飞秒强激光场下分子的场致电离和库仑爆炸

利用飞行时间质谱仪和飞秒激光放大系统,对分子在飞秒强激光脉冲作用下的场致电离和库仑爆炸过程进行了研究.在飞行时间质谱中,原子离子的谱峰分裂标志着这些原子离子来源于高价母体离子的库仑爆炸.通过对不同结构的分子在飞秒强激光下的库仑爆炸研究,发现这些分子离子的爆炸是一个协同过程.母体离子的角分布呈现了高度的各向同性,而原子离子则呈现了高度的各向异性分布.这说明分子在飞秒激光场中发生了空间准直和重新定位.     

基于光电子成像技术的碘甲烷多光子电离行为

利用飞秒光电子成像技术研究了碘甲烷在超短激光脉冲场中的多光子电离解离行为.实验获得了碘甲烷分子在400 nm飞秒激光作用下的飞行时间质谱以及电离产生的光电子影像.实验结果表明,在超短脉冲激光场中,分子的电离通常是非共振电离,电离产物主要为母体离子和极少量的碎片离子.从光电子成像中获得的光电子平动能分布可以得到电离产生的电子p_1(2. 03 eV)和p_2(2. 67 eV)分别来源于母体离子的基态和激发态.从光电子成像中获得的角度分布可以推测出,光电子峰p_1和p_2可以分别近似看做单光子电离和双光子电离过程,且光电子散射角度趋于各向同性分布.     

飞秒激光场中甲醇产物离子的角分布

利用直流切片离子成像技术结合飞行时间质谱技术,我们研究了甲醇(CH_3OH)分子在800 nm飞秒激光场中的多光子解离和库仑爆炸过程.获得了甲醇分子在光场中的飞行时间质谱和产物离子的切片影像,分析得到了不同库仑爆炸通道碎片离子的动能分布和角度分布.本文对比分析了C-O键断裂产生H_2O~+的H转移通道和产生OH~+的非H转移通道的角分布,计算了不同激光强度下两个通道的各向异性参数α_2和(cos~2θ),并根据产物离子角度分布与激光强度和离子价态的关系,揭示了甲醇分子在飞秒光场中的准直机制为动力学准直.     

飞秒激光驱动的分子库仑爆炸研究

飞秒强激光作用下,分子发生多电荷电离,产生高价分子离子.由于电荷间的库仑排斥作用,高价分子离子会发生库仑爆炸,生成的碎片离子具有较大平动能量.本文结合在北京大学开展的飞秒强场分子库仑爆炸研究,介绍了飞秒强激光驱动的分子库仑爆炸的重要进展、潜在应用和未来发展方向.     

分子光谱和光解离动力学研究实验装置的研制

本文介绍了新研制的研究分子光谱和光解离动力学实验装置的主要结构和功能,其特点是集激光光解、激光诱导等离子体、激光诱导荧光、共振增强多光子电离和时间飞行质谱等研究技术于一体.详细介绍了在该实验装置上可开展的研究工作和实验方案设计,诸如:分子、自由基及其离子的共振增强多光子电离谱研究、含金属自由基的激光诱导荧光和共振增强多光子电离研究、多原子分子的光解离动力学研究等.并给出了在该装置上测定的CS2激光共振增强多光子电离的时间飞行质谱信号.     

溴丙烯在800nm和400nm飞秒激光强场下的解离电离

利用自行搭建的飞行时间质谱仪,在800 nm和400 nm飞秒激光强场下对溴丙烯分子进行了电离解离过程的探究.通过分析离子产物的产率与激光功率的依赖关系并结合Keldysh因子计算,给出了实验中母体分子的电离机制;理论上,利用量子化学计算软件(Gaussian 09),对分子的化学键柔性力常数、反应通道出现势进行了计算,确认了溴丙烯分子的电离解离通道,发现了非共振多光子吸收导致的多个化学键的同时断裂,解释了母体分子离子电荷布局对反应路径的影响.     

飞秒激光分子结构成像

飞秒激光具有超短的脉冲宽度和超强的峰值功率,它在科学研究中的广泛应用极大地提高了人类认识物质世界的能力.本文介绍我们基于飞秒强激光作用下分子的隧道电离和库仑爆炸,在分子轨道和分子构型成像方面的研究进展.     

钴原子激发态光电离的实验研究

文章报道了在300-310nm波长范围内3d过渡金属Co原子共振增强多光子电离(REMPI)的实验研究结果.实验中采用激光烧蚀和高压脉冲超声分子束相结合的技术制备等离子体,获得的等离子体与探测激光作用形成光电离产物,由飞行时间质谱仪对光电离产物进行甄别.通过分析光电离产物产额随探测激光强度的变化关系,得到了Co原子激发态的绝对光电离截面.     

邻苯二甲酸为基质用于基质辅助激光解吸/电离飞行时间质谱测定小分子物质

以邻苯二甲酸为基质对多巴胺(153.08 Da)进行基质辅助激光解吸/电离飞行时间质谱(MALDI TOFTOF MS)分析.结果表明,邻苯二甲酸作为基质可以有效解吸电离多巴胺,基质干扰峰明显减少,产生出了分辨率高、离子信号强、信噪比(S/N)高的质谱图,不仅准确测定了多巴胺的相对分子质量,完成了对其定性研究,还找到了一种适合小分子分析而且来源广泛的基质材料.     

无机共轭分子的结构——Ⅲ.A_2B_4型分子

本文用LCAO MO法讨论了A_2B_4型无机分子的结构,具体地分析了包含34,36和38个价电子的A_2B_4型分手和离子的结构和性质。本文着重地研究了N_2O_4分子的键型,认为NN键具有σ性质和π性质,N_2O_4分子中存在Π_6~8键,NN距离比正常单键键长长0.27乃是由于O原子间凡德华斥力以及N原子间静电斥力所引起的。 N_2O_3分子在结构上与N_2O_3分子十分相似,本文也一并讨论。     

Ionization and dissociation of CH<Subscript>2</Subscript>I<Subscript>2</Subscript> and CH<Subscript>2</Subscript>ICl in femtosecond intense field

With the development of ultrafast laser technique,the femtosecond laser electric field is comparable to themolecular field experienced by valence electrons. In thiscase, the classical quantum mechanical theory, based onperturbation theory, becomes inapplicable. Theoreticalunderstanding of the interaction of molecules with intenselaser radiation is quite difficult. The Coulomb explosionhas been extensively studied[1—10] and explained by somesemiclassical models, such as the above threshold ion…     

飞秒激光场下NH3分子光电子能谱的理论研究

模拟了NH3分子在飞秒激光场下通过中间快速预解离态A～的共振增强多光子电离光电子能谱(REMPI-PES).应用两维的含时波包法实施动力学计算,计算过程中使用了离散变量表示(DVR)理论和劈裂算符-表象变换方法.结果表明,激光脉冲的强度、脉宽等对光电子能谱有着很大的影响,能谱中的两组峰簇是由强场对势能面作用所引起的.     

NaI分子在强场作用下的非绝热动力学研究

利用含时量子波包法研究了NaI分子在飞秒激光脉冲场作用下运动到势能面交叉区域的非绝热动力学以及泵浦-探测光电离动力学。根据动力学反射原理,得到了NaI分子在非绝热交叉区域的波包动力学与泵浦-探测光电子能谱之间的对应关系。研究结果给出了NaI分子在强场作用下的非绝热特性。     

Editor’s note

The past two decades have witnessed great progress in development of ultrashort laser pulse in laser science, often at an unexpected speed. It has found various applications, both theoretical and practical, in the frontiers of science.     

kHz 脉冲分子束的产生及其在强场原子分子物理实验中的应用

采用悬臂压电脉冲阀, 制备出最高重复频率达到3 kHz 的脉冲分子束。通过测量氮气分子束在飞秒激光作用下隧道电离生成的N2 +(B-X)荧光光谱, 对脉冲阀的性能做了表征。这种kHz 脉冲分子束搭配kHz 飞秒激光器, 将推动飞秒强激光驱动的原子分子动力学实验研究。     

Attosecond control of electronic processes by intense light fields

The amplitude and frequency of laser light can be routinely measured and controlled on a femtosecond (10(-15) s) timescale. However, in pulses comprising just a few wave cycles, the amplitude envelope and carrier frequency are not sufficient to characterize and control laser radiation, because evolution of the light field is also influenced by a shift of the carrier wave with respect to the pulse peak. This so-called carrier-envelope phase has been predicted and observed to affect strong-field phenomena, but random shot-to-shot shifts have prevented the reproducible guiding of atomic processes using the electric field of light. Here we report the generation of intense, few-cycle laser pulses with a stable carrier envelope phase that permit the triggering and steering of microscopic motion with an ultimate precision limited only by quantum mechanical uncertainty. Using these reproducible light waveforms, we create light-induced atomic currents in ionized matter; the motion of the electronic wave packets can be controlled on timescales shorter than 250 attoseconds (250 x 10(-18) s). This enables us to control the attosecond temporal structure of coherent soft X-ray emission produced by the atomic currents--these X-ray photons provide a sensitive and intuitive tool for determining the carrier-envelope phase.     

Dissociation of NO2 in femtosecond intense fields

The study of molecules in strong laser fields is a challenging topic in molecular science[1―10]. With the advent of short-pulse lasers, the behavior of molecules can be explored on the time scale of vibrational mo-tions. An intense and linearly polarized…     

Adaptive subwavelength control of nano-optical fields

Adaptive shaping of the phase and amplitude of femtosecond laser pulses has been developed into an efficient tool for the directed manipulation of interference phenomena, thus providing coherent control over various quantum-mechanical systems. Temporal resolution in the femtosecond or even attosecond range has been demonstrated, but spatial resolution is limited by diffraction to approximately half the wavelength of the light field (that is, several hundred nanometres). Theory has indicated that the spatial limitation to coherent control can be overcome with the illumination of nanostructures: the spatial near-field distribution was shown to depend on the linear chirp of an irradiating laser pulse. An extension of this idea to adaptive control, combining multiparameter pulse shaping with a learning algorithm, demonstrated the generation of user-specified optical near-field distributions in an optimal and flexible fashion. Shaping of the polarization of the laser pulse provides a particularly efficient and versatile nano-optical manipulation method. Here we demonstrate the feasibility of this concept experimentally, by tailoring the optical near field in the vicinity of silver nanostructures through adaptive polarization shaping of femtosecond laser pulses and then probing the lateral field distribution by two-photon photoemission electron microscopy. In this combination of adaptive control and nano-optics, we achieve subwavelength dynamic localization of electromagnetic intensity on the nanometre scale and thus overcome the spatial restrictions of conventional optics. This experimental realization of theoretical suggestions opens a number of perspectives in coherent control, nano-optics, nonlinear spectroscopy, and other research fields in which optical investigations are carried out with spatial or temporal resolution.