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.     

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.     

Potential for biomolecular imaging with femtosecond X-ray pulses

Sample damage by X-rays and other radiation limits the resolution of structural studies on non-repetitive and non-reproducible structures such as individual biomolecules or cells. Cooling can slow sample deterioration, but cannot eliminate damage-induced sample movement during the time needed for conventional measurements. Analyses of the dynamics of damage formation suggest that the conventional damage barrier (about 200 X-ray photons per A2 with X-rays of 12 keV energy or 1 A wavelength) may be extended at very high dose rates and very short exposure times. Here we have used computer simulations to investigate the structural information that can be recovered from the scattering of intense femtosecond X-ray pulses by single protein molecules and small assemblies. Estimations of radiation damage as a function of photon energy, pulse length, integrated pulse intensity and sample size show that experiments using very high X-ray dose rates and ultrashort exposures may provide useful structural information before radiation damage destroys the sample. We predict that such ultrashort, high-intensity X-ray pulses from free-electron lasers that are currently under development, in combination with container-free sample handling methods based on spraying techniques, will provide a new approach to structural determinations with X-rays.     

Single mimivirus particles intercepted and imaged with an X-ray laser

X-ray lasers offer new capabilities in understanding the structure of biological systems, complex materials and matter under extreme conditions. Very short and extremely bright, coherent X-ray pulses can be used to outrun key damage processes and obtain a single diffraction pattern from a large macromolecule, a virus or a cell before the sample explodes and turns into plasma. The continuous diffraction pattern of non-crystalline objects permits oversampling and direct phase retrieval. Here we show that high-quality diffraction data can be obtained with a single X-ray pulse from a non-crystalline biological sample, a single mimivirus particle, which was injected into the pulsed beam of a hard-X-ray free-electron laser, the Linac Coherent Light Source. Calculations indicate that the energy deposited into the virus by the pulse heated the particle to over 100,000?K after the pulse had left the sample. The reconstructed exit wavefront (image) yielded 32-nm full-period resolution in a single exposure and showed no measurable damage. The reconstruction indicates inhomogeneous arrangement of dense material inside the virion. We expect that significantly higher resolutions will be achieved in such experiments with shorter and brighter photon pulses focused to a smaller area. The resolution in such experiments can be further extended for samples available in multiple identical copies.     

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.     

Probing carrier dynamics in nanostructures by picosecond cathodoluminescence

Picosecond and femtosecond spectroscopy allow the detailed study of carrier dynamics in nanostructured materials. In such experiments, a laser pulse normally excites several nanostructures at once. However, spectroscopic information may also be acquired using pulses from an electron beam in a modern electron microscope, exploiting a phenomenon called cathodoluminescence. This approach offers several advantages. The multimode imaging capabilities of the electron microscope enable the correlation of optical properties (via cathodoluminescence) with surface morphology (secondary electron mode) at the nanometre scale. The broad energy range of the electrons can excite wide-bandgap materials, such as diamond- or gallium-nitride-based structures that are not easily excited by conventional optical means. But perhaps most intriguingly, the small beam can probe a single selected nanostructure. Here we apply an original time-resolved cathodoluminescence set-up to describe carrier dynamics within single gallium-arsenide-based pyramidal nanostructures with a time resolution of 10 picoseconds and a spatial resolution of 50 nanometres. The behaviour of such charge carriers could be useful for evaluating elementary components in quantum computers, optical quantum gates or single photon sources for quantum cryptography.     

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.     

Coherent control of pulsed X-ray beams.

Synchrotrons produce continuous trains of closely spaced X-ray pulses. Application of such sources to the study of atomic-scale motion requires efficient modulation of these beams on timescales ranging from nanoseconds to femtoseconds. However, ultrafast X-ray modulators are not generally available. Here we report efficient subnanosecond coherent switching of synchrotron beams by using acoustic pulses in a crystal to modulate the anomalous low-loss transmission of X-ray pulses. The acoustic excitation transfers energy between two X-ray beams in a time shorter than the synchrotron pulse width of about 100 ps. Gigahertz modulation of the diffracted X-rays is also observed. We report different geometric arrangements, such as a switch based on the collision of two counter-propagating acoustic pulses: this doubles the X-ray modulation frequency, and also provides a means of observing a localized transient strain inside an opaque material. We expect that these techniques could be scaled to produce subpicosecond pulses, through laser-generated coherent optical phonon modulation of X-ray diffraction in crystals. Such ultrafast capabilities have been demonstrated thus far only in laser-generated X-ray sources, or through the use of X-ray streak cameras.     

Shaped-pulse optimization of coherent emission of high-harmonic soft X-rays

When an intense laser pulse is focused into a gas, the light-atom interaction that occurs as atoms are ionized results in an extremely nonlinear optical process--the generation of high harmonics of the driving laser frequency. Harmonics that extend up to orders of about 300 have been reported, some corresponding to photon energies in excess of 500 eV. Because this technique is simple to implement and generates coherent, laser-like, soft X-ray beams, it is currently being developed for applications in science and technology; these include probing the dynamics in chemical and materials systems and imaging. Here we report that by carefully tailoring the shapes of intense light pulses, we can control the interaction of light with an atom during ionization, improving the efficiency of X-ray generation by an order of magnitude. We demonstrate that it is possible to tune the spectral characteristics of the emitted radiation, and to steer the interaction between different orders of nonlinear processes.     

Ultrafast non-thermal control of magnetization by instantaneous photomagnetic pulses

The demand for ever-increasing density of information storage and speed of manipulation has triggered an intense search for ways to control the magnetization of a medium by means other than magnetic fields. Recent experiments on laser-induced demagnetization and spin reorientation use ultrafast lasers as a means to manipulate magnetization, accessing timescales of a picosecond or less. However, in all these cases the observed magnetic excitation is the result of optical absorption followed by a rapid temperature increase. This thermal origin of spin excitation considerably limits potential applications because the repetition frequency is limited by the cooling time. Here we demonstrate that circularly polarized femtosecond laser pulses can be used to non-thermally excite and coherently control the spin dynamics in magnets by way of the inverse Faraday effect. Such a photomagnetic interaction is instantaneous and is limited in time by the pulse width (approximately 200 fs in our experiment). Our finding thus reveals an alternative mechanism of ultrafast coherent spin control, and offers prospects for applications of ultrafast lasers in magnetic devices.     

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.     

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.     

Phase transitions in the incoherent lattice fluctuations in YBa2Cu3O(7-delta)

The growing body of experimental evidence for the existence of complex textures of charges and spins in the high-temperature superconductors has drawn attention to the so-called 'stripe-phase' models as a possible basis for the mechanism of superconductivity in these materials. Such observations have until now been restricted to systems where the texture dynamics are slow or suppressed altogether, and do not include the important case of YBa2Cu3O(7-delta). It seems likely that the dynamic behaviour of stripes, which has been suggested to undergo several phase transitions as a function of temperature, should also be reflected in the lattice properties of the host materials, and this forms the motivation for our present experiments. Specifically, we use MeV helium ion channelling, an ultrafast real-space probe of atomic displacements (with sub-picometre resolution), to probe incoherent lattice fluctuations in YBa2Cu3O(7-delta) as a function of temperature and oxygen doping. We detect lattice fluctuations that are larger than the expected thermal vibration component, and which show anomalies characteristic of the phase transitions anticipated for a dynamic stripe phase. Comparison of our lattice results with single-particle-tunnelling and photoemission data highlights the importance of spin-charge separation phenomena in the copper oxide superconductors.     

强场原子分子物理实验研究中的符合测量技术及其应用

飞秒激光具有超短的脉冲宽度和超强的峰值功率，已经成为测量和操控原子分子超快动力学行为的重要工具．但是强激光场下，原子分子行为非常复杂，多个反应通道纠缠在一起．全微分符合测量技术能够提供特定反应通道精确的动力学数据，推动了强场原子分子物理研究的快速发展．本文结合北京大学新建的冷靶反冲离子动量谱仪，介绍全微分符合测量技术在强场原子分子物理实验研究中的重要应用以及在强场原子分子物理实验研究方面取得的一些重要进展．     

A frequency comb in the extreme ultraviolet

Since 1998, the interaction of precision spectroscopy and ultrafast laser science has led to several notable accomplishments. Femtosecond laser optical frequency 'combs' (evenly spaced spectral lines) have revolutionized the measurement of optical frequencies and enabled optical atomic clocks. The same comb techniques have been used to control the waveform of ultrafast laser pulses, which permitted the generation of single attosecond pulses, and have been used in a recently demonstrated 'oscilloscope' for light waves. Here we demonstrate intra-cavity high harmonic generation in the extreme ultraviolet, which promises to lead to another joint frontier of precision spectroscopy and ultrafast science. We have generated coherent extreme ultraviolet radiation at a repetition frequency of more than 100 MHz, a 1,000-fold improvement over previous experiments. At such a repetition rate, the mode spacing of the frequency comb, which is expected to survive the high harmonic generation process, is large enough for high resolution spectroscopy. Additionally, there may be many other applications of such a quasi-continuous compact and coherent extreme ultraviolet source, including extreme ultraviolet holography, microscopy, nanolithography and X-ray atomic clocks.     

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 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   

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