Nonlinear optics in the extreme ultraviolet

Nonlinear responses to an optical field are universal in nature but have been difficult to observe in the extreme ultraviolet (XUV) and soft X-ray regions owing to a lack of coherent intense light sources. High harmonic generation is a well-known nonlinear optical phenomenon and is now drawing much attention in attosecond pulse generation. For the application of high harmonics to nonlinear optics in the XUV and soft X-ray regime, optical pulses should have both large pulse energy and short pulse duration to achieve a high optical electric field. Here we show the generation of intense isolated pulses from a single harmonic (photon energy 27.9 eV) by using a sub-10-femtosecond blue laser pulse, producing a large dipole moment at the relatively low (ninth) harmonic order nonadiabatically. The XUV pulses with pulse durations of 950 attoseconds and 1.3 femtoseconds were characterized by an autocorrelation technique, based on two-photon above-threshold ionization of helium atoms. Because of the small cross-section for above-threshold ionization, such an autocorrelation measurement of XUV pulses with photon energy larger than the ionization energy of helium has not hitherto been demonstrated. The technique can be extended to the characterization of higher harmonics at shorter wavelengths.     

Atomic transient recorder

In Bohr's model of the hydrogen atom, the electron takes about 150 attoseconds (1 as = 10(-18) s) to orbit around the proton, defining the characteristic timescale for dynamics in the electronic shell of atoms. Recording atomic transients in real time requires excitation and probing on this scale. The recent observation of single sub-femtosecond (1 fs = 10(-15) s) extreme ultraviolet (XUV) light pulses has stimulated the extension of techniques of femtochemistry into the attosecond regime. Here we demonstrate the generation and measurement of single 250-attosecond XUV pulses. We use these pulses to excite atoms, which in turn emit electrons. An intense, waveform-controlled, few cycle laser pulse obtains 'tomographic images' of the time-momentum distribution of the ejected electrons. Tomographic images of primary (photo)electrons yield accurate information of the duration and frequency sweep of the excitation pulse, whereas the same measurements on secondary (Auger) electrons will provide insight into the relaxation dynamics of the electronic shell following excitation. With the current approximately 750-nm laser probe and approximately 100-eV excitation, our transient recorder is capable of resolving atomic electron dynamics within the Bohr orbit time.     

Direct observation of electron dynamics in the attosecond domain

Dynamical processes are commonly investigated using laser pump-probe experiments, with a pump pulse exciting the system of interest and a second probe pulse tracking its temporal evolution as a function of the delay between the pulses. Because the time resolution attainable in such experiments depends on the temporal definition of the laser pulses, pulse compression to 200 attoseconds (1 as = 10(-18) s) is a promising recent development. These ultrafast pulses have been fully characterized, and used to directly measure light waves and electronic relaxation in free atoms. But attosecond pulses can only be realized in the extreme ultraviolet and X-ray regime; in contrast, the optical laser pulses typically used for experiments on complex systems last several femtoseconds (1 fs = 10(-15) s). Here we monitor the dynamics of ultrafast electron transfer--a process important in photo- and electrochemistry and used in solid-state solar cells, molecular electronics and single-electron devices--on attosecond timescales using core-hole spectroscopy. We push the method, which uses the lifetime of a core electron hole as an internal reference clock for following dynamic processes, into the attosecond regime by focusing on short-lived holes with initial and final states in the same electronic shell. This allows us to show that electron transfer from an adsorbed sulphur atom to a ruthenium surface proceeds in about 320 as.     

Direct observation of attosecond light bunching

Temporal probing of a number of fundamental dynamical processes requires intense pulses at femtosecond or even attosecond (1 as = 10(-18) s) timescales. A frequency 'comb' of extreme-ultraviolet odd harmonics can easily be generated in the interaction of subpicosecond laser pulses with rare gases: if the spectral components within this comb possess an appropriate phase relationship to one another, their Fourier synthesis results in an attosecond pulse train. Laser pulses spanning many optical cycles have been used for the production of such light bunching, but in the limit of few-cycle pulses the same process produces isolated attosecond bursts. If these bursts are intense enough to induce a nonlinear process in a target system, they can be used for subfemtosecond pump-probe studies of ultrafast processes. To date, all methods for the quantitative investigation of attosecond light localization and ultrafast dynamics rely on modelling of the cross-correlation process between the extreme-ultraviolet pulses and the fundamental laser field used in their generation. Here we report the direct determination of the temporal characteristics of pulses in the subfemtosecond regime, by measuring the second-order autocorrelation trace of a train of attosecond pulses. The method exhibits distinct capabilities for the characterization and utilization of attosecond pulses for a host of applications in attoscience.     

He^＋离子在啁啾激光和高频脉冲组合场中产生的单个阿秒脉冲

利用数值求解含时薛定谔方程的方法,从理论上研究了一维模型He＋离子在波长为1064nm的线性啁啾激光和高频脉冲形成的组合场中产生的高次谐波以及由这种高次谐波构造的阿秒脉冲特征.发现在组合场中,由于啁啾脉冲的作用和在适当的时刻加入了高频脉冲,不仅使高次谐波谱的平台区域能得到很大的扩展,而且谐波转化效率也得到有效地提高,当对第二平台区域的不同范围内高次谐波迭加都可得到单个阿秒脉冲,最短可达21阿秒.最后通过经典分析和时频分析解释了这种高次谐波展宽与阿秒脉冲发射过程的特点.     

Radiation properties of high-order harmonic generation for the measurements of femto- and attosecond X-ray pulses

Radiation properties of high-order harmonic generation （HHG） are calculated for atoms in a strong laser field. The laser-duration dependence and the carrier-envelope-phase （CEP） dependence of HHG radiation properties are presented. The CEP dependence of the pure single distribution pulse of HHG radiation properties shows interesting 180° periodic structures. The quantum enhancement of the laser-assisted photo-ionization by femtosecond （1 fs=10^-15 s） and attosecond （1 as=10^-18 s） X-ray pulses and the interference patterns of photo-electron energy spectra are theoretically investigated. Transfer equations are presented for pulse reconstructions. The theoretical root-mean-square time （energy） differences of attosecond pulse reconstructions with different durations are less than 2 as （0,8 eV）. These methods may be developed as basic techniques to access ultra-fast measurements and molecular movie.     

Attosecond metrology.

The generation of ultrashort pulses is a key to exploring the dynamic behaviour of matter on ever-shorter timescales. Recent developments have pushed the duration of laser pulses close to its natural limit-the wave cycle, which lasts somewhat longer than one femtosecond (1 fs = 10-15 s) in the visible spectral range. Time-resolved measurements with these pulses are able to trace dynamics of molecular structure, but fail to capture electronic processes occurring on an attosecond (1 as = 10-18 s) timescale. Here we trace electronic dynamics with a time resolution of 相似文献   

Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy

Molecular vibrations have oscillation periods that reflect the molecular structure, and are hence being used as a spectroscopic fingerprint for detection and identification. At present, all nonlinear spectroscopy schemes use two or more laser beams to measure such vibrations. The availability of ultrashort (femtosecond) optical pulses with durations shorter than typical molecular vibration periods has enabled the coherent excitation of molecular vibrations using a single pulse. Here we perform single-pulse vibrational spectroscopy on several molecules in the liquid phase, where both the excitation and the readout processes are performed by the same pulse. The main difficulty with single-pulse spectroscopy is that all vibrational levels with energies within the pulse bandwidth are excited. We achieve high spectral resolution, nearly two orders of magnitude better than the pulse bandwidth, by using quantum coherent control techniques. By appropriately modulating the spectral phase of the pulse we are able to exploit the quantum interference between multiple paths to selectively populate a given vibrational level, and to probe this population using the same pulse. This scheme, using a single broadband laser source, is particularly attractive for nonlinear microscopy applications, as we demonstrate by constructing a coherent anti-Stokes Raman (CARS) microscope operating with a single laser beam.     

Resolving the time when an electron exits a tunnelling barrier

The tunnelling of a particle through a barrier is one of the most fundamental and ubiquitous quantum processes. When induced by an intense laser field, electron tunnelling from atoms and molecules initiates a broad range of phenomena such as the generation of attosecond pulses, laser-induced electron diffraction and holography. These processes evolve on the attosecond timescale (1?attosecond?≡?1?as = 10(-18)?seconds) and are well suited to the investigation of a general issue much debated since the early days of quantum mechanics--the link between the tunnelling of an electron through a barrier and its dynamics outside the barrier. Previous experiments have measured tunnelling rates with attosecond time resolution and tunnelling delay times. Here we study laser-induced tunnelling by using a weak probe field to steer the tunnelled electron in the lateral direction and then monitor the effect on the attosecond light bursts emitted when the liberated electron re-encounters the parent ion. We show that this approach allows us to measure the time at which the electron exits from the tunnelling barrier. We demonstrate the high sensitivity of the measurement by detecting subtle delays in ionization times from two orbitals of a carbon dioxide molecule. Measurement of the tunnelling process is essential for all attosecond experiments where strong-field ionization initiates ultrafast dynamics. Our approach provides a general tool for time-resolving multi-electron rearrangements in atoms and molecules--one of the key challenges in ultrafast science.     

Editor’s note

The past two decades have witnessed great progress in development of ultrashort laser pulse in laser science, often at an unexpected speed. It has found various applications, both theoretical and practical, in the frontiers of science.     

Attosecond spectroscopy in condensed matter

Comprehensive knowledge of the dynamic behaviour of electrons in condensed-matter systems is pertinent to the development of many modern technologies, such as semiconductor and molecular electronics, optoelectronics, information processing and photovoltaics. Yet it remains challenging to probe electronic processes, many of which take place in the attosecond (1 as = 10(-18) s) regime. In contrast, atomic motion occurs on the femtosecond (1 fs = 10(-15) s) timescale and has been mapped in solids in real time using femtosecond X-ray sources. Here we extend the attosecond techniques previously used to study isolated atoms in the gas phase to observe electron motion in condensed-matter systems and on surfaces in real time. We demonstrate our ability to obtain direct time-domain access to charge dynamics with attosecond resolution by probing photoelectron emission from single-crystal tungsten. Our data reveal a delay of approximately 100 attoseconds between the emission of photoelectrons that originate from localized core states of the metal, and those that are freed from delocalized conduction-band states. These results illustrate that attosecond metrology constitutes a powerful tool for exploring not only gas-phase systems, but also fundamental electronic processes occurring on the attosecond timescale in condensed-matter systems and on surfaces.     

Ways to produce and measure atto- and femtosecond soft X-ray pulses

The ways to produce and measure atto-and femtosecond soft X-ray pulses are reported. The laser phase relation of high-order harmonic generation(HHG) shows two different radiation energy distribu-tions in time(or laser phase) domain. These energy-phase relations are helpful for realizing the dy-namic processes of HHG. Two presented parameterized formulas can be used to calculate the durations of the energy distributions with a bandwidth of the pulse. These formulas are useful in calculating and simulating pulses transports and interactions with mediums. The time structures of atto-and femto-second soft X-ray pulses can be directly measured with photoelectron spectrum transfer equations and the related laser phase determination methods without any previous pulse shape and the instantane-ous frequency assumptions. These equations and methods can be used to evaluate and improve the technical parameters of the ultra-short X-ray sources. They have wide measurement ranges and high time resolutions,which may enable ultra-fast measurements to reach metrological precisions,and lead to a new tide of scientific researches in physics,chemistry,biochemistry,etc. The application of atto-and femtosecond X-rays as well as the theoretical and technical problems in measurements are briefly discussed.     

Effects of different nuclear transfer and activation methods on the development of mouse somatic cell cloned embryos

A group of adult somatic cell cloned mice were obtained by using cumulus cells as nuclei donor cells. To study the effect of different nuclear transfer (NT) and activation methods on the development of mouse cloned embryos, embryos were reconstructed using two traditional NT methods (electrofusion and direct injection) and four activation treatments (electric pulse, ethanol, SrCl2 and electric pulse combined with SrCl2). The data showed that the efficiency of reconstruction using the direct injection method is significantly higher (90.7%) than that of the electrofusion method (49.7%). Parthenogenetic embryos can develop to blastocyst stage with three activation conditions, including ethanol, electric pulse and SrCl2; however, the rates of development to blastocyst after ethanol and electric pulse acti-vation (52.4%, 54.2%) are significantly lower than after SrCl2 activation (76.9%). Treatment of embryos for 6 h with 10 mmol/L SrCl2 was found to be the best condition for activation of parthenogenetic as well as reconstructed embryos. By contrast, reconstructed embryos failed to develop to blastocyst stage after being activated by ethanol. The use of either injection or electrofusion for embryo reconstruction affected the pre-implantation development. However, after transfer in pseudopregnant mice, cloned mice were obtained from both methods.     

激光与薄膜靶作用产生X射线阿秒脉冲两种方案的比较

运用一维粒子模拟对经由相对论电子束汤姆逊散射来产生阿秒X射线的两种方案进行了研究。第一种是激光驱动薄膜靶产生相对论电子束以及经过汤姆逊散射产生阿秒X射线,运用倍频探测光的方案可得到更短波长X射线。第二种方案添加了反射厚靶,通过厚靶对驱动激光的反射来减小电子束的横向动量但让其通过,而探测脉冲经过电子束汤姆逊散射后的多普勒频移因子提高,得到的X射线波长也明显减小,光子能量达到1KeV,反射光频谱也明显优与第一种方案．     

气固两相流静电传感器特性的研究

基于点电荷的概念,设计了气固两相流传感器的静电感应实验装置,并实验研究了传感器环状电极的几何尺寸对传感器性能的影响．结果表明,对于直径相同的电极,其长度越短,所构成的传感器的通带频宽越大,但传感器的能量传递系数却变小．因此在设计传感器时,应综合考虑频宽与能量传递系数对测量结果的影响．     

导体表面雷电流测量

为了对雷电流在导体表面的分布情况进行研究,研制了线圈式表面电流探头和巨磁阻表面电流测量系统,设计制作了低压脉冲源,在TEM传输室中对2种测量系统进行了实验和标定。采用这2种测量系统对矩形铝板表面电流密度进行了测量和仿真计算,实测和仿真计算结果一致。结果表明,巨磁阻表面电流测量系统可用于研究雷电流在导体表面的分布;采用合适频率的连续波,线圈式表面电流探头用于替代雷电流密度分布测量也是可行的。     

高能电子束的电光探测方法

本文介绍两种电光探测方法测量电子束长度：延迟扫描法、啁啾脉冲法(包括啁啾脉冲光谱仪法和啁啾脉冲互相关法)，并比较了不同方法的速度、时间分辨率．论文还讨论了使用电光晶体时吸收和色散对电子束电场形状的影响，及电子束与探测脉冲之间的同步问题．     

基于光纤技术的叶端定时传感器

叶端定时测量是一种新型的在线实时测量叶片振动的有效方法，激光光纤叶端定时传感器是整个测试系统设计的关键，该文研究了叶端定时测量方法，并对应用于高速旋转汽轮机叶片振动在线实时监测的光叶端定时传感器进行了设计研究和试验，研究了一个具有高分辨、大频宽和高信噪比的激光光纤传感器的设计方案，并且得到了实验室验证。     

Attosecond control of electrons emitted from a nanoscale metal tip

Attosecond science is based on steering electrons with the electric field of well controlled femtosecond laser pulses. It has led to the generation of extreme-ultraviolet pulses with a duration of less than 100 attoseconds (ref. 3; 1 as = 10(-18) s), to the measurement of intramolecular dynamics (by diffraction of an electron taken from the molecule under scrutiny) and to ultrafast electron holography. All these effects have been observed with atoms or molecules in the gas phase. Electrons liberated from solids by few-cycle laser pulses are also predicted to show a strong light-phase sensitivity, but only very small effects have been observed. Here we report that the spectra of electrons undergoing photoemission from a nanometre-scale tungsten tip show a dependence on the carrier-envelope phase of the laser, with a current modulation of up to 100 per cent. Depending on the carrier-envelope phase, electrons are emitted either from a single sub-500-attosecond interval of the 6-femtosecond laser pulse, or from two such intervals; the latter case leads to spectral interference. We also show that coherent elastic re-scattering of liberated electrons takes place at the metal surface. Owing to field enhancement at the tip, a simple laser oscillator reaches the peak electric field strengths required for attosecond experiments at 100-megahertz repetition rates, rendering complex amplified laser systems dispensable. Practically, this work represents a simple, extremely sensitive carrier-envelope phase sensor, which could be shrunk in volume to about one cubic centimetre. Our results indicate that the attosecond techniques developed with (and for) atoms and molecules can also be used with solids. In particular, we foresee subfemtosecond, subnanometre probing of collective electron dynamics (such as plasmon polaritons) in solid-state systems ranging in scale from mesoscopic solids to clusters and to single protruding atoms.     

Optimal quantum measurement of finite-dimensional systems and coherent anti-Stokes Raman spectroscopy

Quantum measurement is a fundamental problem in quantum control theory and experiments.It can obtain unknown information of quantum systems,and can also change state of the systems inevitably.Both the outcome and back action could be used to control quantum systems.This paper presents recent research progress about optimal control of state transformation in finite-dimensional quantum systems by back action of non-selective quantum measurement,and optimal control of signal and background of CARS (coherent anti-Stokes Raman spectroscopy) by phase shaping technique.In measurement sequence control of finite-dimensional quantum systems,the necessary condition for critical points of the underlying state transformation objective is found to be a highly symmetric form as a chain of equalities,and analytical and numerical solutions in several cases are explored.In the CARS control,it is found that the maximal resonant signal and minimal background at a specific frequency can be achieved by shaping the probe pulse only while keeping pump and Stokes pulses in transform limited forms (TLFs).An arctan-type phase function is obtained for the probe pulse to simultaneously enhance the resonant signal and suppress the background.For broadband background elimination,we find that the optimal phase shaping scheme of probe pulse is quasi-time-delay while keeping the pump and Stokes pulses in TLFs.These conclusions could help design control strategies of quantum devices.