Attosecond Experiments Research Articles

Theoretical and experimental studies of broadband phase-controlled attosecond mirrors

We present procedures to develop and characterise chirped multilayer mirrors for attosecond pulses. The design procedure involves a simulated annealing optimisation algorithm to obtain a multilayer structure with the desired performances. The characterisation step requires the use of well-calibrated attosecond and synchrotron beam lines, allowing one to measure the amplitude and phase response of the mirror. We illustrate these approaches with a set of mirrors designed to have zero or negative dispersion. The remarkable agreement between theoretical and experimental performances validates this overall process, and demonstrates the capability of such mirrors to control the temporal profile of attosecond pulses. These tools and techniques for developing attosecond chirped mirrors will facilitate the generalisation of such components on attosecond experiments.

Attosecond imaging

The natural timescale for electron dynamics reaches down to the attosecond domain. Following the discovery of attosecond laser pulses, about a decade ago, attosecond science has developed into a vibrant, new research field, where the motion of single or multiple electrons and, in molecules, the coupling of electronic and nuclear motion, can be investigated, on attosecond to few-femtosecond timescales. Attosecond experiments require suitable observables. This review describes how "attosecond imaging", basing itself on kinetic energy and angle-resolved detection of photoelectrons and fragment ions using a velocity map imaging (VMI) spectrometer, has been exploited in a number of pump-probe experiments. The use of a VMI spectrometer in attosecond experiments has allowed the characterization of attosecond pulse trains and isolated attosecond pulses, the elucidation of continuum electron dynamics and wave packet interferometry in atomic photoionization and the observation of electron localization in dissociative molecular photoionization.

Attosecond nonlinear optics using gigawatt-scale isolated attosecond pulses

High-energy isolated attosecond pulses required for the most intriguing nonlinear attosecond experiments as well as for attosecond-pump/attosecond-probe spectroscopy are still lacking at present. Here we propose and demonstrate a robust generation method of intense isolated attosecond pulses, which enable us to perform a nonlinear attosecond optics experiment. By combining a two-colour field synthesis and an energy-scaling method of high-order harmonic generation, the maximum pulse energy of the isolated attosecond pulse reaches as high as 1.3 μJ. The generated pulse with a duration of 500 as, as characterized by a nonlinear autocorrelation measurement, is the shortest and highest-energy pulse ever with the ability to induce nonlinear phenomena. The peak power of our tabletop light source reaches 2.6 GW, which even surpasses that of an extreme-ultraviolet free-electron laser.

Simulating Pump–Probe Photoelectron and Absorption Spectroscopy on the Attosecond Timescale with Time‐Dependent Density Functional Theory

Molecular absorption and photoelectron spectra can be efficiently predicted with real-time time-dependent density functional theory. We show herein how these techniques can be easily extended to study time-resolved pump-probe experiments, in which a system response (absorption or electron emission) to a probe pulse is measured in an excited state. This simulation tool helps with the interpretation of fast-evolving attosecond time-resolved spectroscopic experiments, in which electronic motion must be followed at its natural timescale. We show how the extra degrees of freedom (pump-pulse duration, intensity, frequency, and time delay), which are absent in a conventional steady-state experiment, provide additional information about electronic structure and dynamics that improve characterization of a system. As an extension of this approach, time-dependent 2D spectroscopy can also be simulated, in principle, for large-scale structures and extended systems.

How to focus an attosecond pulse

Attosecond experiments involving focusing of attosecond light pulses can suffer from a spread of the attosecond radiation both in space and time due to optical aberrations. We present a detailed numerical study of the distortions induced in the most common focusing geometries that make use of parabolic, spherical, toroidal and ellipsoidal mirrors. We deduce the consequences on the pulse duration and possible issues that could arise in applications of attosecond pulses. This should serve as a guideline for setting up attosecond focusing optics.

Control of bandwidth and central wavelength of an enhanced extreme ultraviolet spectrum generated in shaped laser field

We theoretically investigate the enhancement of a selected spectral range in the high-order harmonic generation driven by the multi-color laser fields. The results show that the central wavelength of the enhanced narrow-bandwidth spectrum can be effectively controlled by adjusting the laser intensity and the time delay between laser pulses of different colors, due to the modified electron trajectory in the shaped laser field. Our approach can offer intense, bandwidth controllable single attosecond pulses for attosecond pump-probe experiments.

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.

Giant half-cycle attosecond pulses

Half-cycle picosecond pulses have been produced from thin photo-conductors, when applying an electric field across the surface and switching on conduction by a short laser pulse. Then the transverse current in the wafer plane emits half-cycle pulses in normal direction, and pulses of 500 fs duration and 1e6 V/m peak electric field have been observed. Here we show that single half-cycle pulses of 50 as duration and up to 1e13 V/m can be produced when irradiating a double foil target by intense few-cycle laser pulses. Focused onto an ultra-thin foil, all electrons are blown out, forming a uniform sheet of relativistic electrons. A second layer, placed at some distance behind, reflects the drive beam, but lets electrons pass straight. Under oblique incidence, beam reflection provides the transverse current, which emits intense half-cycle pulses. Such a pulse may completely ionize even heavier atoms. New types of attosecond pump-probe experiments will become possible.

Femtosecond and Attosecond Spectroscopy in the XUV Regime

Attosecond-duration, fully coherent, extreme-ultraviolet (XUV) photon bursts obtained through laser high-harmonic generation have opened up new possibilities in the study of atomic and molecular dynamics. We discuss experiments elucidating some of the interesting energy redistribution mechanisms that follow the interaction of a high-energy photon with a molecule. The crucial role of synchronized, strong-field, near-IR laser pulses in XUV pump-probe spectroscopy is highlighted. We demonstrate that near-IR pulses can in fact be used to modify the atomic structure and control the electronic dynamics on attosecond timescales. Our measurements show that the Gouy phase slip in the interaction region plays a significant role in these attosecond experiments. We perform precision measurement of interferences between strong field-induced Floquet channels to extract the intensity and phase dependence of photoionization dynamics. Applications of emerging table-top ultrafast XUV sources in the study of core electron dynamics are also discussed.

Modelling beam-transport diffraction in near-infrared few-cycle strong-field experiments

Few-cycle high peak power laser pulses produced in gas-filled hollow fibres have a EH11 Bessel mode. Control of the intensity and phase-matching conditions requiring no additional dispersion is introduced, and is often achieved by closing a hard aperture around the beam. We use the Huygens–Fresnel diffraction integral to propagate such a beam through a numerical model of a typical attosecond beamline, quantifying the distribution of spatial intensity and the shape of the wavefront through the focal volume as the beam is truncated by finite-diameter optics. State-of-the-art attosecond and single-harmonic experiments combining the fundamental NIR with high-harmonic XUV radiation also employ annular optics, again as material dispersion must be avoided. We simulate the additional changes to wavefront shape and spatial intensity distribution on reflection from a spherical annular mirror for a range of annulus and aperture sizes. Finally we predict the change in intensity and focal position as the aperture is reduced. The model's usefulness as a tool for optimisation of an experimental beamline is therefore highlighted.

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.

A semi-classical model of attosecond electron localization in dissociative ionization of hydrogen

In the development of attosecond molecular science, a series of experiments have recently been performed where ionic fragment asymmetries in the dissociative ionization of H(2) into H(+) + H and that of D(2) into D(+) + D were used to uncover electron localization processes that occur on the attosecond and few-femtosecond timescale. Electron localization was observed both in strong-field dissociative ionization using carrier envelope phase-stable few-cycle laser pulses [Kling et al., Science, 2006, 312, 246] and in a two-color extreme ultra-violet + infrared attosecond pump-probe experiment [Sansone et al., Nature, 2010, 465, 763]. Here we show that the observed electron localization can be well understood using a semi-classical model that describes the dynamics in terms of quasi-static states that take the interaction of the molecule with the laser field instantaneously into account. The electron localization is shown to be determined by the passage of the dissociating molecule through a regime where the laser-molecule interaction is neither diabatic nor adiabatic.

Tunable frequency-controlled isolated attosecond pulses characterized by either 750 nm or 400 nm wavelength streak fields

A compact and robust Mach-Zehnder type interferometer coupled with the double optical gating technique provides tunable isolated attosecond pulses and streak field detection with fields centered at either 750 nm or 400 nm. Isolated attosecond pulses produced at 45 eV (with measured pulse duration of 114 ± 4 as) and 20 eV (with measured pulse duration of 395 ± 6 as) are temporally characterized with a 750 nm wavelength streak field. In addition, an isolated 118 ± 10 as pulse at 45 eV is measured with a 400 nm wavelength streak field. The interferometer design used herein provides broad flexibility for attosecond streak experiments, allowing pump and probe pulses to be specified independently. This capability is important for studying selected electronic transitions in atoms and molecules.

Gating attosecond pulse train generation using multicolor laser fields

The process of high-order harmonic generation leads to the production of a train of attosecond-duration extreme ultraviolet (XUV) pulses, with one pulse emitted per optical half-cycle. For attosecond pump-probe experiments, a single, isolated attosecond pulse is preferable, requiring an almost continuous spectrum. We show experimentally and numerically that the addition of a second laser field, and later a third, at a noncommensurate frequency relative to the driving field can modify the subcycle shape of the electric field, leading to the appearance of additional spectral components between the usual odd harmonics and in some cases a quasicontinuum. We perform a parametric study of the frequency ratio between the two first laser fields, the result of which is in good agreement with theoretical selection rules. We also show numerically that using three laser frequencies from an optical parametric amplifier can achieve a single attosecond pulse from a 24-fs laser pulse.

Delay control in attosecond pump-probe experiments

The time delay between the pump and probe pulses in attosecond time-resolved experiments, such as attosecond streaking, is commonly introduced by splitting and recombining the two pulses in an interferometer. This technique suffers from instability in the optical path lengths of the two arms due to mechanical vibration of the optical elements and fluctuating environmental conditions. We present a technique with which the instability of the unconventional interferometer is suppressed while at the same time the time delay is controlled to within 20 as RMS using a feedback loop. Using this scheme, the streaked spectrogram of an attosecond pulse was measured.

Design, fabrication, and analysis of chirped multilayer mirrors for reflection of extreme-ultraviolet attosecond pulses

Chirped Mo/Si multilayer coatings have been designed, fabricated, and characterized for use in extreme-ultraviolet attosecond experiments. By numerically simulating the reflection of the attosecond pulse from a multilayer mirror during the optimization procedure based on a genetic algorithm, we obtain optimized layer designs. We show that normal incidence chirped multilayer mirrors capable of reflecting pulses of approximately 100 attoseconds (as) duration can be designed by enhancing the reflectivity bandwidth and optimizing the phase-shift behavior. The chirped multilayer coatings have been fabricated by electron-beam evaporation in an ultrahigh vacuum in combination with ion-beam polishing of the interfaces and in situ reflectivity measurement for layer thickness control. To analyze the aperiodic layer structure by hard-x-ray reflectometry, we have developed an automatic fitting procedure that allows us to determine the individual layer thicknesses with an error of less than 0.05 nm. The fabricated chirped mirror may be used for production of 150-160 as pulses.