不同核轴取向的O2的高次谐波

分子的高次谐波是强场超快物理的重要研究课题. 采用建立在形式散射理论基础上的频域方法计算了O₂在线偏振激光场下的高次谐波, 探讨了核轴被准直在与激光传输方向垂直的平面内时, 高次谐波随核轴与光电场偏振方向所成夹角θ₀的依赖关系. 结果表明: 各次谐波都是在θ₀约为45°时强度最大, 并有较宽的峰值宽度; 当偏离此角度, 高次谐波的强度变小; 到达平行或垂直取向时, 降到最低. 分析表明, 这是由于高次谐波的强度取决于分子基态的电子在动量空间中的电场方向的布居. 针对核轴被准直在激光传输方向与电场偏振方向所确定的平面内的情况, 计算了高次谐波随θ₀的依赖关系, 结果与前一种情况基本相同. 分析发现, 当核轴被准直固定后, 分子绕核轴旋转的角度ψ没有固定, 所以最后的高次谐波强度需要对不同的ψ 时的高次谐波的贡献求和平均. 平均后相当于波函数相对于核轴旋转对称, 从而导致O₂的高次谐波仅与θ₀有关, 而与核轴被准直在哪个面上无关.     

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.     

Controlling the contributions to high-order harmonic generation from different nuclei of N_2 with an orthogonally polarized two-color laser field

The generation of high-order harmonic and the attosecond pulse of the N2 molecule with an orthogonally polarized two-color laser field are investigated by the strong-field Lewenstein model.We show that the control of contributions to high-order harmonic generation(HHG) from different nuclei is realized by properly selecting the relative phase.When the relative phase is chosen to be φ= 0.4π,the contribution to HHG from one nucleus is much more than that from another.Interference between two nuclei can be suppressed greatly; a supercontinuum spectrum of HHG appears from 40 e V to125 e V.The underlying physical mechanism is well explained by the time–frequency analysis and the semi-classical threestep model with a finite initial transverse velocity.By superposing several orders of harmonics,an isolated attosecond pulse with a duration of 80 as can be generated.     

Infrared diode laser spectroscopy of O2–N2O van der Waals complex in the ν1 symmetric stretch region of N2O

The rovibrational spectrum of O₂–N₂O van der Waals complex is measured in the v₁ symmetric stretch region of N₂O monomer using a tunable diode laser spectrometer. The complex is generated by a slit-pulsed supersonic expansion with gas mixtures of O₂, N₂O, and He. Both a- and b-type transitions are observed. The effective Hamiltonian for an open-shell complex consisting of a diatomic molecule in a ³Σ electronic state and a closed-shell partner is used to analyze the observed spectrum. Molecular constants in the vibrationally excited state are determined accurately. The band-origin of the spectrum is determined to be 1284.7504(25) cm^-1, red-shifted from that of the N₂O monomer by ～ 0.1529 cm^-1.     

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.     

不同取向角下CO2分子波长依赖的垂直谐波效率

通过数值计算, 研究了强激光场中CO₂ 分子在不同波长和取向角下产生的高次谐波辐射的效率. 发现CO₂ 分子的垂直谐波效率在较小的和中间的取向角时倾向于与平行谐波效率可比或更高, 而在较大的取向角时, 垂直谐波效率远低于平行谐波效率. 进一步的分析表明, CO₂ 分子的结构对其垂直谐波效率有重要的影响, 且该影响与波长有关. 建议对于较复杂的分子, 应该在分子的轨道成像实验中考虑垂直谐波的贡献.     

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.     

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     

Rayleigh scattering by sodium vapour in flames

In this paper we report on Rayleigh scattering measurements of sodium on the Na D-doublet in several premixed, laminar, shielded H₂/O₂/N₂, H₂/O₂/Ar and C₂H₂/O₂/N₂ flames at one atm. We performed the measurements under non-saturation conditions. The tunable CW dye-laser used produced linearly polarized light. The laser frequency was tuned well outside the absorption-line width of the sodium D-doublet lines. We have compared the ratio of Rayleigh scattering to collison-induced resonance-fluorescence (measured at fixed detunings of the laser) with theoretical predictions. In some flames, we also measured Rayleigh scattering and its polarization, as a function of detuning of the laser in the 4–40 Å region, for the red Na-D₁ and the blue Na-D₂ wings and found good agreement with theoretical predictions. Polarization of collision-induced fluorescence did not exceed 4% in this wavelength range.     

Two-center interference in high-harmonic generation of H_2~+ in a combination of a mid-infrared laser field and a terahertz field

We theoretically investigate the two-center interference in high-order harmonics generated from the H_2~+ in a combination of a mid-infrared laser and a terahertz field by numerically solving the time-dependent Schr ¨odinger equation(TDSE).The interference minima in high-order harmonic generation(HHG) are effectively suppressed when a THz field is added.The contribution to HHG from the two separate nuclei is used to demonstrate the locating order of the harmonic minima.Furthermore, we also investigate the emission time of harmonics. The results show that the intensity of the short path around 60 thorder after adding a THz field is stronger than that in the mid-infrared laser field, which further illustrates the suppression of the interference minima in HHG.     

超强飞秒激光脉冲作用下氢分子的高次谐波行为——基于含时密度泛函理论的模拟

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,模拟了氢分子在超强飞秒激光脉冲作用下的高次谐波行为. 结果表明氢分子的高次谐波谱具有“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;不同的激光偏振方向会导致高次谐波的截止频率和谱线强度的变化. 关键词： TDDFT 超强飞秒激光 高次谐波 2分子')" href="#">H₂分子     

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.     

激光诱导AlO自由基B2∑+–X2∑+跃迁光谱研究

基于激光诱导击穿光谱技术, 利用Nd:YAG脉冲激光激发Al₂O₃ (含量为99%)陶瓷片产生等离子体, 获得了AlO自由基B²∑⁺–X²∑⁺跃迁的33条发射谱线. 就AlO自由基光谱的时间演化规律和激光能量对谱线的影响规律进行了研究与分析. 结果表明, AlO自由基光谱出现在Al原子和Al离子光谱之后, 且持续时间较长. 当激光的脉冲能量由10 mJ起不断增加时, AlO自由基光谱强度逐渐减小, 且最大值出现时间随激光能量的增加而后移. 在此基础上, 进行了陶瓷等离子体在空气和氩气环境下的对比试验, 发现从Al₂O₃陶瓷片中激发所产生的AlO自由基必须有空气中O₂参与反应. 关键词： 激光诱导击穿光谱 AlO自由基 B²∑⁺–X²∑⁺跃迁光谱')" href="#">B²∑⁺–X²∑⁺跃迁光谱     

Single Ultrashort Attosecond Pulse Generation via Combination of Chirped Fundamental Laser and an Ultraviolet Controlling Pulse

We theoretically study the high-order harmonic generation (HHG) from a hydrogen atom in an intense few-cycle chirped fundamental laser in combination with an ultraviolet (uv) controlling pulse.The high-order harmonic spectrum is calculated by solving the time-dependent Schr¨odinger equation using the split-operator method.In our calculation,we present the difference of the high-order harmonic spectrum from one-dimensional (1D) model hydrogen atom and three-dimensional (3D) real hydrogen atom.We found that the plateau of the high-order harmonic generation from the 1D case and 3D case are all extended effectively to I p + 35U p due to the presence of the chirped laser pulse and the HHG supercontinuum spectrum is generated by adding an ultraviolet controlling pulse at a proper time,but the efficiency of the HHG for 3D case is more higher at the near cut-off region than the 1D case.Therefore,the generation of the attosecond pulse by synthesizing the harmonics near cut-off region have some slight differences between 1D and 3D simulations.As a real 3D case study,we show that an isolated 18 as pulse with a bandwidth of 232.5 eV is generated directly by optmizing the combination laser fields.     

连续辉光放电波导型远红外氘化氰激光器输出性能优化

简要介绍了EAST 装置远红外激光干涉仪光源--DCN 激光器的工作原理、结构和相关改进。DCN 激光器采用He、CD₄、D₂ 和N₂ 4 种工作气体。实验过程中,通过调节气体压强和阴极电流、改变各种工作气体配比等手段优化DCN 激光器输出功率。实验结果显示：输出功率随电流的增大会达到饱和,在电流为1.0A 输出功率达到最大;输出功率随压强先增大后减小,在压强为32Pa 时达到最大值;工作气体的最佳配比为He: CD₄: D₂: N₂=2: 3: 5: 3。     

Effects of surface treatments and annealing on carbon-based molecular sieve membranes for gas separation

A new method in preparing carbon-based molecular sieve (CMS) membranes for gas separation has been proposed. Carbon-based films are deposited on porous Al₂O₃ disks using hexamethyldisiloxane (HMDSO) by remote inductively coupled plasma (ICP) chemical vapor deposition (CVD). After treating the film with ion bombardment and subsequent pyrolysis at a high temperature, carbon-based molecule sieve membranes can be obtained, exhibiting a very high H₂/N₂ selectivity around 100 and an extremely high permeance of H₂ around 1.5 × 10⁻⁶ mol m⁻² s⁻¹ Pa⁻¹ at 298 K. The O₂/N₂ selectivity could reach 5.4 with the O₂ permeance of 2 × 10⁻⁷ mol m⁻² s⁻¹ Pa⁻¹ at 423 K.

During surface treatments, HMDSO ions were found to be more effective than CH₄, Ar, O₂ and N₂ ions to improve the selectivity and permeance. Short and optimized surface treatment periods were required for high efficiency. Without pyrolysis, surface treatments alone greatly reduced the H₂ and N₂ permeances and had no effect on the selectivity. Besides, without any surface treatment, pyrolysis alone greatly increased the H₂ and N₂ permeances, but had no improvement on the selectivity, owing to the creation of large pores by desorption of carbon. A combination of surface treatment and pyrolysis is necessary for simultaneously enhancing the permeance and the selectivity of CMS membranes, very different from the conventional pore-plugging mechanism in typical CVD.     

光谱法结合分子动力学模拟研究臭氧对肌红蛋白结构的作用机制

臭氧(O₃)是一种具有强氧化性作用的杀菌消毒剂,因其安全无害等特点已被广泛用于肉制品生产加工的减菌处理,但O₃减菌处理对红肉色泽具有较强的负面作用,且其作用机制尚缺乏研究。针对肌红蛋白（Mb）存在状态是决定红色肉色泽关键因素的基础,通过紫外-可见吸收光谱法、荧光光谱法和圆二色光谱法（CD）研究O₃作用下Mb的光谱特性变化,结合蛋白质氧化特征指标分析和分子动力学模拟技术探究O₃对Mb分子的作用效果与机制。光谱研究结果表明,O₃处理可使Mb的紫外-可见光谱图在412 nm左右处的铁卟啉环特征峰及540和580 nm附近的氧合肌红蛋白（OMb）特征峰的强度减弱,其中铁卟啉环特征峰发生蓝移;利用固定激发波长280 nm下测定Mb内源性荧光和同步荧光光谱表明O₃会降低Mb的荧光强度,增大铁卟啉基团贡献的荧光峰强度和造成酪氨酸残基荧光光谱特征峰的蓝移;O₃作用使Mb三维荧光光谱特征峰强度的下降及光散射强度的增加。以上变化推断出O₃会促进Mb的氧化,造成其氨基酸残基疏水基团裸露,使Mb所处微环境及其蛋白构象改变;CD分析表明O₃与肌红蛋白接触时间越久,蛋白质二级结构变化越明显,造成α-螺旋的含量下降,无规则卷曲增加。辅以检测不同强度O₃处理Mb的含量及性质的变化,可知O₃处理使OMb含量下降,高铁肌红蛋白（MMb）含量增加,同时O₃处理Mb的羰基含量增加和巯基含量下降,这也进一步证实O₃作用促进了Mb的氧化,此外,O₃处理Mb表面疏水性的增强,说明O₃造成Mb体系微环境的极性变化。分子动力学模拟结果显示O₃会提高Mb肽链的RMSD值,影响Mb肽链的稳定性,减弱铁卟啉环与Mb肽链的相互作用;RMSF结果表明Mb活性口袋附近氨基酸残基的变化较大;蛋白质二级结构分析与光谱学试验研究结果一致,Mb的α-螺旋的含量下降,无规则卷曲增加。总而言之,O₃可作用于Mb的氨基酸残基,导致蛋白质二级结构和疏水性改变,并发生蛋白氧化及铁卟啉环暴露,进而引起红色肉色泽发生改变。该研究可为生鲜红肉护色技术制定等提供一定理论依据。     

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.     

圆偏振激光脉冲附加静电场或太赫兹场时H2+高次谐波产生

本文通过数值求解二维含时薛定谔方程理论的研究了圆偏振激光脉冲(circularly polarized laser pulse, CPLP)作用下H2+的高次谐波产生(high-order harmonic generation, HHG)。通过对比CPLP附加静电场和CPLP附加太赫兹场(terahertz, THz)时的高次谐波发射谱发现,当在CPLP的方向附加静电场时,谐波谱出现双平台结构,且布满调制,通过电子波包概率分布图像发现,电子三次与母核复合,量子轨道之间产生了较严重的干涉。当附加相同强度的THz场时,电子仅两次与母核复合,量子轨道之间的干涉减少,最终得到了86eV到208eV带宽为122eV的连续谱,相比于附加静电场,谐波谱变得连续且平滑,实现了量子轨道调控。最后,利用半经典三步模型、时频分析和电离几率等对谐波发射物理机制进行了深入研究。