pulses in the Vacuum Ultra Violet (VUV) have been generated through the nonlinear interaction of femtosecond KrF pulses with xenon and argon gas. Under near resonant two photon excitation of xenon by a femtosecond KrF laser, parametric four wave mixing processes lead to VUV pulses at 147 and 108 nm with pulse energies in the 10 µJ range. Tuning is demonstrated by mixing the KrF pulse with a 500 fs dye laser pulse at 497 nm, resulting in 165 nm emission. In argon, a three photon resonance leads to third harmonic generation at 83 nm and micro joule level pulses near 127 nm generated by a six wave mixing process. Since the spectra of the VUV pulses show an ionization-induced blue shift with increasing KrF laser intensity, the VUV pulses can be shown to have temporal duration less than the pulse width (450 fs) of the KrF laser. Blue shifting of the third harmonic of the KrF laser in argon is dominated by a reduction in the neutral gas density rather than by an increase in the electron density.     

Pulse compression of a high-order harmonic

The fifth harmonic pulses of an intense femtosecond Ti:sapphire laser were experimentally shown to be negatively chirped by using an LiF plate as a positive dispersive medium. The chirp of the harmonic pulse originates from the intensity-dependent atomic dipole phase, which is estimated to be proportional to 25 U_p, where U_p is the ponderomotive energy. Consequently, we have succeeded in compressing the chirped pulses to 13 fs by compensating the intrinsic negative chirp. Chirp effects of the fundamental laser on the pulse width of the fifth harmonic were consistent with the negative chirp of the fifth harmonic.     

Destructive interference during high harmonic generation in mixed gases

We report on the first experimental evidence of the destructive and constructive interference of high harmonics generated in a mixed gas of He and Ne, which facilitates the coherent control of high harmonic generation. Theoretically, we develop an analytical model of high harmonic generation in mixed gases and succeed in reproducing the experimental results and deriving the optimization conditions for the process. The observed interference modulation is attributed to the difference between the phases of the intrinsically chirped harmonic pulses from He and Ne, which leads to a novel method for broadband measurement of the harmonic phases and for observing the underlying attosecond electron dynamics.     

Pulse inversion ultrasound modulated optical tomography

Pulse inversion acoustic imaging is useful as it allows second harmonic imaging to be obtained with short acoustic pulses. This allows high axial resolution, but removes any overlap in the frequency spectra of fundamental and harmonic. We demonstrate pulse inversion ultrasound modulated optical tomography using an optical speckle based detection method. Inverted and non-inverted acoustic pulses combined with synchronized strobed illumination are applied to an optically scattering medium. Over the acquisition time of a camera, multiple pulses are summed and at the next frame the phase of the ultrasound is shifted by π/2 and the process repeated. Combining the two frames allows a second harmonic signal to be obtained. A reduction in linewidth is observed (DC=9.26 mm, fundamental=4.02 mm, second harmonic=2.43 mm) in line scans of optically absorbing objects embedded in a scattering medium (thickness=16 mm, scattering coefficient=2.3 mm(-1), anisotropy factor=0.938).     

Generation of subpicosecond vacuum ultraviolet pulses at 126 nm by using harmonics of a subpicosecond Ti:Sapphire laser

Subpicosecond vacuum ultraviolet (VUV) pulses at the wavelength of 126 nm have been generated in rare gases as a result of the 7th harmonic radiation of a subpicosecond Ti:Sapphire laser oscillating at 882 nm. The VUV harmonic intensity was optimized in Xe at the pressure of 1.2 Torr. The behavior of the harmonic emission was qualitatively reproduced by the classical nonlinear optics. The increase of the harmonic intensity was limited by multiphoton ionization of Xe.     

Broadband second harmonic generation of an optical frequency comb produced by four-wave mixing in highly nonlinear fibers

We demonstrate broadband second harmonic generation of low-energy pulses produced by injecting two single-frequency lasers into a highly nonlinear fiber. Full nonlinear conversion of the corresponding spectra, consisting of broadband (∼200 nm) optical frequency combs at ∼1580 nm, were obtained by using conventional birefringence phase-matching in two BIBO crystals (2-mm and 100-μm long) with a normal incidence configuration. The crystals were not tilted and the pulses were not compressed. This broadband conversion results from the large phase-matching bandwidth of the nonlinear BIBO crystals at ∼1550 nm, but also seems to be a consequence of a fundamental comb with small spectral phase variation.     

Engineerable compression of ultrashort pulses by use of second-harmonic generation in chirped-period-poled lithium niobate

We demonstrate the use of an aperiodic quasi-phase-matching (QPM) grating to generate second-harmonic pulses that are stretched or compressed relative to input pulses at the fundamental frequency. We frequency doubled an externally chirped erbium-doped fiber laser generating 17-ps (FWHM) pulses at 1560nm to produce near-transform-limited 110-fs (FWHM) pulses at 780nm by use of a 5-cm-long lithium niobate crystal poled with a QPM grating chirped from an 18.2- to a 19.8-microm period.     

空气中激光等离子体通道的三次谐波光谱特性研究

对不同条件下强激光在空气中形成等离子体通道的三次谐波光谱特性进行了研究。单脉冲能量12 mJ,脉宽30 fs,重复频率10 Hz,中心波长795 nm的飞秒激光脉冲经0.5 m焦距的凹面镜聚焦,在空气中形成了等离子体通道, 并在前 向观测到谱线半峰全宽（FWHM）为15 nm的三次谐波。随着脉冲啁啾的变化,三次谐波的光谱出现红移或兰移,当激光脉冲附带+1.3×105fs2的二阶色散时,三次谐波谱线红移且谱峰强度增长了两倍。同时 ,通过改变可编程声光色散滤波器（AOPDF）光谱调制的位置（Hole position）,三次谐波的光谱也发生频移。     

Generation of high average power, 7.5-fs blue pulses at 5 kHz by adaptive phase control

The spectral width of a 5-kHz Ti:sapphire laser system was broadened by spectral control in a regenerative amplifier consisting of broadband chirped mirrors. The dispersion over the wide spectral range was compensated by a deformable mirror along with a genetic algorithm, resulting in a pulse width of 15 fs. The pulse width is the shortest, to our knowledge, in chirped pulse amplification systems with a regenerative amplifier. The phase distortion of broadband frequency doubling in addition to the Ti:sapphire laser was compensated by using the self-diffraction intensity in sapphire as the feedback signal into the genetic algorithm, resulting in a pulse width of 7.5 fs. The average power of the second harmonic was 1 W with a fundamental input of 7 W.     

Spectral phase distribution retrieval through coherent control of harmonic generation

The temporal intensity distribution of the third harmonic of a Ti:sapphire laser generated in Xe gas is fully reconstructed from its spectral phase and amplitude distributions. The spectral phases are retrieved by cross correlating the fundamental laser frequency field with that of the third harmonic, in a three laser versus one harmonic photon coupling scheme. The third harmonic spectral amplitude distribution is extracted from its field autocorrelation. The measured pulse duration is found to be in agreement with that expected from lowest order perturbation theory both for unstretched and chirped pulses.     

Broadband coherent anti-Stokes Raman scattering spectroscopy using soliton pulse trains from a photonic crystal fiber

Pulse trains of fundamental soliton pulses with different center wavelengths and delay times from a photonic crystal fiber were generated and used as Stokes optical pulses in coherent anti-Stokes Raman scattering (CARS) spectroscopy. The pulse trains were created by shaping optical pulses with a pulse shaper and their waveforms were measured by a cross-correlation frequency-resolved optical gating method. By the use of pulse trains, the time required for obtaining broadband CARS signals was reduced to be about one third compared with our previous study without using pulse trains. With this setup, broadband CARS signals between 500 and 3100 cm⁻¹ of a single polystyrene bead sample have been measured and the most of the Raman peaks in this frequency range of samples have been observed clearly.     

Supercontinuum extending from > 1000 to 250 nm, generated by focusing ten-fs laser pulses at 805 nm into Ar

Ten femtosecond pulses at 805 nm with energy up to 1 mJ were produced by self-phase modulation of 45-fs pulses in Ar at atmospheric pressure and subsequent compression by chirped mirrors. Focusing part of this radiation again into Ar at atmospheric pressure generates a single filament with broadband emission covering the range from > 1000 to 250 nm. This range extends farther into the UV than previously observed with such low energies, overlapping even the region of the third harmonic. Only a small fraction of the power is contained outside the central spot. Using a simple prism compressor, pulses were obtained with durations of 70 fs and energies of 700 nJ in the range 270–290 nm.This revised version was published online in March 2005. The last name of the corresponding author W. Fuß was corrected.     

小宽带堆积啁啾脉冲传输放大特性

 采用啁啾脉冲堆积的方法可获得ns量级宽带整形激光脉冲,对堆积啁啾脉冲时间波形的影响因素及传输放大后脉冲波形与光谱形状的特性进行了研究。结果表明：在传输过程中脉冲的演化规律与窄带脉冲的演化规律基本一致,而且传输放大过程也不会改变脉冲的调制结构,但光谱形状在传输放大过程中发生了变化,初步认为是由非线性效应造成的;小宽带堆积啁啾脉冲具有与窄带脉冲基本一致的的增益水平。     

Harmonic Extension and Enhancement Using a Two-Color Chirped Pulse and an Ultrashort Ultraviolet Pulse

A promising method to both extend the harmonic energy and enhance the harmonic intensity is presented when a He atom is exposed to the combination of a two-color chirped pulse and an ultrashort ultraviolet pulse. It is found that: (1) with the introduction of the two chirps, the harmonic energy has been remarkably extended; (2) by properly adding an ultrashort ultraviolet pulse to this synthesized two-color chirped pulse, the harmonic yield is enhanced by 3 orders of magnitude compared with the two-color chirped case; (3) the harmonic spectrum higher than the 96th order shows an ultrabroad supercontinuum with a 395 eV bandwidth, and the proper superposition over the harmonics directly produced a series of intense 40 as pulses which is 3 orders of magnitude higher than that in the two-color chirped case.     

Yb:YAG Innoslab amplifier: efficient high repetition rate subpicosecond pumping system for optical parametric chirped pulse amplification

We report on a Yb:YAG Innoslab laser amplifier system for generation of subpicsecond high energy pump pulses for optical parametric chirped pulse amplification (OPCPA) at high repetition rates. Pulse energies of up to 20 mJ (at 12.5 kHz) and repetition rates of up to 100 kHz were attained with pulse durations of 830 fs and average power in excess of 200 W. We further investigate the possibility to use subpicosecond pulses to derive a stable continuum in a YAG crystal for OPCPA seeding.     

采用光栅角色散的宽带二倍频及聚焦特性分析

针对带宽为20 nm左右、中心波长为1 053 nm的线性啁啾宽带激光,分析了采用光栅角色散方式宽带二倍频的原理,讨论了光栅角色散性能及光栅加工误差引入的基频光位相扰动对二倍频光转换效率及聚焦特性的影响.研究结果表明:采用光栅角色散方式的宽带二倍频光的转换效率、脉冲宽度和带宽均明显增大;在0～22 nm基频光带宽范围内,二倍频光均可保持80％左右的转换效率;对于入射基频光带宽为22 nm的情况,光栅角色散率在30～80 μrad/nm范围内变化时,宽带二倍频转换效率均可保持在70％以上;基频光有位相扰动时,二倍频光带宽对二倍频聚焦光斑的主瓣影响不大,但对旁瓣有一定的匀滑作用,采用光栅角色散方式宽带二倍频的聚焦光斑旁瓣的匀滑效果更为明显.