High field physics and extreme nonlinear optics

Despite the fact that high order harmonic generation (HHG) aims at serving as a table-top light source for imaging applications with extremely high spatial resolution, a general lack of accurate conversion efficiency measurements exists in the field. Here, we present such a measurement for a HHG setup with a semi-infinite gas cell. By combining measurements with a calibrated photodiode sensitive in the extreme ultra-violet (XUV) and spatially resolved spectral measurements of HHG spectra, we are able to determine conversion efficiencies of the HHG process as well as brilliance values for individual harmonics. The method is explained in detail and applicable to any target geometry.     

红外激光场中共振结构原子对极紫外光脉冲的压缩效应

通过数值求解一维原子的含时薛定谔方程, 研究了具有共振结构的原子在双色场(红外激光(IR)+极紫外光(XUV)) 驱动下发射高次谐波的特征. 研究结果表明, 具有共振结构的原子所发射的高次谐波与无共振结构原子(简称为一般原子)发射的高次谐波有明显不同, 共振结构的原子除了在某一能量附近(原子的共振能量+电离能)高次谐波的强度有很大提高外, 它还对XUV光的响应较一般原子表现得更为敏感, 即使XUV光的强度较弱, 也能够明显提高XUV光脉冲中心频率附近的谐波强度, 更重要的是通过调节双色场的时间延迟, 能使输入的XUV光的脉宽得到明显的压缩, 通过时间-频率分析给出了发生这种现象的原因. 由此提出了通过滤波-连续反馈的方式可使XUV光的脉冲从200 as压缩至120 as左右.     

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.     

Efficiency pedestal in quasi-phase-matching devices with random duty-cycle errors

It is shown that random duty-cycle errors in quasi-phase-matching (QPM) nonlinear optical devices enhance the efficiency of processes far from the QPM peak. An analytical theory is shown to agree well with numerical solutions of second-harmonic generation (SHG) in disordered QPM gratings. The measured efficiency of 1550?nm band SHG in a periodically poled lithium niobate (PPLN) waveguide away from the QPM peak agrees with observations of domain disorder in a PPLN wafer by Zygo interferometry. If suppression of parasitic nonlinear interactions is important in a specific application of QPM devices, control of random duty-cycle errors is critical.     

Quasi-phasematching

The use of microstructured crystals in quasi-phasematched (QPM) nonlinear interactions has enabled operation of nonlinear devices in regimes inaccessible to conventional birefringently phasematched media. This review addresses basic aspects of the theory of QPM interactions, microstructured ferroelectrics and semiconductors for QPM, devices based on QPM media, and a series of techniques based on engineering of QPM gratings to tailor spatial and spectral response of QPM interactions. Because it is not possible in a brief review to do justice to the large body of results that have been obtained with QPM media over the past twenty years, the emphasis in this review will be on aspects of QPM interactions beyond their use simply as highly nonlinear alternatives to conventional birefringent media. To cite this article: D.S. Hum, M.M. Fejer, C. R. Physique 8 (2007).     

Generation of higher harmonics of laser radiation in plasma formed by pulses with a 1-kHz repetition rate

Studies of higher-order nonlinearities in plasma plumes by the method of higher-harmonic generation (HHG) upon laser ablation of different materials by pulses with a repetition rate of 1 kHz are reviewed. It is shown that an increase in the pulse repetition rate compared to the previous works on HHG in plasma using lasers with a pulse repetition rate of 10 KHz considerably increases the average power of converted radiation in the far-ultraviolet (FUV) region. The review considers the results of works on the interference of quantum trajectories of accelerated electrons, two-color pumping, HHG in graphite plasma, HHG in gases compared to HHG in plasma plumes, resonant enhancement of harmonics, and stabilization of the output parameters of radiation converted in plasma. It is shown that the new methods of optimization of the HHG process considerably increase the potential of the use of coherent FUV radiation owing to the improvement of some characteristics of harmonics in plasma generated by pulses with a high repetition rate.     

High-order harmonic generation enhanced by XUV light

The combination of high-order harmonic generation (HHG) with resonant XUV excitation of a core electron into the transient valence vacancy that is created in the course of the HHG process is investigated theoretically. In this setup, the first electron performs a HHG three-step process, whereas the second electron Rabi flops between the core and the valence vacancy. The modified HHG spectrum due to recombination with the valence and the core is determined and analyzed for krypton on the 3d→4p resonance in the ion. We assume an 800?nm laser with an intensity of about 10(14)?W/cm2 and XUV radiation from the Free Electron Laser in Hamburg (FLASH) with an intensity in the range 10(13)-10(16)W cm2. Our prediction opens perspectives for nonlinear XUV physics, attosecond x rays, and HHG-based spectroscopy involving core orbitals.     

Optical high harmonic generation in C60

High harmonic generation (HHG) requires a strong laser field, but in C60 a relatively weak laser field is sufficient. Numerical results presented here show that, while its low order harmonics result from the laser field, its high order ones are mainly from the multiple excitations. Since high order harmonics directly correlate with electronic transitions, the HHG spectrum accurately measures transition energies. Therefore, C60 is not only a promising material for HHG, but may also present an opportunity to develop HHG into an electronic structure probing tool.     

Plasma effect on the phase matching of high harmonic generation

By optimizing the phase matching condition of high harmonic generation(HHG) from a supersonic neon gas jet,the enhanced HHG in the region of 60-70 eV has been selected.Three-dimensional numerical calculation shows that plasma plays a significant role in the phase matching process of HHG in a supersonic gas jet with short medium length.Due to plasma formation,the harmonic emission decays as the laser intensity reaches over 3.5 × 10 14 W/cm 2.The plasma induces the broadening and blue shift of the HHG spectra,which provides a method for fine-tuning the harmonic wavelength.     

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.     

Angle-tuned second-harmonic generation in periodically-poled lithium niobate

We investigated angular tuning of quasi-phase-matching (QPM) second-harmonic generation (SHG), in order to extend the tunable range of QPM and to combine the advantages of QPM and birefringence phase-matching. The direction of the input fundamental wave vector was detuned from the QPM grating vector along the crystallographic Z-axis of a periodically-poled lithium niobate (PPLN) crystal in the XY- and XZ-planes. A?larger tuning range of SHG was obtained for the detuning in the XZ-plane, continuously shifting the QPM peak of the fundamental wavelength from 1524 to 1595?nm by changing the detuning angle from 0° (parallel to X-axis as conventional QPM) to 23.2°.     

二维LiNbO3非线性光子晶体

制备了周期为13.64 μm方形格子二维周期性极化的LiNbO₃，利用二阶准相位匹 配实现了波长为1.064μm二倍频，二次谐波的内部转换效率高达42％. 测量了二次谐波输出功率随晶体温度及入射光入射方向的变化，实验值与模拟计算一致. 制备二阶准相位匹配掩模板，解决了在制备一阶准相位匹配掩模板中遇到周期尺寸太小、数据量大的难题，同时还降低了因周期太小造成的极化难度. 关键词： 二维 准相位匹配 二次谐波     

Carrier envelope phase effect on the spatial distribution of high-order harmonic generation in asymmetric molecule

The spatial distribution in high-order harmonic generation(HHG) from the asymmetric diatomic molecule He H~(2+) is investigated by numerically solving the non-Born–Oppenheimer time-dependent Schr?dinger equation(TDSE). The spatial distribution of the HHG spectra shows that there is little contribution in HHG around the geometric center of two nuclei(z = 1.17 a.u.) and the equilibrium internuclear position of the H nucleus(z = 3.11 a.u.). We demonstrate the carrier envelope phase(CEP) effect on the spatial distribution of HHG in a few-cycle laser pulse. The HHG process is investigated by the time evolution of the electronic density distribution. The time–frequency analysis of HHG from two nuclei in HeH~(2+) is presented to further explain the underlying physical mechanism.     

脉冲形状对氢原子高次谐波的影响

在含时密度泛函理论框架下,采用经典和量子相结合的模型,模拟了氢原子在超强飞秒激光脉冲作用下的高次谐波产生现象,并研究了激光脉冲形状对氢原子高次谐波的影响.结果表明,氢原子的高次谐波谱具有典型的原子谐波谱的特征;具有“下降－平台－截止”的结构和偶次谐波被禁闭仅出现奇次谐波的选择性特征;不同的脉冲形状会导致高次谐波的截止频率和谱线强度的变化.     

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.     

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     

Retiming of picosecond pulses by a cascaded second-order nonlinear process in quasi-phase-matched LiNbO3 waveguides

A new technique for reducing timing jitter by using a cascaded second-order nonlinear process in quasi-phase-matched (QPM) LiNbO3 waveguides is proposed. It was found that the timing jitter of a signal at QPM wavelength is not transferred to the converted pulses during cascading in a 30-mm-long LiNbO3 QPM waveguide. Timing-jitter transfer characteristics in QPM LiNbO3 waveguides are evaluated by calculation of pulse evolution, and retiming of 1.5-ps pulses in 10- and 30-mm-long waveguides is demonstrated experimentally.     

Probing subcycle spectral structures and dynamics of high-order harmonic generation in crystals

Subcycle spectral structures and dynamics of high-order harmonic generation (HHG) processes of atoms and molecules driven by intense laser fields on the attosecond time scale have been originally studied theoretically and experimentally. However, the time scale of HHG dynamics in crystals is in the order of sub-femtosecond, and the carrier dynamics of HHG in crystals driven by subcycle laser pulses are largely unexplored. Here we perform a theoretical study of subcycle structures, spectra, and dynamics of HHG of crystals in mid-infrared laser fields subject to excitation by a subcycle laser pulse with a time delay. The HHG spectra as a function of time delay between two laser fields are calculated by using a single-band model for the intra-band carrier dynamics in crystal momentum space and by solving the time-dependent Schrödinger equation in velocity gauge for the treatment of multi-band crystal systems. The results exhibit a complex time-delay-dependent oscillatory pattern, and the enhancement and suppression of the HHG related to subcycle pulse are observed at the given time delay in either single-band or multi-band crystal systems. To understand oscillation structures with respect to the dependence for the subcycle laser fields, the time-frequency characteristics of the HHG as well as the probability density distribution of the radiation are analyzed in detail.     

脉冲激光偏振方向对氧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,模拟了氧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氧分子高次谐波的影响.结果表明氧分子的高次谐波谱具有典型原子谐波谱的特征;当θ=45°(激光偏振方向与分子轴向夹角)时,谐波谱强度最大.这与文献报道的实验结果基本一致.     

任意偏振激光作用下二维模型H原子的谐波发射

采用二维渐近边界条件和辛算法数值求解了任意偏振激光和H原子相互作用的二维含时Schrödinger方程的无穷空间初值问题. 计算了二维H原子在不同偏振激光作用下的谐波发射,得到各种椭圆率下谐波谱的特点与已有文献结果一致.通过电子的基态布居概率和某一时刻的概率密度分布以及电子的平均位移,对不同椭圆率下谐波谱的特点进行了分析. 结果表明,将渐近边界条件和辛算法推广到二维是合理和有效的. 关键词： 二维渐近边界条件 辛算法 任意偏振激光 高次谐波