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.     

Sub-laser-cycle electron pulses for probing molecular dynamics

Experience shows that the ability to make measurements in any new time regime opens new areas of science. Currently, experimental probes for the attosecond time regime (10(-18) 10(-15) s) are being established. The leading approach is the generation of attosecond optical pulses by ionizing atoms with intense laser pulses. This nonlinear process leads to the production of high harmonics during collisions between electrons and the ionized atoms. The underlying mechanism implies control of energetic electrons with attosecond precision. We propose that the electrons themselves can be exploited for ultrafast measurements. We use a 'molecular clock', based on a vibrational wave packet in H(2)(+) to show that distinct bunches of electrons appear during electron ion collisions with high current densities, and durations of about 1 femtosecond (10(-15) s). Furthermore, we use the molecular clock to study the dynamics of non-sequential double ionization.     

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.     

Attosecond control of electronic processes by intense light fields

The amplitude and frequency of laser light can be routinely measured and controlled on a femtosecond (10(-15) s) timescale. However, in pulses comprising just a few wave cycles, the amplitude envelope and carrier frequency are not sufficient to characterize and control laser radiation, because evolution of the light field is also influenced by a shift of the carrier wave with respect to the pulse peak. This so-called carrier-envelope phase has been predicted and observed to affect strong-field phenomena, but random shot-to-shot shifts have prevented the reproducible guiding of atomic processes using the electric field of light. Here we report the generation of intense, few-cycle laser pulses with a stable carrier envelope phase that permit the triggering and steering of microscopic motion with an ultimate precision limited only by quantum mechanical uncertainty. Using these reproducible light waveforms, we create light-induced atomic currents in ionized matter; the motion of the electronic wave packets can be controlled on timescales shorter than 250 attoseconds (250 x 10(-18) s). This enables us to control the attosecond temporal structure of coherent soft X-ray emission produced by the atomic currents--these X-ray photons provide a sensitive and intuitive tool for determining the carrier-envelope phase.     

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.     

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.     

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   

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．     

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.     

Use of photoelectron energy spectrum transfer equation for the measurement of a narrowband XUV pulse

To study the time evolution of a molecular state in an ultra-fast chemical reaction,the use of shorter pulses with higher photon energy and narrower bandwidth for both pump and probe is necessary.However,quick and precise measurement of their detailed time structures is a challenge.Over the last decade,great efforts have been made to measure an attosecond extreme ultraviolet (XUV) pulse.To date,several methods have been developed to measure the pulse duration and completely reconstruct it.The attosecond spectral phase interferometry for direct electric field reconstruction (SPIDER) and attosecond frequency-resolved optical gating (FROG) techniques are often used.However,these methods use state-of-the-art experimental set-ups and complicated data analysis procedures.To develop attosecond metrology for practical use (e.g.timing,measurement,evaluation,calibration,optimization,pumping,probing),we propose a quick and analytical method to precisely observe an attosecond XUV pulse with laser-assisted photo-ionization.The method is based on determining the laser-related phase of each streaked electron and using a transfer equation for one-step pulse reconstruction without any time-resolved measurements,iterative calculations,or data fitting procedures.Temporal errors of the pulse reconstruction are calculated from the XUV bandwidth.Because the transfer equation establishes a direct connection between the XUV pulse properties,the crucial laser parameters (peak intensity,phase,carrier envelope phase),the atomic ionization potential,and the measured photoelectron energy spectrum,we can use it to study any one of these properties from other known information and probe the dynamic processes of an ultra-fast reaction.     

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.     

Controlled injection and acceleration of electrons in plasma wakefields by colliding laser pulses

In laser-plasma-based accelerators, an intense laser pulse drives a large electric field (the wakefield) which accelerates particles to high energies in distances much shorter than in conventional accelerators. These high acceleration gradients, of a few hundreds of gigavolts per metre, hold the promise of compact high-energy particle accelerators. Recently, several experiments have shown that laser-plasma accelerators can produce high-quality electron beams, with quasi-monoenergetic energy distributions at the 100 MeV level. However, these beams do not have the stability and reproducibility that are required for applications. This is because the mechanism responsible for injecting electrons into the wakefield is based on highly nonlinear phenomena, and is therefore hard to control. Here we demonstrate that the injection and subsequent acceleration of electrons can be controlled by using a second laser pulse. The collision of the two laser pulses provides a pre-acceleration stage which provokes the injection of electrons into the wakefield. The experimental results show that the electron beams obtained in this manner are collimated (5 mrad divergence), monoenergetic (with energy spread <10 per cent), tuneable (between 15 and 250 MeV) and, most importantly, stable. In addition, the experimental observations are compatible with electron bunch durations shorter than 10 fs. We anticipate that this stable and compact electron source will have a strong impact on applications requiring short bunches, such as the femtolysis of water, or high stability, such as radiotherapy with high-energy electrons or radiography for materials science.     

不同啁啾调制对光谱连续区的影响

利用啁啾场调控激光波形,理论研究了不同啁啾场对高次谐波光谱的影响. 结果表明：当采用对称中间啁啾调控时,谐波截止能量的延伸及光谱连续区来自于激光中间区域. 当采用不对称负向啁啾调控时,谐波截止能量的延伸及光谱连续区来自于激光下降区域. 虽然,谐波截止能量在不同啁啾调控下都可以得到延伸,但是,不对称负向啁啾场下光谱连续区的强度要比对称中间啁啾场下光谱连续区强度高2个数量级. 最后,通过叠加光谱连续区上的谐波可以获得2个脉宽在38 as的单个阿秒脉冲. 并且,负向啁啾场下获得脉冲强度要比对称中间啁啾场下获得脉冲强度高2个数量级.     

Absolute-phase phenomena in photoionization with few-cycle laser pulses.

Currently, the shortest laser pulses that can be generated in the visible spectrum consist of fewer than two optical cycles (measured at the full-width at half-maximum of the pulse's envelope). The time variation of the electric field in such a pulse depends on the phase of the carrier frequency with respect to the envelope-the absolute phase. Because intense laser-matter interactions generally depend on the electric field of the pulse, the absolute phase is important for a number of nonlinear processes. But clear evidence of absolute-phase effects has yet to be detected experimentally, largely because of the difficulty of stabilizing the absolute phase in powerful laser pulses. Here we use a technique that does not require phase stabilization to demonstrate experimentally the influence of the absolute phase of a short laser pulse on the emission of photoelectrons. Atoms are ionized by a short laser pulse, and the photoelectrons are recorded with two opposing detectors in a plane perpendicular to the laser beam. We detect an anticorrelation in the shot-to-shot analysis of the electron yield.     

Attosecond real-time observation of electron tunnelling in atoms

Atoms exposed to intense light lose one or more electrons and become ions. In strong fields, the process is predicted to occur via tunnelling through the binding potential that is suppressed by the light field near the peaks of its oscillations. Here we report the real-time observation of this most elementary step in strong-field interactions: light-induced electron tunnelling. The process is found to deplete atomic bound states in sharp steps lasting several hundred attoseconds. This suggests a new technique, attosecond tunnelling, for probing short-lived, transient states of atoms or molecules with high temporal resolution. The utility of attosecond tunnelling is demonstrated by capturing multi-electron excitation (shake-up) and relaxation (cascaded Auger decay) processes with subfemtosecond resolution.     

Probing molecular dynamics with attosecond resolution using correlated wave packet pairs

Spectroscopic measurements with increasingly higher time resolution are generally thought to require increasingly shorter laser pulses, as illustrated by the recent monitoring of the decay of core-excited krypton using attosecond photon pulses. However, an alternative approach to probing ultrafast dynamic processes might be provided by entanglement, which has improved the precision of quantum optical measurements. Here we use this approach to observe the motion of a D2+ vibrational wave packet formed during the multiphoton ionization of D2 over several femtoseconds with a precision of about 200 attoseconds and 0.05 ?ngstr?ms, by exploiting the correlation between the electronic and nuclear wave packets formed during the ionization event. An intense infrared laser field drives the electron wave packet, and electron recollision probes the nuclear motion. Our results show that laser pulse duration need not limit the time resolution of a spectroscopic measurement, provided the process studied involves the formation of correlated wave packets, one of which can be controlled; spatial resolution is likewise not limited to the focal spot size or laser wavelength.     

Laser induced photoemission electron and the generation of high Rydberg states of atoms and molecules

Laser induced photoemission electron was produced by directing 532 nm and/or 355 nm onto stainless steel plate on a time of flight mass spectrometer. Multiple charged ions and high Rydberg states of atoms or molecules were successfully generated by impacts of the photoemission electrons. The high Rydberg states ( n ～40-100) thus produced were separated from ions, produced by direct electron impact ionization, by a 3 V DC electric field and then ionized by a delayed pulsed HV electric field in a ZEKE-PFI manner. Relationship between generation/property of high Rydberg states of atoms/molecules and experimental conditions could be investigated. Relationship between the electron accelerating voltage and high Rydberg states of Ar was described.     

空气中产生太赫兹波过程有关离化机制的理论模拟

在利用光电流模型模拟空气中太赫兹辐射的过程中,飞秒激光首先将大气离化,离化后的电子在外场下加速,产生一定量的太赫兹波。当飞秒激光的能量达到一定强度时,离化过程变得复杂,可发生多阶离化,并在产生离子数中扮演重要角色,尤其是二阶离化作用突出。文章重点讨论二阶离化对产生离子数的贡献。     

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.     

High-quality electron beams from a laser wakefield accelerator using plasma-channel guiding

Laser-driven accelerators, in which particles are accelerated by the electric field of a plasma wave (the wakefield) driven by an intense laser, have demonstrated accelerating electric fields of hundreds of GV m(-1) (refs 1-3). These fields are thousands of times greater than those achievable in conventional radio-frequency accelerators, spurring interest in laser accelerators as compact next-generation sources of energetic electrons and radiation. To date, however, acceleration distances have been severely limited by the lack of a controllable method for extending the propagation distance of the focused laser pulse. The ensuing short acceleration distance results in low-energy beams with 100 per cent electron energy spread, which limits potential applications. Here we demonstrate a laser accelerator that produces electron beams with an energy spread of a few per cent, low emittance and increased energy (more than 10(9) electrons above 80 MeV). Our technique involves the use of a preformed plasma density channel to guide a relativistically intense laser, resulting in a longer propagation distance. The results open the way for compact and tunable high-brightness sources of electrons and radiation.