用质谱和光电子能谱研究飞秒强场中的电离动力学

报导了用自制飞秒激光器通过飞秒多光子电离质谱和光电子能谱对飞秒强激光场与分子（氨、苯）相互作用的研究,飞秒激光脉宽约１００ｆｓ,二倍频中心波长４０７．５ｎｍ,聚焦后脉冲功率密度达到１０＾１２Ｗ／ｃｍ＾２,氨的光电子能谱显示了（２＋２）ＲＥＭＰＩ和（２＋２）＋１ＡＴＩ、（２＋２）＋２ＡＴＩ三组电子峰,每组峰又包括伸缩振动ｖ１的带系,ＡＴＩ峰的振动布居出现反转,随着光强增加,谱峰加宽而且振动能级出现平     

Autler-Townes Splitting in Photoelectron Spectrum of Three-Level Li2 Molecule in Ultrashort Pulse Laser Fields

The Autler-Townes （AT） splitting in femtosecond photoelectron spectrum of three-level Li2 molecules is theoretically investigated using time-dependent quantum wave packet method. With proper femtosecond laser pulses, three peaks of the AT splitting can be observed in the photoelectron spectrum. The AT splitting stems from rapid Rabi oscillation caused by intense ultrashort laser pluses. The effects of laser parameters on the molecular ionization dynamics are also discussed.     

Quantum-mechanical analysis of pulse reconstruction for a narrow bandwidth attosecond x-ray pulse

The photoelectron energy spectra (PESs) excited by narrow bandwidth attosecond x-ray pulses in the presence of a few-cycle laser are quantum-mechanically calculated. Transfer equations are used to reconstruct the detailed temporal structure of an attosecond x-ray pulse directly from a measured PES. Theoretical analysis shows that the temporal uncertainties of the pulse reconstruction depend on the x-ray bandwidth. The procedure of pulse reconstruction is direct and simple without making any previous pulse assumption, data fitting analysis and time-resolved measurement of PESs. The temporal measurement range is half of a laser optical cycle.     

Magnetic polaron-related optical properties in Ni(Ⅱ)-doped Cd S nanobelts: Implication for spin nanophotonic devices

Emissions by magnetic polarons and spin-coupled d-d transitions in diluted magnetic semiconductors(DMSs)have become a popular research field due to their unusual optical behaviors.In this work,high-quality NiI₂(Ⅱ)-doped CdS nanobelts are synthesized via chemical vapor deposition(CVD),and then characterized by scanning electron microscopy(SEM),x-ray diffraction,x-ray photoelectron spectroscopy(XPS),and Raman scattering.At low temperatures,the photoluminescence(PL)spectra of the Ni-doped nanobelts demonstrate three peaks near the band edge:the free exciton(FX)peak,the exciton magnetic polaron(EMP)peak out of ferromagnetically coupled spins coupled with FXs,and a small higher-energy peak from the interaction of antiferromagnetic coupled Ni pairs and FXs,called antiferromagnetic magnetic polarons(AMPs).With a higher Ni doping concentration,in addition to the d-d transitions of single Ni ions at 620 nm and 760 nm,two other PL peaks appear at 530 nm and 685 nm,attributed to another EMP emission and the d-d transitions of the antiferromagnetic coupled Ni²⁺-Ni²⁺pair,respectively.Furthermore,single-mode lasing at the first EMP is excited by a femtosecond laser pulse,proving a coherent bosonic lasing of the EMP condensate out of complicated states.These results show that the coupled spins play an important role in forming magnetic polaron and implementing related optical responses.     

Laser-phase determination methods and transfer equations for direct temporal structure measure- ments of atto- and femtosecond XUV pulses

In this paper the laser-phase determination methods and transfer equations are presented to directly reconstruct the detailed temporal structures of ultra-short extreme ultraviolet (xuv) pulses from the measured photoelectron energy spectra (PES). Each transfer equation includes one of PID (proportional-integral-differential) terms of PES. The intensity and instantaneous frequency of attosecond xuv can be retrieved from the integral term of PES. The intensity profiles of narrow bandwidth atto- and femtosecond xuvs can be rebuilt from the proportional and differential terms of PES respectively. The methods and equations may be used to improve time resolutions in measuring ultrashort pulses.     

Sub-wavelength surface structuring of NiTi alloy by femtosecond laser pulses

Generation of self-organized sub-wavelength surface structures on a nickel–titanium alloy plate by femtosecond laser pulses is investigated experimentally through line-scribing experiments in air. It is found that Bragg-like relief gratings, with the orientation perpendicular to the laser polarization, are formed over the entire laser-scribed regions. The average period is measured as 630±30 nm. Distinctive features of these novel surface structures include nanoparticle-covered grating ridges and the maintainable spatial period regardless of incidence angles. With different laser parameters and sample scan speeds, sub-wavelength grating structures can evolve into cellular-like nanotextures. Optimal conditions for forming these surface structures are determined in terms of laser energy and scan speed. Elementary analyses of the structured surfaces by X-ray diffraction and photoelectron spectroscopy reveal that both the crystal structures and the chemical elements can remain in their original states, but the surface grains are refined and the atomic percentages are varied after femtosecond laser treatments.     

利用单飞秒激光脉冲驱动类氖钛X射线激光的研究

提出了一种利用单飞秒激光脉冲驱动类氖钛X射线激光的物理方案.利用自相似方法研究了不同脉冲前沿的单飞秒激光辐照钛平板靶产生的类氖钛X射线激光等离子体的特性,得到了电子温度、电子密度和定标长度三者的定标律,讨论了给定输入参数下各定标律曲线的特性.研究表明,利用单个飞秒激光能够实现X射线激光的产生,而且脉冲前沿强度随时间增长平缓的飞秒激光有利于驱动X射线激光.本研究为实验上实现单飞秒激光脉冲驱动X射线激光提供了一种新的方案.     

Li2分子含时波包动力学的理论研究

利用含时量子波包方法计算得到了Li2分子的光电子能谱,并运用波包动力学理论对含有不同参量的光电子能谱现象给出了合理的解释.通过分析文中的直观图像,研究了波包的动力学过程.结果表明,泵浦-探测脉冲的延迟时间对光电子能谱的形状有重要的影响;在较短延迟时间下,能谱独特的四峰现象是由光诱导势的产生引起的.     

Li2分子含时波包动力学的理论研究

利用含时量子波包方法计算得到了Li2分子的光电子能谱,并运用波包动力学理论对含有不同参量的光电子能谱现象给出了合理的解释。通过分析文中的直观图像,研究了波包的动力学过程。结果表明,泵浦-探测脉冲的延迟时间对光电子能谱的形状有重要的影响;在较短延迟时间下,能谱独特的四峰现象是由光诱导势的产生引起的。     

Soft X-ray ARPES and Fermiology of strongly correlated electron systems and PES by hard X-ray and extremely low energy photons

Bulk sensitivity is inevitable for photoelectron spectroscopy (PES) when one studies bulk electronic structures of strongly correlated electron systems, which are often much different from surface electronic structures. Combination of soft and hard X-ray PES (SXPES and HAXPES) is a promising approach for this purpose by quantitatively evaluating the contribution of the surface in the observed angle integrated PES spectra. Even in the angle resolved PES studies (ARPES), the bulk sensitivity of the SX-ARPES is required to get the real bulk band dispersions and Fermi surface topology, which may be noticeably modified in the surface region as seen in several materials studied in this paper.Although hard X-ray ARPES is feasible, deep attention is required for the discussion of the possible recoil effects for the valence band. Besides, extremely low energy PES (ELEPES) by use of microwave excited Xe, Kr and Ar lamps will be as useful as those by synchrotron radiation and laser to realize a very high resolution of better than 5 meV with bulk sensitivity under certain conditions.     

Fabrication of 3D microfluidic structures inside glass by femtosecond laser micromachining

Femtosecond lasers have opened up new avenues in materials processing due to their unique characteristics of ultrashort pulse widths and extremely high peak intensities. One of the most important features of femtosecond laser processing is that a femtosecond laser beam can induce strong absorption in even transparent materials due to nonlinear multiphoton absorption. This makes it possible to directly create three-dimensional (3D) microfluidic structures in glass that are of great use for fabrication of biochips. For fabrication of the 3D microfluidic structures, two technical approaches are being attempted. One of them employs femtosecond laser-induced internal modification of glass followed by wet chemical etching using an acid solution (Femtosecond laser-assisted wet chemical etching), while the other one performs femtosecond laser 3D ablation of the glass in distilled water (liquid-assisted femtosecond laser drilling). This paper provides a review on these two techniques for fabrication of 3D micro and nanofluidic structures in glass based on our development and experimental results.     

Generation of a directed nanolocalized photoelectron beam by means of femtosecond laser pulses

A directed photoelectron beam is obtained when photoelectrons from a sharp metal tip irradiated by femtosecond laser pulses are passed through a quartz nanocapillary. Such a nanolocalized photoelectron train makes it possible to conduct experiments with simultaneous femtosecond time and nanometer spatial resolutions.     

NaLi分子飞秒含时光电子能谱的理论研究

运用三态模型和含时波包方法,研究了NaLi分子处于强飞秒抽运-探测激光场中的波包动力学过程和时间分辨光电子能谱,并且揭示了飞秒激光脉冲参数与NaLi分子光电子能谱之间的关系.研究发现:对于不同的激光波长,波包的振动周期是不同的,而且随着抽运-探测脉冲延迟时间的不同,NaLi分子光电子能谱的谱峰高度和位置发生变化;当λ1=352 nm并且?t=400 fs时,外阱中相应的光电离信号(0.5 eV处)明显强于内阱中相应的光电离信号(1.35 eV处).计算结果表明,NaLi分子激发态41Σ+上波包动力学的一些信息能够通过其光电子能谱反映出来.这些结果可以为实验上实现分子的光控制以及量子操控过程提供一些有价值的参考信息,并为进一步的理论研究提供重要依据.     

Spatial chemical inhomogeneity and local electronic structure of Mn-doped Ge ferromagnetic semiconductors

We have investigated the chemical distributions and the local electronic structure of potential diluted magnetic semiconductor Ge0.94Mn0.06 single crystals using scanning photoelectron microscopy (SPEM), x-ray absorption spectroscopy (XAS), and photoemission spectroscopy (PES). The SPEM image shows the stripe-shaped microstructures, which arise from the chemical phase separation between the Mn-rich and Mn-depleted phases. The Mn 2p XAS shows that the Mn ions in the Mn-rich region are in the divalent high-spin Mn2+ states but that they do not form metallic Mn clusters. The Mn 3d PES spectrum exhibits a peak centered at approximately 4 eV below E(F) and the negligible spectral weight near E(F). This study suggests that the observed ferromagnetism in Ge1-xMnx arises from the phase-separated Mn-rich phase.     

铁磁薄膜中圆偏振光感应的瞬态磁光Kerr峰的物理起源

使用飞秒时间分辨抽运-探测磁光Kerr光谱技术,实验研究了圆偏振光抽运面内磁化FePt和垂直磁化GdFeCo薄膜的磁化演化动力学,发现在时间延迟零点处均出现瞬态Kerr峰.分析了此Kerr峰的起源,指出此瞬态Kerr峰与铁磁性无关,可能起源于自由电子的顺磁磁化,而顺磁磁化的外磁场来自圆偏振抽运光的逆Faraday效应.基于顺磁磁化模型的计算结果支持此观点.基于此观点,逆Faraday效应感应的磁场脉冲宽度应该与激光脉冲宽度一致.     

Fabrication of Micro -Optical Devices by a Femtosecond Laser

Femtosecond laser is a perfect laser source for materials processing when high accuracy and small structure size are required. Due to the ultra short interaction time and the high peak power, the process is generally characterized by the absence of heat diffusion and, consequently molten layers. Various induced structures have been observed in materials after the femtosecond laser irradiation. Here, we report on fabrication of micro-optical devices by the femtosecond laser. 1) formation of optical waveguide with internal loss less than 0.5dB/cm in the wavelength region from 1.2 to 1.6 mm, by translating a silica glass perpendicular to the axis of the focused femtosecond laser beam; 2) nano-scale valence state manipulation of active ions inside transparent materials; 3) space-selective precipitation and control of metal nanoparticles inside transparent materials; The mechanisms and applications of the femtosecond laser induced phenomena were also discussed.     

Circular dichroism in laser-assisted short-pulse photoionization

A remarkable effect of circular dichroism, i.e., a difference in photoelectron spectra produced by right and left circularly polarized light in two-color multiphoton ionization of atoms, is predicted for the case when the atom is ionized by an extreme ultraviolet or x-ray femtosecond pulse in the field of a strong infrared laser pulse, both pulses being circularly polarized. We show that the sidebands formed in the spectra exhibit different circular dichroism often of different signs both in angle-resolved and angle-integrated experimental conditions. The effect can be used for detecting and measuring circular polarization of x rays in a spectral range where other methods are not effective.     

T-shaped gate AlGaN/GaN HEMTs fabricated by femtosecond laser lithography without ablation

Femtosecond laser as a maskless lithography technique is able to fabricate structures far smaller than the diffraction limit to a value within sub-micrometer resolution. We present the femtosecond laser lithography without ablation on the positive photoresist is applied in fabricating T-shaped gate AlGaN/GaN HEMT. The feature sizes of femtosecond laser lithography were determined by the incident laser power, the scan speed of the laser focus, the number of scan times, and the substrate materials. T-shaped gate with the smallest gate length 204?nm could be fabricated by dielectric-defined process using femtosecond laser lithography. The fabricated AlGaN/GaN HEMT with 380?nm T-gate exhibits a maximum drain current density of 500?mA/mm and a maximum peak extrinsic transconductance of 173?mS/mm.     

Angular-resolved photoelectron spectroscopy of superatom orbitals of fullerenes

Photoelectron angular distributions from both C(60) and C(70) were recorded for low laser intensity femtosecond and picosecond pulses. Rich structure is seen for electron kinetic energies that lie below the photon energy. Strong, broad peaks are observed for photoelectron energies corresponding to single-photon ionization of so-called superatom molecular orbitals (SAMOs). The very simple angular distributions measured for these peaks, the close similarity of the spectra observed from C(60) and C(70), and the comparison with time-dependent density functional theory provide strong support for the SAMO hypothesis.     

Many-body effect in the coincidence L3 and M3 photoelectron spectroscopy spectra of Cu metal

The coincidence L₃ and M₃ photoelectron spectroscopy (PES) main lines of Cu metal are calculated by a many-body theory. There is no peak-energy shift between the singles PES main line and the coincidence one. The asymmetric narrowing of the coincidence PES main line on the low kinetic energy (KE) side is very small. This is in accord with recent experimental findings. In Cu metal, the shakeup satellite intensity is small and the main-line satellite separation energy is much larger than the core–hole lifetime width. The interference via the final-state interaction is negligible. In the PES main line, the imaginary part of the self-energy by shakeup excitations, which is very small compared to the core–hole lifetime width, decreases very slowly in linear with photoelectron KE. The branching ratio of Auger decay of a single hole state then increases very slowly in linear with photoelectron KE so that the deviation of the coincidence PES main line from the singles one is very small. The 939 eV structure seen only in the coincidence L₃ PES spectrum of Cu metal is attributed to the enhancement of the inelastic peak of a smaller energy loss due to electrons of a smaller average emission depth measured in coincidence with the elastic Auger peak. The structure will not be enhanced in the singles PES spectrum. The background subtraction in the coincidence spectrum cannot be the same as that in the singles one. Such consideration is necessary before we can conclude about the asymmetric narrowing on the low KE side. A unique capability of APECS by which one can determine the photoelectron KE dependent part of the imaginary part of the self-energy is pointed out.