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。     

Manifestation of attosecond XUV fields temporal structures in attosecond streaking spectrogram

The features of an attosecond extreme ultraviolet (XUV) field are encoded in the attosecond XUV spectrogram. We investigate the effect of the temporal structures of attosecond XUV fields on the attosecond streaking spectrogram. Factors such as the number of attosecond XUV pulses and the temporal chirp of attosecond XUV pulses are considered. Results indicate that unlike the attosecond streaking spectrogram for an attosecond XUV field with two pulses of a half-cycle separation of streaking field, the spectrogram for the attosecond XUV field with three pulses demonstrates fine spectral fringes in separated traces.     

Attosecond pulse trains generated using two color laser fields

We investigate the spectral and temporal structure of high harmonic emission from argon exposed to an infrared laser field and its second harmonic. For a wide range of generating conditions, trains of attosecond pulses with only one pulse per infrared cycle are generated. The synchronization necessary for producing such trains ensures that they have a stable pulse-to-pulse carrier envelope phase, unlike trains generated from one color fields, which have two pulses per cycle and a pi phase shift between consecutive pulses. Our experiment extends the generation of phase stabilized few cycle pulses to the extreme ultraviolet regime.     

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.     

红外激光场中共振结构原子对极紫外光脉冲的压缩效应

通过数值求解一维原子的含时薛定谔方程, 研究了具有共振结构的原子在双色场(红外激光(IR)+极紫外光(XUV)) 驱动下发射高次谐波的特征. 研究结果表明, 具有共振结构的原子所发射的高次谐波与无共振结构原子(简称为一般原子)发射的高次谐波有明显不同, 共振结构的原子除了在某一能量附近(原子的共振能量+电离能)高次谐波的强度有很大提高外, 它还对XUV光的响应较一般原子表现得更为敏感, 即使XUV光的强度较弱, 也能够明显提高XUV光脉冲中心频率附近的谐波强度, 更重要的是通过调节双色场的时间延迟, 能使输入的XUV光的脉宽得到明显的压缩, 通过时间-频率分析给出了发生这种现象的原因. 由此提出了通过滤波-连续反馈的方式可使XUV光的脉冲从200 as压缩至120 as左右.     

Subfemtosecond K-shell excitation with a few-cycle infrared laser field

Subfemtosecond bursts of extreme ultraviolet radiation, facilitated by a process known as high-order harmonic generation, are a key ingredient for attosecond metrology, providing a tool to precisely initiate and probe ultrafast dynamics in the microcosms of atoms, molecules, and solids. These ultrashort pulses are always, and as a by-product of the way they are generated, accompanied by laser-induced recollisions of electrons with their parent ions. By using a few-cycle infrared (λ(0)=2.1 μm) driving laser, we were able to directly excite high-energy (～870 eV) inner-shell electrons through laser-induced electron recollision, opening the door to time-resolved studies of core-level and concomitant multielectron dynamics.     

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.     

Frequency-resolved optical gating of isolated attosecond pulses in the extreme ultraviolet

The pulse shape and phase of isolated attosecond extreme ultraviolet (XUV) pulses with a duration of 860 asec have been determined simultaneously by using frequency-resolved optical gating based on two-photon above-threshold ionization with 28-eV photons in He. From the detailed characterization, we succeeded in shaping isolated XUV pulses on an attosecond time scale by precise dispersion control with Ar gas density or by changing the driving pulse width. These results offer a novel way to excite and observe an electron motion in atoms and molecules.     

Extreme ultraviolet Fourier-transform spectroscopy with high order harmonics

We demonstrate a new scheme for extreme ultraviolet (xuv) Fourier-transform spectroscopy based on the generation of two phase-locked high-harmonic beams. It allows us to measure for the first time interferograms at wavelengths as short as 90 nm, and open the perspective of performing high-resolution Fourier-transform absorption spectroscopy in the xuv. Our measurements also demonstrate that a precise control of the relative phase of harmonic pulses can be obtained with an accuracy on an attosecond time scale, of importance for future xuv pump-xuv probe attosecond spectroscopy.     

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.     

Use of electron correlation to make attosecond measurements without attosecond pulses

We describe how correlations between electrons can be used to trace the dynamics of correlated two-electron ionization with attosecond precision, without using attosecond pulses. The approach is illustrated using the example of Auger or Coster-Kronig decay triggered by photoionization with an extreme ultraviolet pulse. It requires correlated measurements of angle-resolved energy spectra of both the photo- and Auger electrons in the presence of a laser pulse. To reconstruct the dynamics, we use not only classical time and energy correlation, but also entanglement between the two electrons.     

High-order harmonics generation by few-cycle and multi-cycle femtosecond laser pulses

This paper investigates experimentally high-order harmonic generation(HHG) of neon gas with 5-fs and 25-fs driving laser pulses.It has been demonstrated that the cutoff energy of the harmonic extreme ultraviolet photons is extended to 131 eV and the HHG spectrum near the cutoff region becomes continuum as the driving laser pulse duration is 5 fs;whereas much lower cutoff photon energy and discrete harmonic spectrum near the cutoff region are presented as the laser pulse duration is 25 fs.The results can be explained by the fact that neutral atoms can be exposed to more intense laser field before they are depleted by ionization because of the extremely short rising time of the few-cycle pulse.The 5-fs driving laser pulse paves the way of generation of coherent x-ray in the water window and single attosecond pulse.     

Direct XUV probing of attosecond electron recollision

We demonstrate that the recolliding electron wave packet, fundamental to many strong field phenomena, can be directly imaged with sub-A spatial and attosecond temporal resolution using attosecond extreme ultraviolet (XUV) pulses. When the recolliding electron revisits the parent ion, it can absorb an XUV photon yielding high energy electron and thereby providing a measurement of the electron energy at the moment of recollision. The full temporal evolution of the recollision wave packet can be reconstructed by measuring the photoelectron spectra for different time delays between the driving laser and the attosecond XUV probe. The strength of the photoelectron signal can be used to characterize the spatial distribution of the electron density in the longitudinal direction. Elliptical polarization can be used to characterize the electron probability in transversal direction.     

超快激光的新前沿—阿秒科学

超短脉冲激光正在进行着从飞秒（1fs=10^-15s)向阿秒（1attosecond=10^-18s)的跨越,这一跨越对于激光原理和激光应用来说都有很重要的意义,文章通过阿秒脉冲与飞秒脉冲比较来介绍超快激光的新前沿－阿秒科学,包括阿秒科学的诞生,现状以及由于阿秒脉冲的产生而出现的阿秒科学的概况 。     

Single attosecond pulses from high harmonics driven by self-compressed filaments

We show that isolated subfemtosecond, extreme ultraviolet (XUV) pulses can be generated via harmonic generation in argon by few-cycle infrared pulses formed through filamentation-induced self-compression in neon. Our calculations show that the time structure of the XUV pulses depends sensitively on both the amplitude and the phase modulation that are induced in the driving pulse during the self-compression process.     

Coherent Control of High Harmonic Generation Driven by Metal Nanotip Photoemission

Steering ultrafast electron dynamics with well-controlled laser fields is very important for generation of intense supercontinuum radiation. It can be achieved through coherent control of the symmetry of the interaction between strong-field laser fields and a metal nanotip. We employ a scheme of two-color laser pulses combined with a weak static field to realize the control of a single quantum path to generate high harmonic generation from a single solid-state nanoemitter. Moreover, a smooth and ultrabroad supercontinuum in the extreme ultraviolet region is obtained, which can produce a single attosecond pulse. Our findings are beneficial for efficient generation of isolated sub-100 as XUV pulses from solid-state sources.     

Internal momentum state mapping using high harmonic radiation

We numerically demonstrate so-far undescribed features in ionization and high harmonic generation from bound states with nonvanishing electronic angular momentum. The states' modified response to a strong laser pulse can be exploited for novel measurement and pulse production schemes. It is shown that angularly asymmetric tunneling from the states can be mapped onto variations of high harmonic intensities and that near-circularly polarized isolated attosecond extreme ultraviolet or x-ray pulses can be produced.     

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.     

Generation of an isolated sub-100 attosecond pulse in the water-window spectral region

We propose a scheme to generate isolated attosecond pulses in the water-window spectral region. Based on the numerical solutions of the single active electron model, we investigate high-order harmonic generation in helium atoms driven by a multi-cycle two-colour optical field synthesized by an intense 2000 nm, 20 fs pulse and its frequency-doubled pulse. When the latter is slightly detuned and properly phase shifted with respect to the fundamental laser pulse, an ultra-broad extreme ultraviolet supercontinuum with a spectral width of 130~eV can be generated in the 270--400~eV spectral regions. A supercontinuum from 280--340~eV in the water window can be selected to yield an isolated 67 attosecond pulse without employing any phase compensation. This water window coherent x-ray pulse with less than 100 attosecond duration is a potential tool for studying the ultrafast electronic dynamics of biological samples in water.