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     

利用三色组合脉冲激光获得孤立阿秒脉冲发射

孤立阿秒脉冲因可以跟踪和控制原子及分子内电子的运动过程而备受关注.本文从理论上开展了氦原子在3束飞秒脉冲激光组合场辐照下产生的高次谐波和阿秒脉冲辐射的研究.组合激光场由16 fs/1600 nm,15 fs/1100 nm和5.3 fs/800 nm的钛宝石脉冲构成.与前两束脉冲合成的双色场产生谐波谱相比,附加钛宝石脉冲的三色场产生的高次谐波发射谱呈现出高转换效率及宽带超连续特性,超连续谱范围覆盖从230—690次谐波,傅里叶变换后实现了128 as高强度孤立短脉冲的产生.该结果归因于合成的三色场呈现出高功率及少周期的中红外飞秒脉冲激光特性,可以有效控制原子电离以及复合发生在中红外飞秒脉冲的一个有效光学周期内.     

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.     

线偏振激光场中分子高次谐波椭偏率的调控

高次谐波椭偏率的调控为人们研究磁性材料和手性介质中的超快动力学过程提供了有效途径.本文理论研究了线偏振激光脉冲驱动下,H₂~+和H₃²⁺分子高次谐波的偏振特性及阿秒脉冲产生.结果表明当取向角为0~o时,H₂~+分子谐波的椭偏率几乎为0,而H₃²⁺分子谐波具有较大椭偏率,这是由于分子轨道对称性决定的.通过改变取向角的大小,可以调控高次谐波强度以及谐波椭偏率大小,为产生椭偏XUV脉冲提供了手段.同时,发现椭偏率较大的谐波阶次对应的谐波强度较小,分析表明分子的双中心干涉效应对椭偏率有很大的影响.对于H₂~+和H₃²⁺分子,分别合成了椭偏率为0.75和0.55的椭圆偏振阿秒脉冲.这种大椭偏XUV脉冲的产生为高次谐波在材料与生物科学领域提供了重要应用.     

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     

Theoretical exploration of asymmetric molecular harmonic emission and attosecond pulse generation in the presence of spatially inhomogeneous plasmon-enhanced field

Asymmetric molecular harmonic generation from HeH²⁺ ion in the presence of the spatially inhomogeneous plasmon-enhanced field has been theoretically investigated by solving the two-dimensional non-Born–Oppenheimer time-dependent Schrödinger equation (both the electron and nuclear motions are considered only along the laser polarisation axis). It shows that (1) for the normal homogeneous field, the harmonic cut-off from the asymmetric molecule is beyond the classical harmonic cut-off energy from the atom (I_p + 3.17 U_p). Further analyses show that the multi-channels ionisation–recombination process is responsible for the harmonic extension. (2) For the spatially inhomogeneous plasmon-enhanced field, the harmonic cut-off can be further enhanced, and an optimal 3.0 dB enhanced field with a 482 eV supercontinuum has been obtained. Quantum time-frequency harmonic analyses have been shown to explain the harmonic characteristics and the harmonic extension process. (3) Initial vibrational state and isotopic effects show that intense harmonics can be generated from higher initial vibrational state and the heavier molecule. Finally, by properly superposing the harmonics, a series of sub-30 as attosecond pulses can be obtained.     

High-order harmonic generation and multi-photon ionization of Na2 in laser fields

In this paper high-order harmonic generation （HHG） spectra and the ionization probabilities of various charge states of small cluster Na2 in the multiphoton regimes are calculated by using time-dependent local density approximation （TDLDA） for one-colour （1064 nm） and two-colour （1064 nm and 532 nm） ultrashort （25 fs） laser pulses. HHG spectra of Na2 have not the large extent of plateaus due to pronounced collective effects of electron dynamics. In addition, the two-colour laser field can result in the breaking of the symmetry and generation of the even order harmonic such as the second order harmonic. The results of ionization probabilities show that a two-colour laser field can increase the ionization probability of higher charge state.     

量子路径控制生成宽频软X射线连续辐射谱

数值研究了双色激光脉冲与一维氩原子相互作用的谐波发射功率谱.双色激光脉冲由800 nm和1600 nm的两束激光组成,脉冲持续时间为9.7 fs.计算结果表明,相对相位为π时,谐波截止频率从单色场情形的58 eV大幅度地展宽到316 eV,获得频宽为93 eV的软X射线连续辐射谱.此外,还采用短程的普薛耳－特勒势和长程的软化库仑势进行比对,数值结果表明该连续辐射谱的存在具有普适性.通过半经典的“三步”模型和时频分析小波变换方法对该连续辐射谱进行分析,发现其主要由单一的“短”量子路径生成,直接叠加频率从22 关键词： 红外双色激光脉冲 连续辐射谱 阿秒脉冲     

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.     

正交偏振双色激光场作用下高次谐波的椭偏特性研究

通过数值求解二维含时薛定谔方程,理论研究了正交偏振双色激光场作用下H2+分子高次谐波发射和孤立阿秒脉冲的产生. 数值结果显示,改变激光场的强度比,可以调控高次谐波强度以及谐波椭偏率. 结果表明随着场强比的增加,y方向的谐波强度不断提高. 当场强比为1:2.5时,x方向和y方向分别仅有奇次谐波和偶次谐波产生,并且偶次谐波的强度比奇次谐波强度高2-3个数量级. 此时,奇次谐波的椭偏率最大可以达到0.3,偶次谐波的椭偏率接近于0. 此外,通过改变分子的准直角可以控制谐波的椭偏率,基于这一现象,利用椭圆偏振高次谐波的平台区合成了椭偏率为0.05的椭圆偏振阿秒脉冲链.     

A femtosecond laser study of the endohedral fullerenes Li@C60 and La@C82

The endohedral fullerenes La@C₈₂ and Li@C₆₀ have been studied in the gas phase with femtosecond laser excitation. The two molecules show qualitatively the same behaviour with respect to ion yield vs. pulse energy, but markedly different fragmentation patterns, with La@C₈₂ fragmenting via the shrink-wrap mechanism and Li@C₆₀ predominantly losing the metal atom in the first fragmentation step. The ion yields and electron energy distributions of La@C₈₂ agree well with a recently developed model for fs laser ionisation of C₆₀.     

Single-pass high-harmonic generation at 20.8 MHz repetition rate

We report on single-pass high-harmonic generation (HHG) with amplified driving laser pulses at a repetition rate of 20.8?MHz. An Yb:YAG Innoslab amplifier system provides 35?fs pulses with 20?W average power at 1030?nm after external pulse compression. Following tight focusing into a xenon gas jet, we observe the generation of high-harmonic radiation of up to the seventeenth order. Our results show that state-of-the-art amplifier systems have become a promising alternative to cavity-assisted HHG for applications that require high repetition rates, such as frequency comb spectroscopy in the extreme UV.     

Quantum interference of multi-orbital effects in high-harmonic spectra from aligned carbon dioxide and nitrous oxide

We investigate experimentally multi-orbital effects in high-order harmonic generation(HHG) from aligned CO_2 and N_2O molecules by intense femtosecond laser fields with linear and elliptical polarizations.For either of the aligned molecules, a minimum in the harmonic spectrum is observed, the position of which shifts to lower-order harmonics when decreasing the intensity or increasing the ellipticity of the driving laser.This indicates that the minimum originates from the dynamic interference of different channels, of which the tunneling ionization and recombination are contributed via different molecular orbitals.The results show that both the highest occupied molecular orbital(HOMO) and low-lying HOMO-2 in CO_2(or HOMO-1 in N_2O) contribute to the molecular HHG in both linearly and elliptically polarized strong laser fields.Our study would pave a way for understanding multi-electron dynamics from polyatomic molecules irradiated by strong laser fields.     

5fs驱动激光脉冲的高次谐波选择性优化

研究了在紧聚焦实验条件下, 采用5 fs激光脉冲与氩气相互作用产生的高次谐波特性. 通过优化系统色散、气体靶气压与位置等参数, 观察到在60–73 eV波段范围内高次谐波光谱接近一个量级的增强. 进一步通过对单原子模型和传播方程的数值求解及模拟相位匹配实验参数下高次谐波的产生过程, 发现相位匹配在所观察到的实验现象中起着关键作用, 得到了理论上与实验规律一致的结果. 关键词： 极紫外激光 高次谐波 超快光谱     

Harmonic Enhancement Mechanism of a Superposition State Atom Irradiated by Short Pulses

We investigate the high-order harmonic generation （HHG） of a model atom whose initial state is prepared in a superposition of its ground state and an excited state irradiated by different duration laser pulses. Compared to the HHG generated from an atom whose initial state is in its ground state, its conversion efficiency obtains some enhancement. The enhancement originates from the higher ionization rate （rather than the ionization yield） of the atom with superposition initial state.     

Carrier-envelope phase measurement using plasmonic-field-enhanced high-order harmonic generation of H atom in few-cycle laser pulses

We investigate the plasmonic-field-enhanced high-order harmonic generation (HHG) of H atom driven by few-cycle laser pulses, by solving the time-dependent Schrödinger equation (TDSE). Compared with the homogeneous field, HHG spectra generated by inhomogeneous field exhibit two-plateau structure. We analyze the origin of the two plateaus by using the semiclassical trajectory method. Our results from both classical and TDSE simulations show that the cutoffs of the two plateaus are dramatically affected by the carrier-envelope phase (CEP) of laser pulse in the inhomogeneous field, even for a little longer pulse. Thus, we can determine the CEP of driving laser based on the cutoff position of HHG generated in the inhomogeneous field.     

采用较长脉宽双色场获得孤立阿秒脉冲（第15届全国原子与分子物理会议）

通过数值求解一维含时薛定谔方程,本文研究了具有较长脉宽双色激光脉冲与氢原子模型相互作用产生的谐波辐射谱。研究发现,当采用12个光学周期的特定组合脉冲时,孤立阿秒脉冲可以实现。这里特定组合脉冲由两束类似频率脉冲( )构成,附加脉冲的作用恰是调整基频光电场的形状。不同于入射基频光,整形后的基频光在时间始末端电场振幅被抑制,只有中间部分电场对谐波谱有贡献,它的作用等同于单一6飞秒超短脉冲的效果。从而扩展获得孤立阿秒脉冲所需脉宽从6飞秒到12飞秒。     

采用较长脉宽双色场获得孤立阿秒脉冲

通过数值求解一维含时薛定谔方程,本文研究了具有较长脉宽双色激光脉冲与氢原子模型相互作用产生的谐波辐射谱.研究发现,当采用12个光学周期的特定组合脉冲时,孤立阿秒脉冲可以实现.这里特定组合脉冲由两束类似频率脉冲(ω,ω+δω)构成,附加脉冲的作用恰是调整基频光电场的形状.不同于入射基频光,整形后的基频光在时间始末端电场振幅被抑制,只有中间部分电场对谐波谱有贡献,它的作用等同于单一6飞秒超短脉冲的效果.从而扩展获得孤立阿秒脉冲所需脉宽从6飞秒到12飞秒.     

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.     

Effect of the relative phase between two-colour pump pulses on structure of harmonic spectra

We numerically calculate the high-order harmonic generation (HHG) power spectra from a one-dimensional model atom irradiated by linearly polarised 12 fs two-colour laser pulses composed of a fundamental pulse from Ti:sapphire laser and its second harmonic. It is found that a distinct double plateau structure appears when the relative phase of the two pulses is set as π/8, 2π/8 or 3π/8, and the double plateau structure disappears when the relative phase is set as 4π/8, 5π/8, 6π/8 or 7π/8. The relative-phase-dependent plateau structure is explained by the temporal profile of the synthesised electric fields as well as the semi-classical “three-step” model. Moreover, our numerical result shows that cut-off frequencies of the two-colour pulse HHG spectra can be exactly predicted by use of the semi-classical “three-step” model.