HeH2+分子多通道谐波发射的理论研究

利用非波恩奥本海默近似模型,理论研究了强激光场下HeH2+分子发射高次谐波的特点。计算结果表明,HeH2+分子的谐波截止能量要大于经典预言值。理论分析表明,延伸的谐波截止能量是由于激发态激光诱导电子跃迁所产生的多通道电子电离-回碰过程所导致的。随后利用双色空间非均匀激光场机制,谐波截止能量进一步延伸,形成了1个由单一量子路径贡献而成的482eV的超长平台区。该辐射能量相当于单色激光场场强被增强了3倍的结果。并且高振动激发态会产生强度更高的谐波光谱。最后,通过适当的叠加谐波平台上的谐波, 可获得一系列脉宽在30as的超短X射线光源。     

Nonadiabatic effects in the molecular high-order harmonic generation from two-center molecular ions

The nonadiabatic effects in the molecular high-order harmonic generation (MHHG) from H₂⁺ and its isotope have been theoretically investigated beyond the Born-Oppenheimer approximations. It is found that (i) due to the asymmetric contributions of the harmonic emission on the rising and the falling parts of the laser field, the frequency red-shifts in the MHHG can be found. As the initial vibrational state or the pulse intensity increases, the red-shifts of the harmonics are decreased and even the blue-shifts of the harmonics can be found in the higher pulse intensity with the higher vibrational state. With the increase of the pulse duration, the frequency red-shifts and the blue-shifts in the MHHG are decreased and enhanced, respectively. The shifts of the harmonics from the heavy nuclei are decreased compared with those from the light nuclei. (ii) Due to the coupling of the electron-nuclear dynamics, the non-odd harmonics can be produced at the larger internuclear distance. With the increase of the initial vibrational state or the pulse duration, the generations of the non-odd harmonics can be enhanced. As the pulse intensity increases, the intensities of the non-odd harmonics are first increased and then decreased at the much larger pulse intensity. Due to the slower nuclear motion, the generations of the non-odd harmonics are decreased as the nuclear mass increases. (iii) With the increase of the alignment angle of the molecule ions, the nonadiabatic effects in MHHG (including the shifts of the harmonics and the generations of the non-odd harmonics) are decreased.     

空间非均匀啁啾双色场驱动下氦离子的高次谐波以及孤立阿秒脉冲的产生

本文理论上研究了初态为基态与第一激发态等权叠加的一维氦离子在空间非均匀啁啾双色场驱动下氦离子的高次谐波发射及孤立阿秒脉冲的产生. 研究表明, 一维氦离子在空间非均匀啁啾双色场驱动下发射的高次谐波相对于均匀场情况截止位置得到明显扩展, 得到了光滑的超连续谱,并应用半经典三步模型解释了高次谐波发射的物理机理. 通过小波变换的方法对连续谱进行了时频分析, 并且与电子的经典运动轨迹进行了对比分析, 结果显示在空间非均匀场中长量子轨道消失, 短量子轨道加强. 讨论了空间非均匀啁啾双色场中时间延迟对谐波和孤立阿秒脉冲产生的影响, 发现适当调整时间延迟值可以得到较大延展的光滑的超连续谐波谱, 本方案中时间延迟为t₀=1.6πup/ω₁时得到了最大延展, 通过对谐波中600次到680次(80次)谐波合成得到32 as的孤立脉冲.     

静电场对高次谐波时频特性的影响

通过数值求解含时薛定谔方程，发现在静电场的作用下，对原子高次谐波谱截止区附近的谐波进行叠加可以得到脉冲间隔为一个光周期的阿秒脉冲链. 利用这种性质，用12fs波长为800nm的激光附加强度为激光强度0.25%的静电场脉冲驱动He原子可以得到脉宽为220as的单个脉冲. 当静电场与激光场幅度之比达到0.39时，原子谐波谱的截止区可以被拓宽到I_p+9.1U_p，同时，次数高于I_p+0.7U_p的谐波的相位几乎是锁定的，因此可以得到谱宽大于40eV且相位锁定的谐波. 对这部分谐波进行叠加就可以得到脉宽小于100as的阿秒脉冲链.     

Half-Integer Harmonics Generation in Laser-Produced Plasma

Half integer (3/2ω₀, 1/2ω₀) harmonics generation under oblique incidence of the pump-wave on the spatially inhomogeneous plasma is theoretically investigated. Harmonics generation is connected with the two-plasmon convective instability excitation near the quarter-critical density. Harmonics spectra and intensities depend essentially on the pump wave polarization. In particular, significant harmonics spectra broadening arises under the p-polarized pump wave.     

利用低频场控制轨道直接产生低于50阿秒的单个脉冲

提出一种直接得到脉宽小于50as的单个脉冲的新方法.利用波长为800nm脉宽为5fs的超短脉冲叠加上波长为10μm,强度为超短脉冲强度的10％且脉宽足够长的低频场脉冲驱动氦原子,谐波谱可以拓展到I_p+8.2U_p,同时,高于4.2U_p的谐波几乎是连续的.如果继续调节超短脉冲的载波包络相位,超连续谱可以继续拓宽,从而可以得到低于50as的单个脉冲. 关键词： 阿秒脉冲 超连续谱     

Chirp control on molecular harmonic generation and distribution in H2+

Chirp control on the molecular harmonic emission and distribution in H₂⁺ has been theoretically investigated. The results show that (i) with the introduction of the up-chirped pulse, the intensities of the higher harmonics are decreased; while with the introduction of the down-chirped pulse, the intensities of the higher harmonics can be enhanced. When E(t) < 0.0, the harmonic emission events (HEEs) from the positive-H are higher than those from the negative-H; while when E(t) > 0.0, the HEEs from the negative-H are higher than those from the positive-H. As a result, when the higher harmonics are produced from E(t) < 0.0 or E(t) > 0.0, the positive-H or the negative-H plays the main role in the harmonic spectra. (ii) The distribution of the higher harmonics from the two-H nuclei can be controlled with the introduction of the chirps and the carrier-envelope-phases of the laser field. (iii) Some minima on the harmonic spectra can be obtained, which is attributed to the coupling of the two-center interference and the electron-nuclear dynamics. (iv) By properly superposing the harmonics from the down-chirped pulse, an isolated attosecond pulse (IAP) with the duration of 45 as can be obtained, which is nearly 1 order of magnitude enhancement in pulse intensity compared with the chirp- free case.     

原子在双色组合场中产生高次谐波的转换效率与激光波长的关系

利用分裂算符法求解速度规范下的含时薛定谔方程,研究了一维氦原子处于单色红外场、红外场与紫外场形成的双色组合场中产生的高次谐波谱,分析了在截止位置附近高次谐波的转换效率与激光波长(800—2000 nm)的关系,发现在双色组合场驱动下截止位置附近高次谐波的转换效率随波长的变化为η(λ)∝λ^－x,其中〈x〉的数值取决于激光场的强度,但是只要选取合适场强的组合场就能提高截止位置附近高次谐波的转换效率. 关键词： 双色组合场 分裂算符 高次谐波 转换效率     

少周期激光脉冲附加太赫兹场对高次谐波发射的影响

本文通过数值求解非伯恩奥本海默近似下电子一维核一维的含时薛定谔方程,研究了少周期线偏振激光与氢分子离子相互作用下,太赫兹场的加入对高次谐波的发射影响.我们发现,在短周期线偏振激光脉冲的y方向上附加一个强度较弱的太赫兹场可以有效地扩展谐波的截止位置,并对量子轨道实现调控.通过时频分析、电子波包随时间变化以及半经典三步模型研究了高次谐波发射的物理机制,并对获得的物理现象给出合理的解释.     

啁啾激光与半周期脉冲形成的组合场驱动原子产生单个阿秒脉冲

提出了由波长为800 nm、脉冲宽度为5 fs的啁啾激光与半周期脉冲形成组合场,并利用这种组合场驱动一维模型氦原子获得单个阿秒脉冲. 通过数值求解一维氦原子的含时薛定谔方程,发现氦原子在组合场驱动下高次谐波谱的截止位置可以扩展到I_p+21.6U_p. 对第二平台区域不同范围内高次谐波的叠加都能得到单个阿秒脉冲,最短可达37 as,特别是对平台区域的前端进行叠加不仅能够得到较短的单个阿秒脉冲,而且与截止位置附近高次谐波构造的阿秒脉冲相比,强度提高了3个数量级. 关键词： 啁啾激光场 半周期脉冲 高次谐波 阿秒脉冲     

空间非均匀场下核间距对不对称分子谐波发射的影响

数值研究了空间非均匀场下核间距离对于不对称分子HeH2+发射高次谐波以及阿秒脉冲的影响。计算结果表明,通过适当调节HeH2+分子离子的核间距离以及空间非均匀参数,不仅谐波发射的截止能量得到了延伸,而且单一的短量子路径也被选择出来对谐波发射起作用。随后适当引入第二束控制激光场,谐波截止能量得到了进一步扩展,形成了两个带宽分别在431eV和372eV的连续平台区。 最后,通过适当的叠加谐波,可获得脉宽为31as-65as的一系列阿秒X射线光源。     

Harmonic extension and attosecond pulse generation by using the modified three‐color chirped pulse

Through numerical solution of the quasi‐three‐dimensional time‐dependent Schrödinger equation, the harmonic spectra and attosecond‐pulse generation have been theoretically investigated when a model He atom is exposed to the modified three‐color chirped field (800 nm+1600 nm+1200 nm). It is found that when the chirp parameters are chosen to be β₁ = 0.3 (corresponding to the 800‐nm field), β₂ = 0.6 (corresponding to the 1600‐nm field) and β₃ = ?0.2 (corresponding to the 1200‐nm field), the harmonics have an optimal extension resulting in a 491 eV bandwidth. Further, an isolated 32‐as pulse is directly achieved with proper harmonic superposition.     

Harmonic generation in superconducting Bi(Pb)SrCaCuO thick films

We present a detailed study of harmonic generation in Bi(Pb)SrCaCuO superconducting thick film prepared by screen printing technique. A comparative study of amplitude of harmonics of two films of different J_c have been carried out. The variation of amplitudes of the harmonics are studied as a function of magnitude of ac and dc field. The temperature dependence of amplitude of third harmonic (V³) is studied with increasing amplitude as well as frequency of ac field. These results are analyzed in the frame work of critical state model. V₃ -T curve also indicates the presence of two phases in Bi(Pb)SrCaCuO film.     

Attosecond manipulation of ionization and efficient broadband supercontinuum generation in stretched molecules

<正>We theoretically investigate the high-order harmonic generation from stretched molecules in a linearly polarized intense field.By adopting an infrared pulse combined with an ultraviolet(UV) attosecond pulse,the ionization process can be controlled effectively.In this excitation scheme,the harmonic spectrum beyond I_p+3.17U_P is significantly enhanced by two orders,where I_p and U_p=e~2E_0~2/(4m_eω~2) are the ionization and ponderomotive potential,then smooth broadband supercontinuum with the bandwidth of about 120 eV is obtained,which leads to an isolated sub-60- as attosecond pulse with a high signal-noise ratio.Moreover,the bandwidth of the supercontinuum is weakly dependent on the location and pulse duration of the UV pulse.     

Electron‐Nuclear Dynamics in Molecular Harmonic Generation Driven by a Plasmonic Nonhomogeneous Field

Electron (z)‐nuclear (R) dynamics in the molecular high‐order harmonic generation (MHHG) from H₂⁺ driven by the plasmonic nonhomogeneous field, generated by the surface plasmon polaritons in the bowtie‐shaped nanostructure, have been theoretically investigated through solving the two dimensional time‐dependent Schrödinger equation with the Non‐Bohn‐Oppenheimer approximation. It is found that (i) due to the plasmonic enhancement of the laser intensity, the harmonic cutoff can be extended when the spatial position of H₂⁺ is away from the gap center of the nanostructure. However, due to the limit of the gap size, the threshold value of the harmonic cutoff can be obtained at a given position of H₂⁺. (ii) Due to the asymmetric enhancement of the laser intensity in space, the extended higher harmonics are respectively from E(t) > 0 a.u. or E(t) < 0 a.u. for the cases of the positive and the negative spatial position of H₂⁺. As a result, the intensities of the extended higher harmonics are different and can be controlled by changing the carrier‐envelope phase and the pulse duration of the laser field. (iii) In the few‐cycle pulse duration, the MHHG mainly comes from the multi‐photon resonance ionization (MPRI), while as the pulse duration increases, the MPRI, the charge‐resonance enhanced ionization (CREI) and even the dissociative ionization (DI) are contributed to the MHHG. Moreover, as the spatial position of H₂⁺ moves, the contributions of the MHHG from the MPRI, the CERI and the DI can be controlled. (iv) The contributions of the MHHG from the two‐H nuclei have been investigated and found that when E(t) > 0 a.u., the intensities of the harmonics from the negative‐H is higher than those from the positive‐H; while when E(t) < 0 a.u., the intensities of the harmonics from the positive‐H plays the main role in the MHHG. Moreover, the multi‐minima, caused by the two‐center interference can also be found. (v) Finally, by superposing a properly selected harmonics, a single isolated attosecond pulse (SIAP) with the full width at half maximum (FWHM) of 34 as can be obtained.     

Understanding the reaction between muonium atoms and hydrogen molecules: zero point energy,tunnelling, and vibrational adiabaticity

The advent of very precise measurements of rate coefficients in reactions of muonium (Mu), the lightest hydrogen isotope, with H₂ in its ground and first vibrational state and of kinetic isotope effects with respect to heavier isotopes has triggered a renewed interests in the field of muonic chemistry. The aim of the present article is to review the most recent results about the dynamics and mechanism of the reaction Mu+H₂ to shed light on the importance of quantum effects such as tunnelling, the preservation of the zero point energy, and the vibrational adiabaticity. In addition to accurate quantum mechanical (QM) calculations, quasiclassical trajectories (QCT) have been run in order to check the reliability of this method for this isotopic variant. It has been found that the reaction with H₂(v=0) is dominated by the high zero point energy (ZPE) of the products and that tunnelling is largely irrelevant. Accordingly, both QCT calculations that preserve the products’ ZPE as well as those based on the Ring Polymer Molecular Dynamics methodology can reproduce the QM rate coefficients. However, when the hydrogen molecule is vibrationally excited, QCT calculations fail completely in the prediction of the huge vibrational enhancement of the reactivity. This failure is attributed to tunnelling, which plays a decisive role breaking the vibrational adiabaticity when v=1. By means of the analysis of the results, it can be concluded that the tunnelling takes place through the ν₁=1 collinear barrier. Somehow, the tunnelling that is missing in the Mu+H₂(v=0) reaction is found in Mu+H₂(v=1).     

The microwave spectrum,harmonic force field,and structure of carbonyl chlorofluoride,OCCIF

Rotational spectra of three isotopic species of carbonyl chlorofluoride, OCCIF, have been extensively measured, and have been analyzed for rotational constants, quartic centrifugal distortion constants, and chlorine nuclear quadrupole coupling constants. Ab initio calculations of the harmonic force field have been made using several different sets of basis functions, and their relative cost efficiency has been assessed. The measured distortion constants have been combined with vibrational wavenumbers (both from the literature and from the present work) and with the ab initio force constants to refine the force field. Ground state effective (r₀) and average (r_z) structures have been evaluated for the molecule.     

Schloegl’s Second Model for Autocatalysis on a Cubic Lattice: Mean-Field-Type Discrete Reaction-Diffusion Equation Analysis

Schloegl’s second model for autocatalysis on a hypercubic lattice of dimension d≥2 involves: (i) spontaneous annihilation of particles at lattice sites with rate p; and (ii) autocatalytic creation of particles at vacant sites at a rate proportional to the number of diagonal pairs of particles on neighboring sites. Kinetic Monte Carlo simulations for a d=3 cubic lattice reveal a discontinuous transition from a populated state to a vacuum state as p increases above p=p _e . However, stationary points, p=p _eq (≤p _e ), for planar interfaces separating these states depend on interface orientation. Our focus is on analysis of interface dynamics via discrete reaction-diffusion equations (dRDE’s) obtained from mean-field type approximations to the exact master equations for spatially inhomogeneous states. These dRDE can display propagation failure absent due to fluctuations in the stochastic model. However, accounting for this anomaly, dRDE analysis elucidates exact behavior with quantitative accuracy for higher-level approximations.     

The microwave spectrum,harmonic force field,and structure of difluorodichloromethane

Very large numbers of rotational transitions have been accurately measured for ¹²CF₂³⁵Cl₂, ¹²CF₂³⁵Cl³⁷Cl, and ¹³CF₂³⁵Cl₂, and have been analyzed for rotational constants and quartic centrifugal distortion constants. The distortion constants have been combined with vibrational wavenumbers (both from the literature and from the present work), and with ab initio force constants also evaluated in the present work, to give an approximate harmonic force field. The rotational constants and force field have been used to evaluate ground state effective, substitution, and ground state average structures for the molecule.     

反应物分子初始振动激发对O+HCl→OH+Cl反应的立体动力学性质的影响

在Peterson的高精度从头计算势能面上,运用准经典轨线方法讨论了反应物分子初始振动激发对O+HCl→OH+Cl反应的立体动力学性质的影响.反映两矢量k-j′相关的P(θr)函数的分布说明产物的转动角动量j′在垂直于反应物相对速度矢量k的方向上的排列取向程度随着初始反应物振动量子数的增加而增加;反映三矢量k-k′-j′相关的极角分布函数P(r)显示产物的转动角动量有比较弱的定向效应,且随着初始振动量子数的增加,这种弱的定向效应由沿Y轴负向变为沿Y轴正向.说明反应物分子的初始振动激发有利于增强产物分子的转动排列取向效应,但对产物分子P(r)分布的影响则不明显.