Enhanced photoemission and ionization of He+ by simultaneous irradiation of fundamental laser and high-order harmonic pulses

We simulate the response of He⁺ exposed simultaneously to fundamental and 27th harmonic pulses from an intense Ti:sapphire laser. High-order harmonic emission from He⁺ is enhanced by 17 orders of magnitude compared with the case of the fundamental pulse alone. Moreover, while an individual 10 fs laser with a fundamental wavelength of 800 nm and a peak intensity of 3×10¹⁴ W/cm², or its 27th harmonic pulse with a peak intensity of 10¹³ W/cm², ionizes no more than 5×10^-6 of He⁺, their combined pulses lead to a surprisingly high He²⁺ yield of 17%. The underlying mechanism is either harmonic generation from a coherent superposition of states or two-color frequency mixing, depending on the laser wavelength. PACS 32.80.Rm; 42.50.Hz; 42.65.Ky     

High harmonic XUV spectral phase interferometry for direct electric-field reconstruction

We demonstrate the first experimental complete temporal characterization of high-harmonic XUV pulses by spectral phase interferometry, with an all-optical setup. This method allows us to perform single-shot measurements of the harmonic temporal profile and phase, revealing a remarkable shot-to-shot stability. We characterize harmonics generated in argon by a 50 fs 800 nm laser pulse. The 11th harmonic is found to be 22 fs long with a negative chirp rate of -4.8 x 10(27) s(-2). This duration can be reduced to 13 fs by modulating the polarization of the generating laser. The technique is easy to implement and could be routinely used in femtosecond XUV pump-probe experiments with harmonics.     

Two-Photon Ionization of He through a Superposition of Higher Harmonics

We present experimental results and theoretical analysis of two-photon ionization of He by a superposition of the 7th to the 13th harmonic of a Ti:sapphire laser. Solving the time-dependent Schr?dinger equation for He in a coherent polychromatic field, the He+ yield is calculated. From this yield the number of He+ ions produced has been estimated and found in reasonable agreement with its measured value. The present results establish the feasibility of a second-order autocorrelation measurement of superposition of harmonics, and thus they represent the precursor towards the direct temporal characterization of attosecond pulse trains.     

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。     

附加谐波脉冲生成强的39阿秒孤立脉冲

采用多周期800 nm激光组合它的27次谐波脉冲生成超短、宽频的孤立阿秒脉冲.研究表明,脉宽为1 fs的27次谐波脉冲可以有效地控制电子动力学过程.将其加入到单色激光场的特定时域,可以控制电离概率在半个光学周期内迅速提升,使得谐波的转化效率相对于单色场情形增强4个数量级,并实现单一的短量子路径选择,出现频宽为108 eV的超连续辐射谱,叠加该连续谱140次到210次谐波获得了脉宽为39as的强、短孤立脉冲.与文献[7]中采用5 fs/800 nm激光附加紫外阿秒脉冲的方法相比,该方案生成的连续谱频带增宽一 关键词： 组合激光脉冲 连续辐射谱 阿秒脉冲     

Strong resonance enhancement of a single harmonic generated in the extreme ultraviolet range

We report the demonstration of strong resonance enhancement of a single high-order harmonic in the extreme ultraviolet (XUV) region generated from the interaction of a femtosecond pulse with low-ionized In ablation. A strong 13th harmonic (61.2 nm) of Ti:sapphire laser radiation with output intensity almost two orders of magnitude higher than neighboring harmonics was observed in these studies. The high conversion efficiency of the 13th harmonic (8 x 10(-5)) is attributed to multiple collisions of electron trajectories with the origin due to multiphoton resonance with the In ion.     

Pulse width measurement of high-order harmonics by autocorrelation

Pulse widths of the 7th and 9th harmonics of a Ti:sapphire (TiS) laser have been measured by an autocorrelation technique using two-photon and three-photon ionization of He and Ar as nonlinear phenomena. The pulse widths of the 7th and 9th harmonics were 47 fs and 27 fs, respectively, where the pulse width of the fundamental pulse was 34 fs. The pulse width of the 9th harmonic depends strongly on the peak intensity of the fundamental pulse. These results can be explained by quantum theory by taking into account the temporal and spatial distribution of the fundamental beam. Received: 15 June 1999 / Revised version: 8 October 1999 / Published online: 2 February 2000     

叠加态下3色场波形优化增大谐波辐射截止能量及强度

在He~+离子1s态和2s态的叠加态作为初始态时,提出一种优化3束激光场来增大谐波截止能量和强度的方法.结果表明:在叠加初始态下,谐波强度要比基态初始态下增强3个数量级以上.随后,在3色场波形优化下,谐波截止能量又得到增大,进而获得一个高强度、高光子能量的谐波光谱连续区.通过叠加光谱连续区上最后100次的谐波可以获得一个27 as的孤立阿秒脉冲.     

On the feasibility of performing non-linear autocorrelation with attosecond pulse trains

We present experimental results in which a second-order effect, namely two-photon ionization of atomic He induced by a superposition of harmonics, is observed. The harmonics are generated in a Xe gas-jet using a 790-nm 10-Hz femtosecond Ti:sapphire laser and are subsequently focused into a He gas-jet with a Kirkpatrick–Baez arrangement. The superposition is formed by using a thin In filter and it comprises the 7th to 13th harmonics. Solving the time-dependent Schrödinger equation for He in a polychromatic laser field, the He ⁺ ion yield is calculated as a function of the total XUV intensity. Using the calculated yield and taking into account the focusing and transmission properties of the arrangement, the number of He ⁺ ions produced per laser pulse is estimated and is found to be in reasonable agreement with its measured value. The total number of ions produced non-resonantly follows a nearly quadratic dependence on the harmonic intensity, thus establishing the feasibility of a second-order auto-correlation measurement of the superposition of harmonics, i.e., of a direct temporal characterization of attosecond pulse trains.     

Production of doubly charged helium ions by two-photon absorption of an intense sub-10-fs soft x-ray pulse at 42 eV photon energy

We report on the observation of doubly charged helium ions produced by a nonlinear interaction between a helium atom and photons with a photon energy of 42 eV which are generated with the 27th harmonic of a femtosecond pulse from a Ti:sapphire laser. The number of ions is proportional to the square of the intensity of the 27th harmonic pulse, and thus two-photon double ionization should be dominantly induced as compared with other nonlinear processes accompanying sequential ionization via a singly charged ion. This phenomenon is utilized to measure the pulse duration of the 27th harmonic pulse by using an autocorrelation technique, for the first time to our knowledge, and as a result a duration of 8 fs is found.     

Generation of picosecond UV pulses by stimulated anti-Stokes Raman scattering

Picosecond stimulated anti-Stokes Raman scattering of hydrogen gas in the ultraviolet region has been studied, using the second harmonic of a modelocked Nd³⁺: YAG laser as an incident pulse (25 ps, 532 nm, 10 mJ). Good conversion efficiency for higher-order anti-Stokes lines has been realized, yielding 2 μJ (200 kW, 10 ps) output for the 8th one at 192 nm. Some features of transient stimulated Raman scattering have been examined and discussed.     

HeH2+分子谐波辐射的空间分布

理论研究了HeH2+分子发射高次谐波的空间分布情况。结果表明：分子谐波发射主要集中在He核和H核附近。当核间距离较小时,He核辐射谐波强度要比H核辐射谐波强度高2~3个数量级。当核间距离较大时,He核辐射谐波强度要比H核辐射谐波强度高4~5个数量级。当空间非均匀激光场引入后,谐波截止能量得到延伸,并且,随着空间非均匀激光场位置由负向到正向移动(-100 a.u.到100 a.u.),谐波截止得到进一步延伸。但是He核辐射谐波强度依然大于H核。最后,通过叠加谐波可获得脉宽在60 as的超短脉冲。     

HeH2+分子谐波辐射的空间分布

理论研究了HeH2+分子发射高次谐波的空间分布情况。结果表明：分子谐波发射主要集中在He核和H核附近。当核间距离较小时,He核辐射谐波强度要比H核辐射谐波强度高2~3个数量级。当核间距离较大时,He核辐射谐波强度要比H核辐射谐波强度高4~5个数量级。当空间非均匀激光场引入后,谐波截止能量得到延伸,并且,随着空间非均匀激光场位置由负向到正向移动(-100 a.u.到100 a.u.),谐波截止得到进一步延伸。但是He核辐射谐波强度依然大于H核。最后,通过叠加谐波可获得脉宽在60 as的超短脉冲。     

Self-focusing, channel formation, and high-energy ion generation in interaction of an intense short laser pulse with a He jet

Using interferometry, we investigate the dynamics of interaction of a relativistically intense 4-TW, 400-fs laser pulse with a He gas jet. We observe a stable plasma channel 1 mm long and less than 30 microm in diameter, with a radial gradient of electron density approximately 5 x 10(22) cm(-4) and with an on-axis electron density approximately ten times less than its maximum value of 8 x 10(19) cm(-3). A high radial velocity of the surrounding gas ionization of approximately 3.8 x 10(8) cm/s has been observed after the channel formation, and it is attributed to the fast ions expelled from the laser channel and propagating radially outward. We developed a kinetic model which describes the plasma channel formation and the subsequent ambient gas excitation and ionization. Comparing the model predictions with the interferometric data, we reconstructed the axial profile of laser channel and on-axis laser intensity. The estimated maximum energy of accelerated ions is about 500 keV, and the total energy of the fast ions is 5% of the laser pulse energy.     

HeH~(2+)分子谐波辐射的空间分布

理论研究了HeH~(2+)分子发射高次谐波的空间分布情况.结果表明:分子谐波发射主要集中在He核和H核附近.当核间距离较小时,He核辐射谐波强度要比H核辐射谐波强度高2~3个数量级.当核间距离较大时,He核辐射谐波强度要比H核辐射谐波强度高4~5个数量级.当空间非均匀激光场引入后,谐波截止能量得到延伸,并且,随着空间非均匀激光场位置由负向到正向移动(-100 a.u.到100a.u.),谐波截止得到进一步延伸.但是He核辐射谐波强度依然大于H核.最后,通过叠加谐波可获得脉宽在60 as的超短脉冲.     

三色激光控制量子路径生成短于30阿秒的孤立脉冲

采用多周期的800 nm钛宝石激光组合1600 nm中红外脉 冲辐照氦离子产生高次谐波发射功率谱. 相对于单色场情形, 谐波谱出现明显的双平台结构, 且在第二平台区出现了光滑的连续辐射谱, 其转化效率相对于第一平台低了约两个数量级. 通过附加脉宽为1 fs的27次谐波脉冲到双色激光场的特定时域, 可以控制电子电离在半个光学周期内迅速提升, 获得了由单一短量子路径贡献的连续辐射谱, 使得第二平台区谐波的转化效率相对于组合场情形增强4个数量级, 且连续谱的频谱范围从第二平台区扩展到第一平台区, 叠加该连续谱190次到285次谐波生成了脉宽为29 as的强、短孤立脉冲.     

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.     

Crossed beam photodissociation imaging of HeH+ with vacuum ultraviolet free-electron laser pulses

Molecular photofragmentation has been studied by event imaging on HeH+ ions at 32 nm (38.7 eV) in a fast ion beam crossed with the free-electron laser in Hamburg (FLASH), analyzing neutral He product directions and energies. Fragmentation into He(1snl,n > or = 2)+H+ was observed to yield significant photodissociation at 32 nm with an absolute cross section of (1.4+/-0.7) x 10(-18) cm2, releasing energies of 10-20 eV. A clear dominance of photodissociation perpendicular to the laser polarization was found in contrast to the excitation paths so far emphasized in theoretical studies.     

Controlling HD+ and H+2 dissociation with the carrier-envelope phase difference of an intense ultrashort laser pulse

Carrier-envelope phase difference effects in the dissociation of the HD+ molecular ion in the field of an intense, linearly polarized, ultrashort laser pulse are studied in the framework of the time-dependent Schr?dinger equation. We consider a reduced-dimensionality model in which the nuclei are free to vibrate along the field polarization and the electrons move in two dimensions. The laser has a central wavelength of 790 nm and a pulse length of 10 fs with intensities in the range 6x10(14) to 9x10(14) W/cm(2). We find that the angular distribution of dissociation to p+D and H+d can be controlled by varying the phase difference, generating differences between the dissociation channels of more than a factor of 2. Moreover, the asymmetry is nearly as large for H+2 dissociation.     

Efficient high-order harmonic generation in a two-color laser field

We report efficient high-order harmonic generation achieved using a two-color laser field. By inserting a second-harmonic generation crystal in the path of a converging laser pulse, the overall efficiency for high-harmonic generation was enhanced by more than an order of magnitude. In addition, even-order harmonics were also generated. The 2(2n+1)th -order harmonics were very strong and, in particular, the 38th harmonic (21.6 nm), obtained with a single laser shot of 2 mJ, saturated the X-ray charge-coupled device (CCD) of an extreme-ultraviolet spectrometer even with an Al filter of 1.5 m thickness installed in front of the CCD. PACS 42.65.Ky; 32.80.-t; 42.65.Re