Attosecond spectroscopy for filming the ultrafast movies of atoms,molecules and solids

Three decades ago, a highly nonlinear nonpertubative phenomenon, now well-known as the high harmonic generation (HHG), was discovered when intense laser irradiates gaseous atoms. As the HHG produces broadband coherent radiation, it becomes the most promising source to obtain attosecond pulses. The door to the attosecond science was opened ever since. In this review, we will revisit the incredible adventure to the attoworld. Firstly, the progress of attosecond pulse generation is outlined. Then, we introduce the efforts on imaging the structures or filming the ultrafast dynamics of nuclei and electrons with unprecedented attosecond temporal and Angstrom spatial resolutions, utilizing the obtained attosecond pulses as well as the high harmonic spectrum itself.     

双色光场驱动产生单个阿秒脉冲过程中的宏观效应

通过数值模拟三维传播方程研究了双色场产生高次谐波过程中宏观效应的影响,重点分析了阿秒脉冲的时域形状.在6 fs/800 nm和21.3 fs/400 nm组成的双色场中,通过调节双色场间的相对延时,双色场各焦点相对于气体盒子入口的间距和双色场束腰半径和气体压强等参数,可以在平台区得到超宽带连续谱.对该连续谱中420—540 eV的谐波直接进行滤波后可以得到时间同步性很好的单个阿秒脉冲.这种性质对实验上通过双色场方案产生超短的阿秒脉冲非常有利. 关键词： 传播效应 阿秒脉冲 时间同步性     

Numerical characterization of high harmonic attosecond pulses

A numerical simulation of attosecond harmonic pulse generation in a three-dimensional field-ionizing gas is presented. Calculated harmonic efficiencies quantitatively reproduce experimental findings. This allows a quantitative characterization of attosecond pulse generation revealing information currently not accessible by experiment. The rapid phase variation and spatiotemporal distortions of harmonics are smaller than anticipated, allowing focusing of 30-nm, 750-as pulses to intensities in excess of 10(13) W/cm(2). Feasibility of such pulses brings novel applications such as extreme ultraviolet nonlinear optics and attosecond pump probe spectroscopy within reach.     

阿秒脉冲测量的研究进展

对于发生在原子范围内的电子动力学过程的观测需要阿秒量级的时间分辨率.理论和实验研究都已证明,用周期量级超短脉冲直接泵浦的高次谐波过程可以产生阿秒脉冲序列甚至单个的阿秒脉冲,将阿秒脉冲用于测量超快动力学过程之前先要对阿秒脉冲本身性质做出描述,传统的自相关方法和互相关方法不能直接推广到阿秒量级超短脉冲的测量.文章详细介绍了近几年发展起来的阿秒脉冲测量方法,分析了它们的分辨极限和局限性.     

Polarization state of high-order harmonic emission from aligned molecules

High harmonic emission in isotropic gases is polarized in the same direction as the incident laser polarization. Laser-induced molecular alignment allows us to break the symmetry of the gas medium. By using aligned molecules in high harmonic generation experiments, we show that the polarization of the extreme ultraviolet emission depends strongly on the molecular alignment and the orbital structure. Polarization measurements give insight into the molecular orbital symmetry. Furthermore, molecular alignment will allow us to produce attosecond pulses with time-dependent polarization.     

Double optical gating of high-order harmonic generation with carrier-envelope phase stabilized lasers

We demonstrated a novel optical switch to control the high-order harmonic generation process so that single attosecond pulses can be generated with multiple-cycle pulses. The technique combines two powerful optical gating methods: polarization gating and two-color gating. An extreme ultraviolet supercontinuum supporting 130 as was generated with neon gas using 9 fs laser pulses. We discovered a unique dependence of the harmonic spectra on the carrier-envelope phase of the laser fields, which repeats every 2 pi radians.     

Self-referencing, spectrally, or spatially encoded spectral interferometry for the complete characterization of attosecond electromagnetic pulses

We propose a method for the complete characterization of attosecond duration electromagnetic pulses produced by high harmonic generation in an atomic gas. Our method is based on self-referencing spectral interferometry of two spectrally sheared extreme ultraviolet pulses, which is achieved by pumping the harmonic source with two sheared optical driving pulses. The resulting interferogram contains sufficient information to completely reconstruct the temporal behavior of the electric field. We demonstrate that such a method is feasible, and outline two possible experimental configurations.     

Effects of pressure and gas-jet thickness on the generation of attosecond pulse

We investigate how the intensity and duration of an attosecond pulse generated from high-order harmonic generation are affected by the pressure and thickness of the gas jet by taking into account the macroscopic propagation of both fundamental and harmonic fields. Our simulations show that, limited by the propagation effects, especially the absorption of harmonics, the intensity of an attosecond pulse cannot be improved by just independently increasing the gas pressure or the medium length. On the other hand, due to good phase-matching conditions, the duration of a generated attosecond pulse can be improved by changing the gas pressure.     

Generation of attosecond pulses in a system with permanent dipole moment

The generation of attosecond pulses in a two-level system with permanent dipole moment is investigated. It is shown due to the presence of permanent dipole moments, that the plateau of the high-order harmonic generation spectrum can be extended to X-ray range. Moreover, attosecond pulses with higher intensity can be synthesized by using both even and odd harmonics because of their quantum interference.     

Amplitude and phase control of attosecond light pulses

We report the generation, compression, and delivery on target of ultrashort extreme-ultraviolet light pulses using external amplitude and phase control. Broadband harmonic radiation is first generated by focusing an infrared laser with a carefully chosen intensity into a gas cell containing argon atoms. The emitted light then goes through a hard aperture and a thin aluminum filter that selects a 30-eV bandwidth around a 30-eV photon energy and synchronizes all of the components, thereby enabling the formation of a train of almost Fourier-transform-limited single-cycle 170 attosecond pulses. Our experiment demonstrates a practical method for synthesizing and controlling attosecond waveforms.     

圆偏振激光附加太赫兹场作用下的高次谐波发射和孤立阿秒脉冲的产生

本文通过数值求解二维含时薛定谔方程,研究了圆偏振激光和太赫兹组合场作用下,H+2的高次谐波发射和孤立阿秒(1 as=10-18s)脉冲的产生.研究发现,无论在圆偏振激光场的x或y方向附加一个太赫兹场,都可以产生一个比较平滑的连续谐波谱.通过时频分析我们发现,高次谐波的贡献主要来自于短轨道.适当选取一些级次的连续谐波进行叠加,可以得到129 as或83 as的孤立阿秒脉冲.     

圆偏振激光附加太赫兹场作用下的高次谐波发射和孤立阿秒脉冲的产生

本文通过数值求解二维含时薛定谔方程,研究了圆偏振激光和太赫兹组合场作用下,H2+的高次谐波发射和孤立阿秒脉冲的产生。研究发现,无论在圆偏振激光场的 或 方向附加一个太赫兹场,都可以产生一个比较平滑的连续谐波谱。通过时频分析我们发现,高次谐波的贡献主要来自于短轨道。适当选取一些级次的连续谐波进行叠加,可以得到129 as或83 as的孤立阿秒脉冲。     

Control mechanism of atomic ionization and high-order harmonic generation assisted by attosecond pulses

Attosecond pulses combined with infrared laser constitute a powerful tool for controlling atomic photoionization and high-order harmonic generation (HHG). We apply the intense-field many-body S-matrix theory to solve such two-pulse excitation problems. The theory can give a clear explanation for the oscillation of ionization probability as a function of time delay between infrared field and attosecond pulses with central frequency lying below ionization threshold at moderate infrared intensities. The HHG assisted by such attosecond pulses is also interpreted. In addition to a known dramatic enhancement of HHG, a harmonic emission from rapid oscillation of bound-state population caused by the counter-rotating wave is presented.     

Destructive interference during high harmonic generation in mixed gases

We report on the first experimental evidence of the destructive and constructive interference of high harmonics generated in a mixed gas of He and Ne, which facilitates the coherent control of high harmonic generation. Theoretically, we develop an analytical model of high harmonic generation in mixed gases and succeed in reproducing the experimental results and deriving the optimization conditions for the process. The observed interference modulation is attributed to the difference between the phases of the intrinsically chirped harmonic pulses from He and Ne, which leads to a novel method for broadband measurement of the harmonic phases and for observing the underlying attosecond electron dynamics.     

High order harmonic generation from solid targets: Towards intense attosecond pulses

Experiments and computer simulations on high order harmonic generation (HOHG) from steep plasma gradients using intense femtosecond laser pulses are presented. The importance of the plasma scale length for the efficiency of HOHG is demonstrated. By changing the pump intensity and the target parameters the regime of HOHG can be switched from non-relativistic to relativistic. Simulations show that attosecond pulses should already be present in our experiments in both interaction regimes. Two-color driven harmonic generation is shown to provide a highly efficient way of attosecond pulse production.     

线偏振激光场中分子高次谐波椭偏率的调控

高次谐波椭偏率的调控为人们研究磁性材料和手性介质中的超快动力学过程提供了有效途径.本文理论研究了线偏振激光脉冲驱动下,H₂~+和H₃²⁺分子高次谐波的偏振特性及阿秒脉冲产生.结果表明当取向角为0~o时,H₂~+分子谐波的椭偏率几乎为0,而H₃²⁺分子谐波具有较大椭偏率,这是由于分子轨道对称性决定的.通过改变取向角的大小,可以调控高次谐波强度以及谐波椭偏率大小,为产生椭偏XUV脉冲提供了手段.同时,发现椭偏率较大的谐波阶次对应的谐波强度较小,分析表明分子的双中心干涉效应对椭偏率有很大的影响.对于H₂~+和H₃²⁺分子,分别合成了椭偏率为0.75和0.55的椭圆偏振阿秒脉冲.这种大椭偏XUV脉冲的产生为高次谐波在材料与生物科学领域提供了重要应用.     

不同激光等离子体条件下的阿秒光脉冲产生

通过一维粒子模拟研究了利用相对论少周期强激光与固体密度等离子体表面相互作用实现单个孤立阿秒光脉冲产生的参数条件。主要研究描述相互作用的多维参数,如激光强度、入射角和等离子体标尺长度等,对相对论高次谐波能量转换效率和孤立阿秒光脉冲分离度的影响。研究发现,虽然激光等离子体参数对阿秒光脉冲产生的影响是复杂的,但是存在着能够实现大能量孤立阿秒光脉冲的最佳等离子体标尺长度和最佳入射角。当其他相互作用条件确定时,使用中等强度的相对论强激光可以在较宽的参数范围内实现孤立的阿秒光脉冲。大角度入射时,孤立阿秒光脉冲的分离度较高,能够实现孤立阿秒光脉冲的相互作用参数范围也较宽。     

利用三束中红外空间非均匀激光场产生超长平台区

数值研究了氦离子在三束中红外激光场下发射高次谐波以及阿秒脉冲的特点. 计算结果表明, 通过适当调节三束激光场的延迟时间和相位角, 不仅谐波发射的截止能量得到了延伸, 而且单一的量子路径也被选择出来对谐波发射起作用, 随后通过适当的引入空间非均匀参数,谐波截止能量得到了进一步扩展,形成了一个超长的1773eV的平台区. 并且我们发现当选择氦离子的基态和第一激发态为叠加初始态时,谐波的强度被增强了4-6个数量级. 最后, 通过叠加谐波谱上的谐波, 可获得一系列脉宽为32as左右的阿秒X射线光源. 并且这些光源的强度比氦离子基态作为初始态时增强了4-6个数量级.     

利用三束中红外空间非均匀激光场产生超长平台区

数值研究了氦离子在三束中红外激光场下发射高次谐波以及阿秒脉冲的特点. 计算结果表明, 通过适当调节三束激光场的延迟时间和相位角, 不仅谐波发射的截止能量得到了延伸, 而且单一的量子路径也被选择出来对谐波发射起作用, 随后通过适当的引入空间非均匀参数,谐波截止能量得到了进一步扩展,形成了一个超长的1773eV的平台区. 并且我们发现当选择氦离子的基态和第一激发态为叠加初始态时,谐波的强度被增强了4-6个数量级. 最后, 通过叠加谐波谱上的谐波, 可获得一系列脉宽为32as左右的阿秒X射线光源. 并且这些光源的强度比氦离子基态作为初始态时增强了4-6个数量级.     

Circularly polarised attosecond pulses: generation and applications

ABSTRACT

Molecular high-order harmonic generation(MHOHG) is simulated for H⁺₂ in the nonlinear nonperturbative regime of laser-molecule interactions with ultrashort intense circularly polarised laser pulses. It is shown that combinations of co-rotating or counter-rotating pulses produce laser-induced Coriolis forces with electron-parent ion recollisions, thus enhancing circularly polarised MHOHG, the source of circularly polarised attosecond pulses. Such pulses can be used to induce electron attosecond currents for the generation of attosecond magnetic field pulses, new tools for molecular attomagnetism.