高次谐波产生阿秒极紫外和X光脉冲研究新进展

 近年来在可见光谱范围内已经把激光脉冲压缩到接近一个光学周期(2～3 fs)的物理极限,几fs的时间分辨精度可以描述分子化学反应过程,但是要探测远小于可见光周期的电子跃迁过程则需要阿秒(as)量级的光脉冲。利用脉冲间具有相同载波包络相位的阿秒脉冲序列能把可见光波段的光学频率梳向极紫外波段扩展;利用电子和离子碰撞复合过程短于一个光周期这个时间窗,通过测量激光场椭圆极化率对电子轨迹的微扰实现了as精度的分辨率;通过测量碰撞复合过程中的高能电子的辐射谱可以重构阿秒X光脉冲以及探测强场下束缚态和连续态电子动力学。     

Attosecond resolved charging of ions in a rare-gas cluster

A scheme to probe dissipative multielectron motion in time is introduced. In this context attosecond probing enables one to obtain information which is lost at later times and cannot be retrieved by conventional methods in the energy domain due to the incoherent nature of the dynamics. As a specific example we will trace the transient charging of ions in a rare-gas cluster during a strong femtosecond vacuum-ultraviolet pulse by means of delayed attosecond pulses.     

Magneto optics and time resolved terahertz spectrocopy

Exploring, manipulating, and understanding new exotic quantum phenomena in condensed-matter systems have generated great interest in the scientific community. Static and time resolved optical spectroscopies after photoexcitations are important experimental tools for probing charge dynamics and quasiparticle excitations in quantum materials. In Synergetic Extreme Condition User Facility(SECUF), we shall construct magneto-infrared and terahertz measurement systems and develop a number of ultrafast femtosecond laser based systems, including intense near to mid-infrared pump terahertz probe. In this article, we shall describe several systems to be constructed and developed in the facilities, then present some examples explaining the application of magneto optics and time resolved spectroscopy techniques.     

Nanoscopic ultrafast space-time-resolved spectroscopy

We propose and analyze a scheme for ultrafast spectroscopy with nanometer spatial and femtosecond temporal resolution. The interaction of polarization-shaped laser pulses with a nanostructure allows us to control the spatial and temporal evolution of the optical near field. Employing a learning algorithm, the field is tailored such that pump and probe excitation occur at different positions and at different times. Both excitations can be restricted to subdiffraction extensions and are separable on a nanometer length scale. This enables the direct spatial probing of nanoscale energy transfer or charge transfer processes.     

Characterization of high-order harmonic radiation on femtosecond and attosecond time scales

We characterize the temporal structure of high-order harmonic radiation on both the femtosecond and attosecond time scales. The harmonic emission is characterized by mixed-color two-photon ionization with an infrared femtosecond laser using a Mach–Zehnder interferometer where both pump and probe arms travel completely separate paths. In a first experiment, we measure the duration and chirp of individual harmonics. In a second experiment, we resolve, for the first time with this type of setup, the attosecond beating of several harmonics generated under conditions similar to the first experiment. We suggest that the results of both measurements can be combined to determine the full attosecond time structure of the harmonic emission. PACS 32.80.Rm; 42.65.Ky     

稀土材料的超快共振非线性光学特性研究

用抽运-探测技术测量光学响应材料非线性极化率的方法，研究了稀土材料非线性折射率的共振增强和超快响应的非线性动力学过程。测得钕玻璃的三阶非线性折射 率强度系数为10^-14cm^2/W，比其基质的非线性折射率强度系数提高了2个量级。用该方法研究了Nd:YVO4、Er:YAG等晶体的超快非线性响应过程。实验结果与理论分析表明，抽支-探测技术是测量非线性极化率的简单而又灵敏的方法。这一测量技术对研究与开发超高速光响应器件具有重要的实用价值。     

Ultrafast femtosecond all-optical modulation through nondegenerate two-photon absorption in silicon-on-insulator waveguides

We present numerical investigations of ultrafast femtosecond (with time duration of 100 fs at 1/e intensity point) all-optical modulation of a pump-probe wave arrangement by using nondegenerate two-photon absorption (TPA), namely cross absorption, inside silicon-on-insulator (SOI) optical waveguides. Our results show that when a pump pulse with femtosecond duration and a continuous probe wave are co-propagating along the SOI, the probe wave can be modulated inversely by the ultrafast pump pulse, whose modulation depth depends strongly on the system parameters such as the waveguide length, the peak power and initial chirp of the pump wave, the group velocity dispersion (GVD), etc.; this means that the modulation depth can be improved by an appropriate increase of the waveguide length, the pump peak, and the initial chirp, in addition, which has a larger value for the probe wavelength in the normal dispersion regime compared with the case of abnormal dispersion when the center wavelength of the pump wave is located at the zero-dispersion wavelength.     

Ultra‐fast nano‐optics

Ultra‐fast nano‐optics is a comparatively young and rapidly growing field of research aiming at probing, manipulating and controlling ultrafast optical excitations on nanometer length scales. This ability to control light on nanometric length and femtosecond time scales opens up exciting possibilities for probing dynamic processes in nanostructures in real time and space. This article gives a brief introduction into the emerging research field of ultrafast nano‐optics and discusses recent progress made in it. A particular emphasis is laid on the recent experimental work performed in the authors' laboratories. We specifically discuss how ultrafast nano‐optical techniques can be used to probe and manipulate coherent optical excitations in individual and dipole‐coupled pairs of quantum dots, probe the dynamics of surface plasmon polariton excitations in metallic nanostructures, generate novel nanometer‐sized ultrafast light and electron sources and reveal the dipole interaction between excitons and surface plasmon polaritons in hybrid metal‐semiconductor nanostructures. Our results indicate that such hybrid nanostructures carry significant potential for realizing novel nano‐optical devices such as ultrafast nano‐optical switches as well as surface plasmon polariton amplifiers and lasers.     

飞秒时间分辨实验中相关函数和时间零点的确定

结合飞秒激光在研究分子激发态弛豫动力学中的应用,介绍了几种飞秒时间分辨实验中确定泵浦激光脉冲与探测激光脉冲的相关函数和时间零点的方法.对于波长在可见波段的泵浦和探测激光脉冲,我们可以利用非线性光学的技术手段,探测泵浦光与探测光的和频光的强度随二者间的时间延迟的变化来确定相关函数和时间零点;对于波长在紫外甚至更短的波段的泵浦和探测激光脉冲,由于单脉冲能量比较低,目前还很难利用技术手段来测定泵浦激光与探测激光的相关函数及时间零点,可以利用某些原子气体(如Xe)或某些具有短寿命态的分子作平行实验进行间接测量.     

基于阿秒XUV-飞秒IR泵浦-探测的冷靶反冲离子动量成像谱仪

利用多道可见光谱探测系统测量了Hα、CⅢ(464.7nm)和OⅡ(441.5nnm)谱线的时间行为,得出了碳、氢和氧元素的入射通量。在简化模型下算出了氧碳间的化学溅射率,结果表明HT-6M托卡马克边界杂质产生机制主要是氢氧间的化学溅射和氧碳间的化学溅射,因此控制氧杂质尤其重要。     

飞秒时间分辨实验中泵浦-探测交叉相关函数的测量和时间零点的确定

飞秒激光技术的出现使得实时探测与跟踪激发态超快弛豫动力学过程成为可能,并能够给出激发态动力学过程清晰的物理图像。而在飞秒时间分辨实验中,泵浦-探测相关函数和时间零点直接影响实验结果的可靠性和准确性。本文结合飞秒激光在分子激发态超快动力学过程中的应用进展,介绍了根据实验条件和要求,在具体实验过程中泵浦-探测相关函数测量和时间零点确定的几种方法。实验中选择可见光作为泵浦光和探测光时,可以通过测定随泵浦-探测时间延迟变化的泵浦激光与探测激光的和频/差频光强来确定泵浦探测交叉相关函数和时间零点;而选择中心波长在紫外甚至真空紫外的激光脉冲作为泵浦光或探测光时,泵浦-探测交叉相关函数通常采用校正的方法测量。     

利用三色组合脉冲激光获得孤立阿秒脉冲发射

孤立阿秒脉冲因可以跟踪和控制原子及分子内电子的运动过程而备受关注.本文从理论上开展了氦原子在3束飞秒脉冲激光组合场辐照下产生的高次谐波和阿秒脉冲辐射的研究.组合激光场由16 fs/1600 nm,15 fs/1100 nm和5.3 fs/800 nm的钛宝石脉冲构成.与前两束脉冲合成的双色场产生谐波谱相比,附加钛宝石脉冲的三色场产生的高次谐波发射谱呈现出高转换效率及宽带超连续特性,超连续谱范围覆盖从230—690次谐波,傅里叶变换后实现了128 as高强度孤立短脉冲的产生.该结果归因于合成的三色场呈现出高功率及少周期的中红外飞秒脉冲激光特性,可以有效控制原子电离以及复合发生在中红外飞秒脉冲的一个有效光学周期内.     

Attosecond lighthouses: how to use spatiotemporally coupled light fields to generate isolated attosecond pulses

Under the effect of even simple optical components, the spatial properties of femtosecond laser beams can vary over the duration of the light pulse. We show how using such spatiotemporally coupled light fields in high harmonic generation experiments (e.g., in gases or dense plasmas) enables the production of attosecond lighthouses, i.e., sources emitting a collection of angularly well-separated light beams, each consisting of an isolated attosecond pulse. This general effect opens the way to a new generation of light sources, particularly suitable for attosecond pump-probe experiments, and provides a new tool for ultrafast metrology, for instance, giving direct access to fluctuations of the carrier-envelope relative phase of even the most intense ultrashort lasers.     

Attosecond laser station

The attosecond laser station(ALS) at the Synergetic Extreme Condition User Facility(SECUF) is a sophisticated and user-friendly platform for the investigation of the electron dynamics in atoms, molecules, and condensed matter on timescales ranging from tens of femtoseconds to tens of attoseconds. Short and tunable coherent extreme-ultraviolet(XUV)light sources based on high-order harmonic generation in atomic gases are being developed to drive a variety of endstations for inspecting and controlling ultrafast electron dynamics in real time. The combination of such light sources and end-stations offers a route to investigate fundamental physical processes in atoms, molecules, and condensed matter. The ALS consists of four beamlines, each containing a light source designed specifically for application experiments that will be performed in its own end-station. The first beamline will produce broadband XUV light for attosecond photoelectron spectroscopy and attosecond transient absorption spectroscopy. It is also capable of performing attosecond streaking to characterize isolated attosecond pulses and will allow studies on the electron dynamics in atoms, moleculars, and condensed matter. The second XUV beamline will produce narrowband femtosecond XUV pulses for time-resolved and angle-resolved photoelectron spectroscopy, to study the electronic dynamics on the timescale of fundamental correlations and interactions in solids, especially in superconductors and topological insulators. The third beamline will produce broadband XUV pulses for attosecond coincidence spectroscopy in a cold-target recoil-ion momentum spectrometer, to study the ultrafast dynamics and reactions in atomic and molecular systems. The last beamline produces broadband attosecond XUV pulses designed for time-resolved photoemission electron microscopy, to study the ultrafast dynamics of plasmons in nanostructures and the surfaces of solid materials with high temporal and spatial resolutions simultaneously. The main object of the ALS is to provide domestic and international scientists with unique tools to study fundamental processes in physics, chemistry,biology, and material sciences with ultrafast temporal resolutions on the atomic scale.     

超快X射线自由电子激光研究进展北大核心CSCD

现代光源的发展不断推动着人们从更深层次上理解物质的基本结构和动力学行为。X射线自由电子激光作为最先进的光源,其超高的峰值功率、超短的脉冲长度和优良的相干性,为人们以原子级时空分辨率探测和操控物质中的超快过程提供了可能。目前全世界已有多个X射线自由电子激光装置建成并投入使用,在原子分子物理、化学、生命科学、材料科学等各学科应用中都显示出了重要价值。同时大量的研究工作也集中于继续提高X射线自由电子激光的性能,包括把脉冲持续时间从fs量级进一步缩短至as量级,这将为超快科学的发展带来新突破。以超快脉冲产生为主线,综述了近年来超快X射线自由电子激光产生方案的研究进展,从产生原理、方案特性、最新成果等方面介绍了各类产生方案,总结对比了各方案的优缺点,最后对超快X射线自由电子激光的未来发展方向进行了展望。     

All-optical tunable photonic bandgap microcavities with a femtosecond time response

An all-optical tunable photonic bandgap microcavity made from a two-dimensional polystyrene photonic crystal is fabricated by focused ion beam etching. The pump and probe scheme is adopted to measure tunability based on the femtosecond optical Kerr effect. An ultrafast response time of less than 120 fs is achieved for the tunable photonic bandgap microcavity. The microcavity resonant wavelength shifts 3.1 nm under excitation of 9.4 GW/cm2 pump intensity, which is in agreement with the theoretical prediction.     

Optical second harmonic generation and its photoinduced dynamics in ferroelectric semiconductor Sn<Subscript>2</Subscript>P<Subscript>2</Subscript>S<Subscript>6</Subscript>

By means of optical pump–probe technique, the ultrafast dynamics of nonlinear optical response of the ferroelectric semiconductor Sn₂P₂S₆ crystal excited with a femtosecond laser pulse has been investigated. It has been shown that, under the action of femtosecond pulses, change in optical second harmonic generation occurs in the sample, which can be due to screening of existing electric polarization.     

Amplitude and phase reconstruction of electron wave packets for probing ultrafast photoionization dynamics

Ultrafast atomic processes, such as excitation and ionization occurring on the femtosecond or shorter time scale, were explored by employing attosecond high-harmonic pulses. With the absorption of a suitable high-harmonic photon a He atom was ionized, or resonantly excited with further ionization by absorbing a number of infrared photons. The electron wave packets liberated by the two processes generated an interference containing the information on ultrafast atomic dynamics. The attosecond electron wave packet, including the phase, from the ground state was reconstructed first and, subsequently, that from the 1s3p state was retrieved by applying the holographic technique to the photoelectron spectra comprising the interference between the two ionization paths. The reconstructed electron wave packet revealed details of the ultrafast photoionization dynamics, such as the instantaneous two-photon ionization rate.     

Femtosecond response from two copolymers with intense two-photon absorption

Under excitation of femtosecond laser pulses at 800 nm, intense two-photon absorption induced fluorescence was observed from two copolymers, linear structure copolymer M2 and tri-branched copolymer M3. In a one-color pump–probe experiment at 800 nm, an ultrafast transient absorption was observed, which was mainly from the simultaneous absorption of the one photon from the pump beam and another photon from the probe beam. This analysis was further confirmed by a two-color pump–probe measurement with a pump at 800 nm and a probe at 556 nm, respectively. The other two decaying processes in transient absorption have a lifetime of about 14 and 126 ps, which reflects the intraband relaxation and the decay of the excited state via intersystem crossing or the solvation effect, respectively.     

Ablation and ultrafast dynamics of zinc selenide under femtosecond laser irradiation

The ablation in zinc selenide (ZnSe) crystal is studied by using 150-fs, 800-nm laser system. The images of the ablation pit measured by scanning electronic microscope (SEM) show no thermal stress and melting dynamics. The threshold fluence is measured to be 0.7 J/cm2. The ultrafast ablation dynamics is studied by using pump and probe method. The result suggests that optical breakdown and ultrafast melting take place in ZnSe irradiated under femtosecond laser pulses.