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.     

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.     

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.     

Dependence of third-order nonlinear susceptibility on strain induced piezoelectric field in InxGa1-xN/GaN quantum well

The third-order susceptibility of InxGa1-xN/GaN quantum well (QW) has been investigated by taking into account the strain-induced piezoelectric (PZ) field, and the effective-mass SchrSdinger equation is solved numerically. It is shovn that the third-order susceptibility for third harmonic generation (THG)of InxGa1-x,N/GaN QW is related to indium content in QW and the intensity of the PZ field. The characteristics ofX(3)THG(-3ω,(3) ω, ω,ω) as the function of the wavelength of incident beam, well width and indium content, have been analyzed.     

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.     

On the enhancement of the nonlinear frequency transformation in periodic media

It is theoretically shown that an enhancement of the nonlinear frequency transformation in a periodic medium occurs under definite conditions if it is accompanied by light diffraction in this medium. The enhancement of the phase-matched frequency transformation occurs if the harmonic frequency ω approaches the stop band frequency ω_e. In the nondepleted pump approximation the corresponding increase of the harmonic intensity is proportional to ω_e(ω?ω_e)^?1 and is restricted by a quantity proportional to the fourth power of the sample thickness. The formulas for the enhancement of second harmonic generation are presented.     

Generation of an isolated sub-30 attosecond pulse in a two-color laser field and a static electric field

We theoretically investigate high-order harmonic generation(HHG) from a helium ion model in a two-color laser field,which is synthesized by a fundamental pulse and its second harmonic pulse.It is shown that a supercontinuum spectrum can be generated in the two-color field.However,the spectral intensity is very low,limiting the application of the generated attosecond(as) pulse.By adding a static electric field to the synthesized two-color field,not only is the ionization yield of electrons contributing to the harmonic emission remarkably increased,but also the quantum paths of the HHG can be significantly modulated.As a result,the extension and enhancement of the supercontinuum spectrum are achieved,producing an intense isolated 26-as pulse with a bandwidth of about 170.5 eV.In particular,we also analyse the influence of the laser parameters on the ultrabroad supercontinuum spectrum and isolated sub-30-as pulse generation.     

High harmonic generation in H2 + and HD + by two-colour femtosecond laser pulses

We have theoretically investigated the high harmonic generation (HHG) spectra of H₂ ^?+? and HD^?+? using a time-dependent wave packet approach for the nuclear motion with combined two-colour (1ω _L –3ω _L ) pulsed lasers for ω _L corresponding to wavelengths 1064 nm and 800 nm. The 1ω _L and 3ω _L lasers have peak intensities of I ₁ ⁰?=?5.0×10¹³ W/cm² and I ₂ ⁰?=?2.0×10¹⁴ W/cm², respectively. We have taken the pulse duration of T = 50 fs for both the fields, and the molecular initial vibrational level v ₀?=?0. We have argued that for these combinations, the harmonic generation due to transitions in the electronic continuum by tunnelling or multiphoton ionization may be neglected and only the electronic transitions within the two lowest electronic states would be important. Thus, the characteristic features of HHG spectra in the two-colour field are determined, in our model, by the nuclear motions on the two lowest field-coupled electronic states between which interelectronic and intraelectronic (due to the intrinsic dipole moments in case of HD^?+?) radiative transitions can take place. We have studied the role of relative phase (φ) of the two fields on the HHG spectra of the molecular ions. In case of HD^?+?, the effect of nonadiabatic (NA) nonradiative interaction between the two lowest Born-Oppenheimer (BO) electronic states (1sσ _g , 2pσ _u ) has been taken into account. Our calculations give realistic HHG spectra which are reasonably efficient and extended for both H₂ ^?+? and HD^?+? in the mixed two-colour field without involving the electronic continuum. The use of two-colour (1ω _L –3ω _L ) field enables us to generate high harmonics beyond that achievable with a single 1ω _L or 3ω _L field of the corresponding intensity, frequency and pulse time.     

Nonlinear susceptibilities of vapors and solutions of organic dyes

Results of theoretical studies of laser and Kerr nonlinear susceptibilities of vapors and solutions of organic dyes using a series of polycyclic arenes as an example are presented. Nonlinear susceptibilities of the third χ⁽³⁾ (?3ω; ω, ω, ω) and the fifth χ⁽⁵⁾ (?3ω; ω, ω, ω, ω, ?ω) orders of a series of organic dyes responsible for third harmonic generation of Nd:YAG laser radiation are calculated within the context of the free electron model. Results of calculations of their Kerr third-order nonlinear susceptibilities χ⁽³⁾ (?ω; ω, ?ω, ω) and non-linear refractive indices n ₂ are presented. The calculation results are compared with experimental data on third harmonic generation in naphthalene vapors and with χ⁽³⁾ (?ω; ω, ?ω, ω) as well as n ₂ of paraterphenyl and naphthalene solutions.     

Spectral-temporal investigations of the backscattered radiation from laser plasma

Spectral and time-resolved investigations of the back-scattered light from aluminium laser-produced plasmas at frequencies ω_L and 2ω_L are performed. Good correlation between maxima of the scattered light at ω_L and minima at 2ω_L was discovered. This correlation has been predicted by the theory. These experiments show that the spectrum width and intensity of the second harmonic essentially depend on the velocity of the expanding plasma.     

Effects of laser pulsewidth on higher-order harmonic generation in the barrier-suppression-ionization intensity regime

We studied the highest harmonic photon energies of high-order harmonic generation (HHG) for He, Ne, Ar, Kr, Xe, and N₂. This research employed 65-fs and 150-fs Ti:sapphire laser pulses, of which the peak intensities in a vacuum are higher than the barrier-suppression-ionization (BSI) intensities. We fitted two analytical formulae to the experimental results of HHG. One formula, which was obtained by fitting an analytical formula to the results by a quantum mechanical simulation of HHG, expresses the highest interaction intensity by a function of the BSI intensity and the Keldysh γ-parameter. The other formula is derived by introducing the saturation intensity of HHG, which was proposed by Chang et al. [Phys. Rev. Lett. 79, 2967 (1997)]. We discuss the highest interaction intensity for the condition when the peak laser intensities are higher than the BSI intensities. Received: 19 March 1999 / Revised version: 13 August 1999 / Published online: 27 October 1999     

Helicity of harmonic generation and attosecond polarization with bichromatic circularly polarized laser fields

We theoretically investigate the high-order harmonic generation(HHG) of helium atom driven by bichromatic counterrotating circularly polarized laser fields. By changing the intensity ratio of the two driving laser fields, the spectral chirality of the HHG can be controlled. As the intensity ratio increases, the spectral chirality will change from positive-to negativevalue around a large intensity ratio of the two driving fields when the total laser intensity keeps unchanged. However, the sign of the spectral chirality can be changed from positive to negative around a small intensity ratio of the two driving fields when the total laser intensity changes. At this time, we can effectively control the helicity of the harmonic spectrum and the polarization of the resulting attosecond pulses by adjusting the intensity ratio of the two driving laser fields. As the intensity ratio and the total intensity of the driving laser fields increase, the relative intensity of either the left-circularly or right-circularly polarized harmonic can be enhanced. The attosecond pulses can evolve from being elliptical to near linear correspondingly.     

电荷共振增强电离和离解电离在H~+_2谐波辐射中的贡献

理论研究了电荷共振增强电离和离解电离在H~+_2谐波辐射中的贡献.结果表明:在少周期激光场下,谐波辐射只由电荷共振增强电离贡献产生,谐波光谱呈规则的奇次谐波.在多周期激光场下,谐波辐射由电荷共振增强电离和离解电离共同贡献产生,但是电荷共振增强电离在谐波辐射中起主要作用.并且低阶谐波呈现偶次谐波.最后,通过分析含时核运动,电离几率以及谐波辐射时频分析图解释了少周期和多周期激光场驱动H~+_2辐射谐波的过程.     

Influence of circular aperture on high-order harmonic generation

The influence of circular aperture on the intensity of high-order harmonic generation (HHG) with intense femtosecond laser pulse was studied both experimentally and theoretically. The intensity variety of HHG with the diameter of circular aperture was observed in pulsed Ar gas. The result was discussed and interpreted in terms of the theory of Hankel transform. It is found that using the Gaussian beam truncated by an aperture could enhance the conversion efficiency of HHG at certain conditions.     

理论研究激光强度对H2+分子高次谐波产生的影响

本文通过求解非波恩-奥本海默近似条件下的一维含时薛定谔方程来研究脉冲强度对H₂⁺分子高次谐波的影响.由于干涉相消,在啁啾激光场的条件下在谐波谱中出现了干涉最小值.我们用全量子方法计算的时频分布图分析了分子高次谐波产生中的微观机制.此外,数值计算结果显示随着脉冲强度的增加电子的有质动力势随之增加,同时干涉最小值的位置移向谐波的高阶部分.     

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.     

Tunable spectral shift of high-order harmonic generation in atoms using a sinusoidally phase-modulated pulse

High-order harmonic generation (HHG) from an atom illuminated by a sinusoidally phase-modulated pulse is investigated by solving the time-dependent Schrödinger equation. The spectral shift that occurs in atomic HHG can be achieved easily using our laser pulse. It is shown that the photon energy of the generated harmonics is controllable within the range of 1 eV. The shift of the frequency peak position is rooted in the asymmetry of the rising and falling parts of the laser pulse. We also show that by varying the phase parameters in the frequency domain of the laser one can adjust and control the shift in atomic harmonic spectra.     

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.     

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.     

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.