飞秒激光激发空气电离的阈值研究

报道在脉宽50fs—22ps,波长800nm脉冲激光作用下的空气电离阈值的研究结果.利用探测等离子体发光信号的方法,实验测量了激发空气电离所需的阈值激光强度.结果表明,当激光脉冲宽度从50fs增加到22ps时,阈值光强I_th从8.7×10¹⁴W/cm²下降到2.7×10¹³W/cm²;I_th经历了由迅速降低逐渐发展为缓慢降低的过程.在50fs—1p 关键词： 飞秒激光 阈值 多光子电离 碰撞电离     

利用相干光照明的纹影成像装置研究飞秒激光脉冲烧蚀铝靶喷射物相位的超快时间演化

本文提出了一种基于纹影成像装置的新型相位检测方法, 并使用该方法对飞秒激光烧蚀铝靶产生的喷射物的超快相位演化过程进行了实验研究. 与传统的纹影法不同, 本文的相位检测方法使用相干光作为成像照明光, 利用未透过样品的背景光作为参考光, 借助透过样品后在纹影装置刀口处衍射的照明光与背景照明光的干涉, 检测样品的相位; 其最显著的优点是能够清晰反映被测样品mπ或2mπ (m为整数) 的相位改变. 利用该方法, 结合抽运-探测技术, 研究了激光流量为5.4 J/cm²的50 fs脉冲激光烧蚀铝靶产生的喷射物的超快相位演化. 实验发现, 烧蚀过程中形成的喷射物可分为三个相位不同的区域, 分别对应等离子体态的喷射物、后续的垂直靶面喷射的物质和冲击波. 其中, 等离子体态的喷射物在0–9.0 ns的时间延迟内, 由于膨胀和电子复合作用, 相位变化超过π; 而后续的垂直靶面的喷射物在此时间内的相位变化没有超过π. 关键词： 相位检测方法 纹影成像技术 相干光照明 抽运-探测技术     

CHClF2在强红外激光作用下C2*d3Пg态的形成机制

用TEACO₂激光辐照CHCIF₂分子生成电子激发态C₂^*自由基,观察到斯旺带系的六个谱带。本文根据C₂分子态位能曲线的特点,提出C₂^*d³Π_g态的形成机制。C₂是少数较特殊的分子之一,其激发态b³Σ_g^-与第一激发态a关键词：     

C_2^+ (X^4 Σ_g^-,1^4 Σ_u^+)离子体系解析势能函数、光谱常数和振动能级研究

采用多参考组态相互作用(MRCI)方法,结合aug-cc-pV6Z(AV6Z)基组,计算了C₂⁺(X⁴Σ_g^-,1⁴Σ_u⁺)的势能曲线,计算过程中考虑了Davidson修正和相对论效应,并将结果外推至完备基组(CBS)的极限.基于得到的单点能量,用最小二乘法方法进行了Murrell-Sorbie函数拟合,得到了势能函数解析式(APEF).基于APEF,计算了C₂⁺(X⁴Σ_g^-,1⁴Σ_u⁺)离子体系的离解能D_e,平衡核间距R_e,光谱常数ω_e,ω_eχ_e,B_e,α_e,结果与实验和其他理论计算值符合...     

H$lt;sub$gt;2$lt;/sub$gt;$lt;sup$gt;+$lt;/sup$gt;在强激光场中的解离及其量子调控的理论研究

利用非波恩-奥本海默近似的三维含时量子波包法,理论研究了氢分子离子在强激光场中的解离动力学.通过分析H₂⁺在不同的初始振动态（ν=0–9）和激光场强度下的解离核动能谱,得到了H₂⁺的光解离机理及其随激光场的变化规律.研究结果表明：当激光场的强度I₁=5.0×10¹³ W/cm²时,分子的解离来源于高振动态ν=5–9,其解离机理主要是通过键软化、键硬化和阈下解离过程.当激光场的强度I₂=1.0×10¹⁴ W/cm² 时,H₂⁺在低振动态ν=3–4上的阈上解离起主导作用,而高振动态的键软化、键硬化和阈下解离所占的比重明显地下降了.研究结果为后续的量子调控的实验研究提供了科学的理论预测和指导. 关键词： 光解离 氢分子离子 含时波包法 核动能谱     

控制场对宽带超连续谱产生的影响

研究了控制场对宽带超连续谱产生的影响,计算表明控制脉冲的波长在1.6±0.2 μm范围内调节时,谐波谱的超连续部分形状几乎没有变化,截止区位置和超连续谱宽度变化都小于5%.随着控制场相对于基频场强度的增加,谐波谱上超连续部分的宽度会增加.采用强度为6×10¹⁴ W/cm²,波长为800 nm,脉冲宽度为12 fs的多光周期基频脉冲叠加脉冲宽度为30 fs,波长为1.6 μm,相对相位为-0.1π,相对强度为20%的控制场作为驱动脉冲,选出了短量子轨道并产生105 关键词： 宽带 超连续谱 阿秒脉冲 短量子轨道     

氟利昂F1110分子在飞秒激光脉冲作用下的多光子解离动力学

含氟利昂在内的含氯化合物在太阳光辐射下解离生成破坏臭氧的游离态氯原子, 是破坏大气臭氧层的主要元凶. 本文利用飞行时间质谱技术及离子速度成像技术研究了氟利昂F1110(四氯乙烯)分子在800 nm飞秒脉冲光作用下的多光子解离动力学. 利用飞行时间质谱探测技术, 得到了四氯乙烯在800 nm飞秒激光脉冲作用下发生多光子解离产生的碎片质谱, 发现了两个主要碎片离子C₂Cl₃⁺和 C₂Cl₂⁺. 对应的解离机理分别为单个C-Cl键断裂直接生产氯自由基C₂Cl₄⁺→C₂Cl₃⁺ +Cl 和两个C—Cl 键断裂C₂Cl₄⁺→C₂Cl₂⁺+2Cl: 利用离子速度成像技术对这两种机理产生的碎片离子进行成像, 得到了C₂Cl₃⁺ 和C₂Cl₂⁺ 离子的速度影像. 分析发现这两个碎片离子的动能分布均可由两个高斯分布曲线拟合, 说明这两种解离机理分别还对应了两种解离通道. 通过影像分析得到了解离的平动能分布和角向分布各向异性参数等详尽的动力学信息. 通过高精度密度泛函理论计算对解离动力学进行了进一步的分析和讨论.     

非平行偏振双色场驱动产生脉宽稳定的单个宽谱阿秒脉冲

提出一种直接得到脉宽稳定的单个宽谱阿秒脉冲的新方法.利用波长为800 nm脉宽为5 fs的超短脉冲叠加上偏振方向与主脉冲成π/3,脉宽同样为5 fs的二次谐波脉冲驱动氦原子,可以得到宽度达到50 eV的超连续谱.当二次谐波的强度大于10¹⁴ W/cm²时,超连续谱的位置以及谱宽几乎不会随着二次谐波脉冲的强度的改变而改变.对85—125 eV的超连续谱进行滤波可以直接得到100 as左右的单个阿秒脉冲,这个性质对于实验上获得单个宽谱阿秒脉冲而言是非常有利的. 关键词： 阿秒脉冲 超连续谱     

利用速度成像技术研究碘乙烷多光子电离解离动力学

卤代烷烃会破坏臭氧层,而碘乙烷（C₂H₅I）是卤代烷烃中重要代表物质之一.采用离子速度成像技术、飞秒激光技术和飞行时间质谱技术,探究了C₂H₅I的多光子电离解离动力学.通过分析C₂H₅I在强场作用下多光子电离解离得到的解离通道、碎片的动能、角度分布和各向异性参数等信息来研究碘乙烷离子（C₂H₅I⁺）C–I键裂解机理.根据飞行时间质谱实验,C₂H₅I在飞秒激光脉冲作用下发生多光子电离解离得到的碎片有C₂H₅⁺,I⁺,CH₂I⁺,C₂H₂⁺,C₂H₃⁺,C₂H₄⁺等.与C–I键相关的碎片为C₂H₅⁺和I⁺,解离机制分别对应于C₂H₅I⁺→C₂H₅⁺+I和C₂H₅I⁺→C₂H₅+I⁺.同时,采用离子速度成像技术研究C₂H₅I⁺的C–I键裂解产生的C₂H₅⁺和I⁺的速度影像,得出两者的速度分布和动能分布,分析结果表明C–I键裂解产生C₂H₅⁺和I⁺的过程都存在高能通道和低能通道.进一步分析解离碎片离子的角度分布发现C₂H₅⁺解离时各向异性参数接近于0,可能对应于慢速的振动预解离过程.I⁺在解离时各向异性参数较高,可能源于排斥势能面上的快速解离过程.最后采用密度泛函理论计算了C₂H₅I分子电离前后构型变化、离子态的能级强度及谐振强度,对C₂H₅I⁺的解离机制做了更进一步的分析和讨论.     

氟利昂F113分子在飞秒激光作用下的多光子电离解离动力学

大气臭氧层因吸收太阳紫外光, 是人类必不可少的保护伞. 氟利昂在太阳光辐射下解离生成破坏臭氧的游离态氯原子, 是破坏大气臭氧层的主要元凶之一. 本文利用飞行时间质谱技术和离子速度成像技术研究了氟利昂F113(三氟三氯乙烷)分子在800 nm 飞秒光作用下的多光子电离解离动力学. 利用飞行时间质谱探测技术, 得到了三氟三氯乙烷在该波长飞秒激光作用下发生多光子电离解离产生的碎片质谱. 通过荷质比对碎片质谱进行了详细的标定和分析. 在质谱上未发现母体离子, 所有观察到的离子都是由于激光脉冲作用下产生的碎片. 三个最主要的碎片离子是CFCl₂⁺, CF₂Cl⁺, C₂F₃Cl₂⁺. 通过飞行时间质谱标定, 发现并归属了多个解离通道. 三个主要的解离机理分别为: 1) C-Cl键断裂直接生产氯自由基的通道C₂F₃Cl₃⁺→C₂F₃Cl₂⁺+Cl; 2) C--C键断裂C₂F₃Cl₃⁺→CFCl₂⁺+CF₂Cl; 3) C--C键断裂C₂F₃Cl₃⁺→CF₂Cl⁺+CFCl₂. 利用离子速度成像技术对这三个主要通道产生的碎片离子进行成像, 得到了C₂F₃Cl₂⁺, CFCl₂⁺和CF₂Cl⁺离子的速度影像. 由C--Cl键断裂产生的碎片离子C₂F₃Cl₂^{+}的速度分布由两个高斯分布曲线拟合, 而由C--C键断裂产生的碎片离子CFCl₂⁺和CF₂Cl⁺可以用一个高斯曲线拟合. 通过影像分析得到了解离碎片的平动能分布和角向分布各向异性参数等详尽的动力学信息. 结合高精度密度泛函理论计算对解离动力学进行了进一步的分析和讨论.深入认识氟利昂的解离动力学可为进一步控制破坏臭氧层提供理论参考和实验依据.     

Femtosecond laser ablation of DAST

High rate femtosecond (fs) laser ablation of the organic salt 4-N,N-dimethylamino-4-N-methyl-stilbazolium tosylate (DAST), an organic crystal with very high optical nonlinearities has been demonstrated. The threshold fluence and the ideal fluence range for damage free ablation for the wavelengths 550, 600, and 775 nm have been determined and the quality of the produced grooves has been investigated. The threshold fluences are in the order of 10–70 mJ/cm² and the ideal fluence range for damage free ablation is ranging from 30 to 300 mJ/cm², depending on the wavelength. The optimal focussing for ablation has been investigated and first results towards the structuring of a ridge waveguide are presented. We conclude that this method is most promising for waveguide patterning of DAST surfaces for integrated optics applications.     

Picosecond and femtosecond pulsed laser ablation and deposition of quasicrystals

A Nd:glass laser with pulse duration of 250 fs and 1.3 ps has been used to evaporate a Al₆₅Cu₂₃Fe₁₂ quasicrystalline target. The gaseous phase obtained from the ablation process has been characterised by several techniques such as emission spectroscopy, quadrupole mass spectrometry and ICCD imaging, used to study the plume composition, energy and morphology. The results show that the ablation processes in the short-pulse regimes are very different to the nanosecond one. In particular the plume angular distribution shows a characteristic high cosine exponent and the composition is completely stoichiometric and independent from the laser fluence. Furthermore the mass spectra indicate the presence of clusters, both neutral and ionised and the emission from the target suggest a rapid thermalisation leading to the melting of the surface. To clarify the ablation process some films have been deposited, on oriented silicon, at different experimental conditions and analysed by scanning electron microscopy, atomic force microscopy, energy dispersive X-ray analysis and X-ray diffraction. The analyses show the presence of nanostructured films retaining the target stoichiometry but consisting of different crystalline and non crystalline phases. In particular the nanostructure supports the hypothesis of the melting of the target during the ablation and a mechanism of material ejection is proposed for both picosecond and femtosecond regimes.     

Features of plasma plume evolution and material removal efficiency during femtosecond laser ablation of nickel in high vacuum

We present an experimental characterization describing the characteristics features of the plasma plume dynamics and material removal efficiency during ultrashort, visible (527 nm, ≈300 fs) laser ablation of nickel in high vacuum. The spatio-temporal structure and expansion dynamics of the laser ablation plasma plume are investigated by using both time-gated fast imaging and optical emission spectroscopy. The spatio-temporal evolution of the ablation plume exhibits a layered structure which changes with the laser pulse fluence F. At low laser fluences (F<0.5 J/cm²) the plume consists of two main populations: fast Ni atoms and slower Ni nanoparticles, with average velocities of ≈10⁴ m/s for the atomic state and ≈10² m/s for the condensed state. At larger fluences (F>0.5 J/cm²), a third component of much faster atoms is observed to precede the main atomic plume component. These atoms can be ascribed to the recombination of faster ions with electrons in the early stages of the plume evolution. A particularly interesting feature of our analysis is that the study of the ablation efficiency as a function of the laser fluence indicates the existence of an optimal fluence range (a maximum) for nanoparticles generation, and an increase of atomization at larger fluences. PACS 52.50.-b; 52.38.Mf; 79.20.Ds; 81.07.-b     

Femtosecond uv excimer laser ablation

Experiments on the ablation of polymethylmethacrylate (PMMA) with 300 fs uv excimer laser pulses at 248 nm are reported for the first time. With these ultrashort pulses, ablation can be done at fluences up to five times lower than the threshold fluence for 16 ns ablation of PMMA, and the surface morphology is improved, also for several other materials. A model for ablation is proposed, assuming a non-constant absorption coefficient _eff depending on the degree of incubation of the irradiated material and the intensity of the incoming excimer laser pulse. The agreement between our model and our experimental observations is excellent for 16 ns excimer laser pulses, also predicting perfectly the shape of a pulse transmitted through a thin PMMA sample under high fluence irradiation. Qualitative agreement for 300 fs excimer laser pulses is obtained so far.     

飞秒激光对高反膜的破坏及其超快动力学过程

研究了800nm飞秒激光照射下45°高反膜ZrO2-Si O2的破坏及其超快动力学过程。利用原子力显微镜和扫描电镜观察了材料的烧蚀形貌,测量了破坏阈值与脉冲宽度、烧蚀深度与脉冲能量的依赖关系。随着脉冲宽度从50fs增加到900fs,其烧蚀阈值从0.35J/cm2增加到1.78J/cm2。烧蚀深度与激光能流密度近似成对数关系。当激光强度略高于烧蚀阈值时,材料很快被烧蚀到几百纳米,烧蚀深度表现出明显的层状特性。同时,利用建立的抽运探针实验系统,测量了高强度抽运脉冲作用下材料对探针光的反射率随延迟时间的变化,揭示了薄膜烧蚀的超快动力学过程。实验结果表明高反膜表层的材料对烧蚀特性有重要影响。     

Ad-hoc design of temporally shaped fs laser pulses based on plasma dynamics for deep ablation in fused silica

We have analyzed the ablation depth yield of fused silica irradiated with shaped pulse trains with a separation of 500 fs and increasing or decreasing intensity envelopes. This temporal separation value is extracted from previous studies on ablation dynamics upon irradiation with transform-limited 100 fs laser pulses. The use of decreasing intensity pulse trains leads to a strong increase of the induced ablation depth when compared to the behavior, at the same pulse fluence, of intensity increasing pulse trains. In addition, we have studied the material response under stretched (500 fs, FWHM) and transform-limited (100 fs, FWHM) pulses, for which avalanche or multiphoton ionization respectively dominates the carrier generation process. The comparison of the corresponding evolution of the ablated depth vs. fluence suggests that the use of pulse trains with decreasing intensity at high fluences should lead to enhanced single exposure ablation depths, beyond the limits corresponding to MPI- or AI-alone dominated processes.     

Pulsed laser ablation of La0.5Sr0.5CoO3

The ablation process of La_0.5Sr_0.5CoO₃ by a spatial uniform 248 nm excimer laser beam has been characterized. Ablation rates, changes in the target surface morphology and composition have been studied as a function of the laser fluence. The dependence of the ablation rate on the laser fluence has been explained by a model based on plasma absorption. The threshold fluence for complete dissociation of the surface has been determined and is found equal to 0.7 J/cm². Above this threshold, a steady-state target surface condition is obtained within 30 pulses. Below the threshold fluence, CoO nuclei form, which have a pronounced effect on the target composition and morphology. In addition, ellipsometric and reflectance spectra have been measured in the photon energy range of 1.8 to 5.0 eV.     

Two-dimensional imaging of atomic and nanoparticle components in copper plasma plume produced by ultrafast laser ablation

We report on the spatial and temporal evolution of the plume generated during ultrafast laser ablation of a pure copper target with 800 nm, ≈50 fs, Ti: Sapphire laser pulses. Time-gated imaging was used to record 2-dimensional images of plume populations. The temporal evolution of neutral (Cu*), and ionic (Cu⁺) components of the plume are separately imaged by exploiting bandpass interference filters, while nanoparticles are investigated by collecting their characteristic broadband emission. The ionic component of the plume moves two to three times faster than the neutral component, with a velocity which is almost independent of laser fluence. Plume emission intensity variations at different fluences and delay times are studied for both atomic and nanoparticle components.     

Temporal evolution of laser-ablated Co ions probed by time-of-flight mass spectrometry

A pulsed-field time-of-flight mass spectrometric (TOFMS) technique was used to investigate the expansion dynamics of the ionic species ejected from the visible (λ=532 nm) laser ablation of cobalt target at low laser fluence less than 1 J/cm². The temporal evolution of Co⁺ ions was studied by varying the delay time of the ion repelling pulse with respect to the laser irradiation, which provides significant information on the ablated plume characterization. The obtained TOF mass spectra were well fitted by shifted Maxwell–Boltzmann distributions on a stream velocity, commonly used to describe the measured velocity distributions. The TOF distribution of Co⁺ ions showed a bimodal distribution with fast and slow velocities. These velocities show a decreasing tendency with delay time, which is attributed to the gas collisions between the plume ejecta and to the related gas dynamics. The present results suggest that the in situ measurements of the most probable velocity of ablated ions along the normal to the solid target can be accomplished by the simple technique of a laser ablation/TOFMS.