椭圆偏振强激光场中准直的乙炔分子的高次谐波发射

We perform an experimental study on high-order harmonic generation (HHG) of aligned acetylene molecules induced by a 35-fs 800-nm strong laser field, by using a home-built HHG spectrometer. It is observed that the molecular HHG probability declines with increasing the laser ellipticity, which is in consistence with the deduction from the well-known tunneling-plus-rescattering scenario. By introducing a weak femtosecond laser pulse to nonadiabatically align the molecules, we investigated the molecular orbital effect on the HHG in both linearly and elliptically polarized driving laser fields. The results show that the harmonic intensity is maximum for the molecular axis aligned perpendicularly to the laser electric field. It indicates that both the highest occupied molecular orbitals (HOMO) and HOMO-1 contribute to the strong-field HHG of acetylene molecules. Our study should pave the way for understanding the interaction of molecules with ultrafast strong laser fields.     

High-order harmonic generation by double-photoionization accounting for the correlation between continuum electrons

We report systematic analytical and numerical studies of the double-ionization of atoms by strong fields, leading to high-order harmonic generation (HHG). The model properly account for the correlation between the double continuum electrons. Calculations are performed within the frame of non-perturbative fully quantum-mechanical strong-field-approximation approach (SFA). To implement the model, we chose He atom as nonlinear medium. The production of HHG is investigated over a broad range of intensities 7.5×10¹⁴ to 4.5×10¹⁵ W/cm² using Nd:YAG and Ti:Sapph incident lasers. The results are in quite good agreement with the cutoff low. We demonstrate that the length of the plateau grows with the laser intensities. We obtain harmonics up to the order 427th and 479th with Nd:YAG and Ti:Sapph incident lasers, respectively. We show that the nature of the incident laser introduces significant changes in the HHG emission rate. This work confirms the predominance of single-ionization processes during the interaction of He with laser fields.     

High-order harmonic generation from organic molecules in ultra-short pulses

We have studied high-order harmonic generation (HHG) from organic molecules irradiated with near-infrared high intensity laser pulses of 70 fs and 240 fs duration. The molecular systems studied were the aromatics benzene and naphthalene and the alkanes cyclopropane and cyclohexane (cyclic) and n-hexane (linear). Harmonic intensities were measured both as a function of laser intensity (in the range 5×10¹³-5×10¹⁵ W cm^-2) and as a function of ellipticity of the laser field polarisation. The results were compared with those from the xenon atom. For 70 fs pulses, harmonic generation from the organic systems was similar to that of xenon, revealing an atom-like behaviour for molecules when the laser pulse duration is shorter than the fragmentation timescale of the molecule. We note significant differences between molecules with respect to HHG efficiencies and the suppression of HHG in larger species. We discuss these differences in the context of the molecular properties, electronic structure and behaviour of ionisation and fragmentation that result in enhancement of field ionisation in larger systems. Study of the polarisation ellipticity dependence of HHG shows that the harmonic yield in molecules is less sensitive to the polarisation than for atoms (xenon). This is consistent with the expected behaviour given the larger recollision cross-section presented by the core in the molecular system compared to the atom. Our results suggest that study of HHG from molecules exposed to ultra-short pulses is potentially a powerful tool for understanding the electron dynamics of molecules exposed to an intense field. Received 14 September 2000 and Received in final form 6 December 2000     

Isolated sub-30-attosecond pulse generation using a multicycle two-color chirped laser and a static electric field

We present a theoretical investigation of high-order harmonic generation in a chirped two-color laser field, which is synthesized by a 10-fs/800-nm fundamental chirped pulse and a 10-fs/1760-nm subharmonic pulse. It is shown that a supercontinuum can be produced using the multicycle two-color chirped field. However, the supercontinuum reveals a strong modulation structure, which is not good for the generation of an isolated attosecond pulse. By adding a static electric field to the multicycle two-color chirped field, not only the harmonic cutoff is extended remarkably, but also the quantum paths of the high-order harmonic generation （HHG） are modified significantly. As a result, both the extension of the supercontinuum and the selection of a single quantum path are achieved, producing an isolated 23-as pulse with a bandwidth of about 170.6 eV. Furthermore, the influences of the laser intensities on the supercontinuum and isolated attosecond pulse generation are investigated.     

High-order harmonics generation by few-cycle and multi-cycle femtosecond laser pulses

This paper investigates experimentally high-order harmonic generation(HHG) of neon gas with 5-fs and 25-fs driving laser pulses.It has been demonstrated that the cutoff energy of the harmonic extreme ultraviolet photons is extended to 131 eV and the HHG spectrum near the cutoff region becomes continuum as the driving laser pulse duration is 5 fs;whereas much lower cutoff photon energy and discrete harmonic spectrum near the cutoff region are presented as the laser pulse duration is 25 fs.The results can be explained by the fact that neutral atoms can be exposed to more intense laser field before they are depleted by ionization because of the extremely short rising time of the few-cycle pulse.The 5-fs driving laser pulse paves the way of generation of coherent x-ray in the water window and single attosecond pulse.     

Time-energy properties of an attosecond extreme ultra-violet pulse

The time-energy properties of high-order harmonic generation (HHG) are calculated for a linearly polarized 7-fs laser pulse with different carrier-envelope phases (CEPs). The quantum trajectory paths that contribute to an as (1 as=10-18 s) pulse in HHG are identified. The laser-duration dependence and the CEP dependence of HHG energy property are investigated. The study shows that an as extreme ultra-violet (XUV) pulse can be selected from HHG spectrum near cut-off energy with a bandpass optical filter. The theoretical prediction of the pulse duration is proportional to bandwidth. Analysis suggests that a measured narrowband as XUV pulse may consist of instantaneous shorter pulses each dependent on laser pulse duration, intensity, and CEP. These information can be used as references for producing, selecting, improving and manipulating (timing) as pulses.     

脉冲激光偏振方向对氮分子高次谐波的影响－－基于含时密度泛函理论的模拟

采用含时密度泛函方法，结合赝势模型和电子交换相关作用的广义梯度近似，模拟了氮分子在超强飞秒激光脉冲作用下的高次谐波产生现象，并研究了激光脉冲偏振方向对氮分子高次谐波的影响.结果表明氮分子的高次谐波谱具有典型原子谐波谱的特征；谐波谱强度随着θ(激光偏振方向与分子轴向夹角)的增大而减小.这与J.Itatanl在Nature上报道的实验结果基本一致. 关键词： 含时密度泛函理论 激光偏振方向 高次谐波 氮分子     

Generation of isolated attosecond pulses with a specific waveform two-color laser field

We theoretically propose a new method for generating intense isolated attosecond pulses during high-order harmonic generation (HHG) process by accurately controlling electron motion with a two-color laser field,which consists of an 800-nm,4-fs elliptically polarized laser field and a 1400-nm,～43-fs linearly polarized laser field.With this method,the supercontinua with a spectral width above 200 eV are obtained,which can support a ～15-as isolated pulse after phase compensation.Classical and quantum analyses explain the controlling effects well.In particular,when the pulse duration of the 800-nm laser field increases to 20-fs,sub-100-as isolated pulses can be obtained even without any phase compensation.     

激光强度依赖的阈下谐波产生机制

利用广义伪谱方法精确数值求解了氢原子在强激光场中的三维含时薛定谔方程,获得了强激光中氢原子的含时波函数,利用时间依赖的偶极矩的傅里叶变换得到了高次谐波谱,研究了氢原子在强激光场中发射低于电离阈值的谐波谱对激光强度的依赖性.研究发现,激光强度在低于电离阈值的谐波产生的通道选择的过程中扮演着重要角色,主要有两种量子通道对阈下谐波的产生有贡献,即广义的短轨道和长轨道,其中长轨道对激光场强度比较敏感.结合小波时频变换、经典轨道分析、以及强度依赖的量子通道选择分析,本文阐明了其背后的物理机制.     

High-order harmonic generation of pulses with multiple timescales: selection rules,carrier envelope phase and cutoff energy

ABSTRACT

High harmonic generation (HHG) is sensitive to the carrier envelope phase (CEP) of its driving laser field if it is a sufficiently short pulse (several-cycle pulse). Here we show that strong CEP effects can also be found in HHG from long duration multi-cycle pulses (up to 200?fs at 800?nm central wavelength). We find that HHG from multi-cycle pulses may be CEP dependent when the driving pulse exhibits two distinct timescales (multi-timescale pulse): (i) a short timescale associated with the average frequency, and (ii) a long timescale associated with the pulse’s temporal periodicity. The interplay of these timescales results in significant changes to both the cutoff frequency, and the appearance of symmetry allowed harmonics in the spectrum as function of CEP, similar to HHG from several-cycle pulses. We relate this effect to the multi-timescale intensity variations in the driving pulse, and construct an analytical condition to access the phenomenon. Lastly, we numerically demonstrate reconstruction of the CEP through HHG from long duration multi-timescale pulses. Our work may be useful in several areas of strong-field physics and attosecond science, for example, allowing spectroscopy of multi-timescale processes (e.g. HHG from vibrationally active media), and paving the way towards CEP characterisation using long pulses.     

Ionization effects on field-free molecular alignment observed with high-order harmonic generation

In this paper, high-order harmonic generation (HHG) is demonstrated to provide a sensitive way for studying the dynamic process in the field-free molecular alignment. The dependence of the harmonic yield and the degree of alignment on the intensity of aligning pulse is observed in impulsively aligned CO₂ molecules. A good agreement is found between the experimental and calculated results. At low pump intensities, the harmonic yield increases monotonously until the ionization induced refractive index gradient and neutral molecule depletion are significant. The results show that the optimum intensity is around 8.95 × 10¹³ W/cm²; this value is related to the molecular ionization potential.     

强激光场中模型氢原子和真实氢原子产生高次谐波的比较

通过数值求解原子在强激光场中的含时薛定谔方程,研究了有库仑奇点和无库仑奇点的一维模型氢原子和三维真实氢原子产生高次谐波的特性.结果表明,有库仑奇点和无库仑奇点的一维模型氢原子和三维真实氢原子产生高次谐波的截止位置相同,但是高次谐波强度变化特征明显不同,进一步的研究表明,无库仑奇点的模型氢原子产生的高次谐波谱相对变化趋势与三维真实氢原子的高次谐波谱变化趋势是完全一致的.     

强激光场中模型氢原子和真实氢原子产生高次谐波的比较

通过数值求解原子在强激光场中的含时薛定谔方程,研究了有库仑奇点和无库仑奇点的一维模型氢原子和三维真实氢原子产生高次谐波的特性。结果表明,有库仑奇点和无库仑奇点的一维模型氢原子和三维真实氢原子产生高次谐波的截止位置相同,但是高次谐波强度变化特征明显不同,进一步的研究表明,无库仑奇点的模型氢原子产生的高次谐波谱相对变化趋势与三维真实氢原子的高次谐波谱变化趋势是完全一致的。     

Minimum structure of high-harmonic spectrafrom aligned O2 and N2 molecules

We experimentally investigated the high-order harmonic generation (HHG) from aligned O₂ and N₂ molecules in a linearly polarized laser field, and presented the dependence of the harmonic spectrum on the driving laser intensity and molecular alignment angle. The minimum position of HHG of O₂ varies with changing the laser intensity, which is caused by multi-orbital interference. However, the location of the observed minimum structure in N₂ harmonic spectrum remained unchanged upon changing the laser intensity. The mechanism of the spectral minimum for N₂ case is regarded as a Cooper-like minimum in HHG associated with the molecular electronic structure. This work indicates that harmonic spectroscopy can effectively uncover information about molecular structure and electron dynamics.     

Use of carbon-containing materials for efficient high-order harmonic generation of laser radiation

A systematic study of the high-order harmonic generation (HHG) of laser radiation in various carbon-containing plasma plumes (CCPPs) is presented. The materials studied are: graphite, boron carbide, C₆₀, polytetrafluoroethylene, polyethylene, carbon nanotubes, and soot. These studies show that CCPPs present the best plasma media for efficient lower order (from 9th to 19th) harmonic generation, while the harmonic cutoff restricted to the 29th order. The advantages of CCPPs for the harmonic generation are confirmed by comparison of the HHG conversion efficiency with that in Ag and In plasma plumes, where the highest conversion efficiency was reported. Use of two-color pump scheme allows further enhancement of harmonic yield from the CCPPs.     

Interference and spectral broadening of higher harmonics of laser radiation in plasma torches containing ions,nanoparticles, and fullerenes

We analyze the interference between two processes of higher harmonic generation (HHG) in plasma containing mixtures of different materials (silver and gold nanoparticles, as well as graphite and boron). We find that, for mixtures and individual ingredients, the limiting orders of generated harmonics of laser radiation approximately coincide with one another. At the same time, for plasma torches formed by the ablation of mixtures of materials, the HHG efficiency is considerably reduced compared to the case of the frequency transformation of laser radiation in individual ingredients of these mixtures as a result of destructive interference in the former case. We demonstrate a considerable spectral broadening of harmonics generated in laser plasma with pulses passed through filaments formed in air. In this case, the HHG efficiency increases fourfold (from 3 × 10⁻⁶ to 1.2 × 10⁻⁵) compared to the case of radiation free of phase and frequency modulation. The generation of harmonics is also observed upon the passage of 120-fs laser pulses through plasma containing fullerenes. In this case, the limiting value of generated harmonics achieves the 33rd order. The efficiency of harmonics in fullerene plasma considerably exceeds a similar process in silver plasma.     

A scaling law of high-order harmonic generation

Using a nonperturbative quantum electrodynamics theory of high-order harmonic generation (HHG), a scaling law of HHG is established. The scaling law states that when the atomic binding energy E_b, the wavelength λ and the intensity I of the laser field change simultaneously to kE_b, λ/k, and k³I, respectively. The characteristics of the HHG spectrum remain unchanged, while the harmonic yield is enhanced k³ times. That HHG obeys the same scaling law with above-threshold ionization is a solid proof of the fact that the two physical processes have similar physical mechanisms. The variation of integrated harmonic yields is also discussed.     

相对论圆偏振激光与固体靶作用产生高次谐波

超短超强激光与固体靶表面等离子体相互作用可以通过高次谐波的方式产生从极紫外到软X射线波段的相干辐射,获得飞秒甚至阿秒量级的超短脉冲,可用于观测原子或分子中的电子运动等超快动力学过程.本文实验研究了相对论圆偏振飞秒激光与固体靶相互作用的高次谐波产生过程,实验结果表明,在较大入射角下,圆偏振激光也可以有效地产生高次谐波辐射.通过预脉冲控制靶表面的预等离子体密度标长,发现高次谐波的产生效率随密度标长的增加而单调下降.进一步通过二维粒子模拟程序,分析了激光的偏振以及预等离子体密度标长对高次谐波产生的影响,很好地解释了实验观测结果.     

Spatial characteristics of Kα radiation from weakly relativistic laser plasmas

The spatial dependence of K _α emission generated from laser-produced hot electrons is investigated experimentally and theoretically. In addition, the conversion efficiency of K _α production as a function of laser intensity is measured and compared with modeling results. We use the terawatt Ti:sapphire laser at MPQ and vary the peak intensity from 10¹⁵ to 10¹⁸ W/cm² with a pulse duration of 200 fs. A solid Cu target is placed at various positions in the laser focus, which allows one to vary the intensity but keep the total energy on the target constant. When the target is near best focus, the FWHM of the K _α emission, measured using a knife-edge, is considerably larger than the FWHM of the laser intensity. In measuring the efficiency of K _α production using the fundamental wavelength of the laser, a clear maximum of K _α emission is observed at a position away from best focus, where the peak intensity is down by more than an order of magnitude from the value at best focus. When the second harmonic of the laser is used, the K _α emission is peaked near best focus. The K _α emission from layer targets is used to obtain an estimate of the temperature of the hot electrons. Modeling of K _α production, using a Monte Carlo electron/photon transport code, shows the relationship between incident electron energy and the emitted K _α emission. Efficient K _α generation from the low-intensity wings of the laser pulse contributes to the large spot size of the K _α emission. The lower electron temperatures that are expected for the second harmonic explain the differences in the location of maximum K _α emission for the two wavelengths. We discuss the use of K _α emission in photoionizing inner-shell electrons with the goal of achieving X-ray lasing at short wavelengths. Received: 6 April 1999 / Revised version: 31 May 1999 / Published online: 11 August 1999     

高次谐波发射中的超拉曼发射

本文研究了单电子分子离子与强激光场相互作用下的高次谐波发射谱。从光谱中观察到除了存在入射激光频率奇数倍的谐波谱线外,还存在其他频率的超拉曼谱线。在理论上阐明了超拉曼谱线不同于高次谐波谱线的物理产生机制。研究发现当体系初态为基态和较高激发态的叠加态时能够较清晰的观察到超拉曼谱线,从而说明激发态电子的布居对超拉曼谱线的产生起着关键作用。因此在实验上,制备一个叠加态使得电子从激发态电离,是观察到超拉曼谱线的重要条件。