Probing orbital structure of polyatomic molecules by high-order harmonic generation

The effects of electronic structure and symmetry are observed in laser driven high-order harmonic generation for laser aligned conjugated polyatomic molecular systems. The dependence of the harmonic yield on the angle between the molecular axis and the polarization of the driving laser field is seen to contain the fingerprint of the highest occupied molecular orbitals in acetylene and allene, a good quantitative agreement with calculations employing the strong field approximation was found. These measurements support the extension of the recently proposed molecular orbital imaging techniques beyond simple diatomic molecules to larger molecular systems.     

Atomic scale temporal structure inherent to high-order harmonic generation

Using intense lasers, several laboratories have generated high-order harmonic spectra which are flat over 20 eV. If the harmonics are appropriately phased, this bandwidth corresponds to temporal pulses on the order of 5 × 10^-17 s, and thereby motivates a search for a new regime of short-pulse generation.     

Multiple collisions in crystal high-order harmonic generation

We theoretically investigate high-order harmonic generation (HHG) in crystals induced by linearly polarized laser fields. We obtain the HHG spectra by solving the semiconductor Bloch equations and analyze the radiation process by different models. Here we propose a multiple collision model, in which the electrons and holes are produced at different times and places. It is found that the multiple collision trajectories can help us comprehensively and better explain the results of the quantum calculation. Moreover, we find that the harmonic suppression occurs due to the overlap of multiple collision trajectories.     

Double optical gating of high-order harmonic generation with carrier-envelope phase stabilized lasers

We demonstrated a novel optical switch to control the high-order harmonic generation process so that single attosecond pulses can be generated with multiple-cycle pulses. The technique combines two powerful optical gating methods: polarization gating and two-color gating. An extreme ultraviolet supercontinuum supporting 130 as was generated with neon gas using 9 fs laser pulses. We discovered a unique dependence of the harmonic spectra on the carrier-envelope phase of the laser fields, which repeats every 2 pi radians.     

Bohmian mechanics to high-order harmonic generation

This paper introduces Bohmian mechanics (BM) into the intense laser-atom physics to study high-order harmonic generation. In BM, the trajectories of atomic electron in an intense laser field can be obtained with the Bohm--Newton equation. The power spectrum with the trajectory of an atomic electron is calculated, which is found to be irregular. Next, the power spectrum associated with an atom ensemble from BM is considered, where the power spectrum becomes regular and consistent with that from quantum mechanics. Finally, the reason of the generation of the irregular spectrum is discussed.     

高次谐波辐射发射特性研究

报告由不同脉冲宽度(半高宽,FWHM)和不同载波-包络相位(CEP,Φ)的激光产生的高次谐波辐射能量输出时间特性即发射特性的研究结果. 计算表明,由宽度为几个周期的激光产生的高次谐波辐射的截止能量明显低于由无限长脉冲宽度激光产生的截止能量ω_max=3.17U_p+I_p(其中ω_max为光子角频率,U_p和I_p分别为激光有质动力势和原子的电离能). 例如,由两周期(FWHM),Φ＝15°的激光产生的高次谐波辐射的截止能量为ω_max=2.90U_p+I_p,此时发射特性单脉冲(即分布单脉冲)具有最大的能量带宽0.86U_p. 脉冲中心位置的载波相位和时间宽度分别为0.94rad(弧度)和1.29rad. 而该激光脉冲在Φ＝-75°时能产生截止能量为ω_max=2.70U_p+I_p,最大能量带宽为0.70U_p的双分布脉冲,其中心位置分别为-0.58rad和2.43rad,宽度分别为1.22rad和1.33rad. 随着激光脉冲宽度的增加,分布单脉冲的能量带宽比时间宽度下降得更快. 对于一定宽度的激光脉冲,所产生的分布单脉冲的能量带宽和时间宽度的CEP依赖性显示出180°的周期结构. 利用这个有趣的特点,在实验上可以通过调节CEP来选择分布脉冲的能量参数,也可用来定位和控制阿秒脉冲的时间参数. 理论分析指出,只要选择合适的阿秒X射线能量带宽,CEP不稳定性对于光电子谱和测量结果的影响将大为降低,甚至在最大程度上消除这种影响. 这些研究结果不仅有助于在物理上深入了解高次谐波辐射的动力学过程,而且对于进一步在实验上优化和选择阿秒单脉冲和双脉冲具有重要的参考和指导意义. 关键词： 高次谐波产生 鞍点方法 谐波发射特性 分布脉冲     

Quantum path interferences in high-order harmonic generation

We have investigated the intensity dependence of high-order harmonic generation in argon when the two shortest quantum paths contribute to the harmonic emission. For the first time to our knowledge, experimental conditions were found to clearly observe interference between these two quantum paths that are in excellent agreement with theoretical predictions. This result is a first step towards the direct experimental characterization of the full single-atom dipole moment and demonstrates an unprecedented accuracy of quantum path control on an attosecond time scale.     

Dramatic enhancement of high-order harmonic generation

We present a dramatic enhancement [Phys. Rev. Lett. 91, 043002 (2003)] of high-order harmonic generation by simultaneous irradiation of booster harmonics. A key feature of our experiment is the use of mixed gases (Xe and He) with different ionization energies. The harmonics from Xe atoms act as a booster to increase the harmonic yield from He by a factor of 4 x 10(3). The dominance of the dramatic enhancement effect is supported by simulation with the time-dependent Schr?dinger equation as well as the observed spatial characteristic of the generated harmonics and dependence on medium conditions.     

Modelling harmonic generation measurements in solids

Harmonic generation measurements typically make use of the plane wave result when extracting values for the nonlinearity parameter, β, from experimental measurements. This approach, however, ignores the effects of diffraction, attenuation, and receiver integration which are common features in a typical experiment. Our aim is to determine the importance of these effects when making measurements of β over different sample dimensions, or using different input frequencies. We describe a three-dimensional numerical model designed to accurately predict the results of a typical experiment, based on a quasi-linear assumption. An experiment is designed to measure the axial variation of the fundamental and second harmonic amplitude components in an ultrasonic beam, and the results are compared with those predicted by the model. The absolute β values are then extracted from the experimental data using both the simulation and the standard plane wave result. A difference is observed between the values returned by the two methods, which varies with axial range and input frequency.     

Second harmonic generation by periodic laminar structure of nonlinear optical crystal

The phase-matched second harmonic generation by periodic structures composed of laminae of nonlinear optical crystals has been studied experimentally. It is shown that the intensity of the second harmonic is approximately proportional to the square of the number of laminae under phase-matched condition, which is satisfied over a broad frequency range by the variation of the angle of incidence when a laminar structure with a period much larger than the coherence length is used.     

Spectrally resolved maker fringes in high-order harmonic generation

We investigate macroscopic interference effects in high-order harmonic generation using a Ti:sapphire laser operating at a 100 kHz repetition rate. The structure and behavior of spectral and spatial interference fringes are explained and analytically described by transient phase matching of the long electron trajectory contribution. Time-frequency mapping due to the temporal chirp of the harmonic emission allows us to observe Maker fringes directly in the spectral domain.     

Multi-photon resonance enhanced super high-order harmonic generation

This paper proposes highly charged ions pumped by intense laser to produce very high order harmonics.Numerical simulations and full quantum theory of Ne 9+ ions driven by laser pulses at 1064 nm in the power range of 10 9 W/cm 2 ～ 10 15 W/cm 2 show that the emission spectrum corresponds to the electronic transitions from the excited states to the ground state,which is very different from the spectrum of general high-order harmonic generation.In such situation,harmonic order as high as 1000 can be obtained without producing lower order harmonics and the energy conversion efficiency is close to general high order harmonic generation of hydrogen atom in the same laser field.     

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.     

Controlling paths of high-order harmonic generation by orthogonal two-color fields

Controlling paths of high-order harmonic generation from H^2+ is theoretically investigated by numerically solving the time-dependent Schrodinger equation based on the Born-Oppenheimer approximation in orthogonal two-color fields.Our simulations show that the change of harmonic emission paths is dependent on time-dependent distribution of electrons.Compared with one-dimensional linearly polarized long wavelength laser,multiple returns are suppressed and short paths are dominant in the process of harmonic emission by two-dimensional orthogonal ω/2ω laser fields.Furthermore,not only are multiple returns weaken,but also the harmonic emission varies from twice to once in an optical cycle by orthogonalω/1.5ωlaser fields.Combining the time-frequency distributions and the time-dependent electron wave packets probability density,the mechanism of controlling paths is further explained.As a result,a 68-as isolated attosecond pulse is obtained by superposing a proper range of the harmonics.     

高次谐波辐射光子的能量-激光相位关系研究

原子在强激光电场中高次谐波辐射的理论与实验研究是当今科学前沿之一.利用量子力学理论和鞍点方法,细致地研究了高次谐波辐射光子的能量与激光相位的关系.对于时间宽度无限长激光,在一个激光周期内特定相位处产生的高阶辐射(X射线)有特定的能量.能量分布在7180°处成峰,有高斯形函数的对称形状.给出了这种分布的参数化公式.对于不同宽度的飞秒激光,能量分布的成峰位置、最大值和带宽等参数会发生变化.计算表明,三个振荡周期(半高宽)的飞秒激光,当载波-包络相位为175°和105°时,可以分别得到纯净的阿秒单脉冲和双脉 关键词： 超短脉冲激光 高次谐波产生 鞍点方法 能量相位关系     

Direct observation of laser filamentation in high-order harmonic generation

We investigate the spatial evolution of a laser pulse used to generate high-order harmonics (orders ranging from 45 to 91) in a semi-infinite helium-filled gas cell. The 5 mJ, 30 fs laser pulses experience elongated focusing with two distinct waists when focused with f/125 optics in 80 Torr of helium. Extended phase matching for the generation of harmonics occurs in the region between the double foci of the laser, where the laser beam changes from diverging to converging.     

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     

拉伸分子高次谐波产生的阿秒控制

通过数值求解一维含时薛定谔方程,本文研究了高频阿秒脉冲对拉伸双原子分子模型与低频飞秒激光脉冲相互作用产生高次谐波谱的影响.研究表明,若阿秒脉冲在低频脉冲的第二个光学周期截止处注入时,只第二个平台截止位置IP 5.6UP(IP为电离势,UP为有质动力能)附近谐波的效率得到显著提高;若阿秒脉冲的包络峰值处于低频脉冲第三个光学周期T/4(为飞秒激光脉冲的光学周期)附近时,则谐波谱出现了明显的整体抬高现象.对此,本文根据拉伸分子谐波谱的四种产生机制及阿秒脉冲在飞秒激光不同相位注入时的电子电离曲线,对这些谐波谱的结构给出了合理解释.