Praveen Kumar Maroju, Cesare Grazioli, Michele Di Fraia, Matteo Moioli, Dominik Ertel, Hamed Ahmadi, Oksana Plekan, Paola Finetti, Enrico Allaria, Luca Giannessi, Giovanni De Ninno, Carlo Spezzani, Giuseppe Penco, Alexander Demidovich, Miltcho Danailov, Roberto Borghes, Georgios Kourousias, Carlos Eduardo Sanches Dos Reis, Fulvio Billé, Alberto A. Lutman, Richard J. Squibb, Raimund Feifel, Paolo Carpeggiani, Maurizio Reduzzi, Tommaso Mazza, Michael Meyer, Samuel Bengtsson, Neven Ibrakovic, Emma Rose Simpson, Johan Mauritsson, Tamás Csizmadia, Mathieu Dumergue, Sergei Kühn, Harshitha N. G., Daehyun You, Kiyoshi Ueda, Marie Labeye, Jens Egebjerg Bækhøj, Kenneth J. Schafer, Elena V. Gryzlova, Alexei N. Grum-Grzhimailo, Kevin C. Prince, Carlo Callegari, Giuseppe Sansone
Attosecond pulses are fundamental for the investigation of valence and core-electron dynamics on their natural timescale. At present the reproducible generation and characterisation of attosecond waveforms has been demonstrated only through the process of high-order harmonic generation. Several methods for the shaping of attosecond waveforms have been proposed, including metallic filters, multilayer mirrors and manipulation of the driving field. However, none of these approaches allow for the flexible manipulation of the temporal characteristics of the attosecond waveforms, and they suffer from the low conversion efficiency of the high-order harmonic generation process. Free Electron Lasers, on the contrary, deliver femtosecond, extreme ultraviolet and X-ray pulses with energies ranging from tens of $\mathrmμ$J to a few mJ. Recent experiments have shown that they can generate sub-fs spikes, but with temporal characteristics that change shot-to-shot. Here we show the first demonstration of reproducible generation of high energy ($\mathrmμ$J level) attosecond waveforms using a seeded Free Electron Laser. We demonstrate amplitude and phase manipulation of the harmonic components of an attosecond pulse train in combination with a novel approach for its temporal reconstruction. The results presented here open the way to perform attosecond time-resolved experiments with Free Electron Lasers.
A model is presented which demonstrates that the attosecond pulse structure of a High Harmonic Generation (HHG) seed may be retained through to saturation in an FEL amplifier. At wavelengths of ~12nm a train of attosecond pulses of widths ~300 attoseconds with peak powers in excess of 1 GW are predicted from full 3D simulation. Methods for improving these results are discussed.
We propose a method for programmable shaping of the amplitude and phase of the XUV and x-ray attosecond pulses produced by high-order harmonic generation. It overcomes the bandwidth limitations of existing spectral filters and enables removal of the intrinsic attosecond chirp as well as the synthesis of pulse sequences. It is based on partial phase matching, such as quasi-phase matching, using a longitudinally addressable modulation.
We study high-order harmonic generation (HHG) driven by seeded plasmonic-enhanced fields. On one hand, plasmonic-enhanced fields have shown a great potential to extend the HHG cutoff, an instrumental pre-requisite for the generation of attosecond pulses. On another hand, the use of XUV seeds appears to have a considerable potential to improve the HHG conversion efficiency, which is typically modest when a unique fundamental laser pulse is employed. By mixing these two sources, we show it is possible to, simultaneously, boost the HHG cutoff and to increase the harmonic photon flux. The combinat…
Attosecond pulses created by high-order harmonic generation in gases often exhibit strong chromatic aberrations, arising from the broad bandwidth and wavelength-dependent nonlinear light-matter interaction. When the driving laser intensity varies spatially, as for Gaussian driving beams, the apparent source position of the harmonics differs significantly from one order to the next, thus affecting the achievable intensity and duration of the attosecond pulses when they are focused on a target. We show that these chromatic aberrations can be reduced by spatially shaping the fundamental beam to g…
We demonstrate the ability to control and shape the spectro-temporal content of extreme-ultraviolet (XUV) pulses produced by a seeded free-electron laser (FEL). The control over the spectro-temporal properties of XUV light was achieved by precisely manipulating the linear frequency chirp of the seed laser. Our results agree with existing theory, which allows retrieving the temporal properties (amplitude and phase) of the FEL pulse from measurements of the spectra as a function of the FEL operating parameters. Furthermore, we show the first direct evidence of the full temporal coherence of FEL …
Temporally shaping the density of electron beams using light forms the basis for a wide range of established and emerging technologies, including free-electron lasers and attosecond electron microscopy. The modulation depth of compressed electron pulses is a key figure of merit limiting applications. In this work, we present an approach for generating background-free attosecond electron pulse trains by sequential inelastic electron-light scattering. Harnessing quantum interference in the fractional Talbot effect, we suppress unwanted background density in electron compression by several orders…
We demonstrate control over attosecond pulse generation and shaping by numerically optimizing the synthesis of few-cycle to sub-cycle driver waveforms. The optical waveform synthesis takes place in an ultrabroad spectral band covering the ultraviolet-infrared domain. These optimized driver waves are used for ultrashort single and double attosecond pulse production (with tunable separation) revealing the potentials of the light wave synthesizer device demonstrated by Wirth et al. [Science 334, 195 (2011)]. The results are also analyzed with respect to attosecond pulse propagation phenomena.
High-repetition-rate attosecond pulse sources are indispensable tools of time-resolved studies of electron dynamics, such as coincidence spectroscopy and experiments with high demands on statistics or signal-to-noise ratio, especially in case of solid and big molecule samples in chemistry and biology. Although with the high-repetition-rate lasers such attosecond pulses in a pump-probe configuration are possible to achieve, until now only a few such light sources have been demonstrated. Here, by shaping the driving laser to an annular beam, a 100-kHz attosecond pulse train (APT) is reported wit…
We derive the analytical theory describing the process of sub-femtosecond pulse formation from a quasi-monochromatic seeding extreme ultraviolet (XUV) radiation, which propagates in active medium of a hydrogen-like plasma-based X-ray laser dressed by a strong infrared laser field. We discuss the ultimate capabilities and limitations of this process on the basis of the derived analytical solution and extensive numerical studies for the case of Li2+ plasma-based X-ray laser with a carrier wavelength 13.5nm. We analyze the role of plasma dispersion and find the optimal conditions for the formatio…
Single-cycle optical pulses with a controlled electromagnetic waveform allow to steer the motion of low-energy electrons in atoms, molecules, nanostructures or condensed-matter on attosecond dimensions in time. However, high-energy electrons under single-cycle light control would be an enabling technology for beam-based attosecond physics with free-electron lasers or electron microscopy. Here we report the control of freely propagating keV electrons with an isolated optical cycle of mid-infrared light and create a modulated electron current with a peak-cycle-specific sub-femtosecond structure …
Optical amplifiers in all ranges of the electromagnetic spectrum exhibit two essential characteristics: i) the input signal during the propagation in the medium is multiplied by the avalanche effect of the stimulated emission to produce exponential growth and ii) the amplification saturates at increasing input signal. We demonstrate that the strong-field theory in the frame of high harmonic generation fully supports the appearance of both the avalanche and saturation effects in the amplification of extreme ultraviolet attosecond pulse trains. We confirm that the amplification takes place only …
Sub-10-attosecond pulses with half-cycle electric fields provide exceptional options to detect and manipulate electrons in the atomic timescale. However, the availability of such pulses is still challenging. Here, we propose a method to generate isolated sub-10-attosecond half-cycle pulses based on a cascade process naturally happening in plasma. A 100s-attosecond pulse is first generated by shooting a moderate overdense plasma with a one-cycle femtosecond pulse. After that, the generated attosecond pulse cascadedly produce a sub-10-attosecond half-cycle pulse in the transmission direction by …
Shaping electron beams with the cycles of light provides femtosecond and attosecond time resolution in electron microscopy and enables fundamental quantum-coherent measurements. However, efficient light-electron control requires a prolonged interaction between the two beams for cascaded transfer of photon energy and momentum to the freely propagating electrons. Here we report the use of traveling evanescent terahertz waves to achieve velocity matching and thereby high acceleration gradients both in space and in time. With experiment and simulations, we demonstrate attosecond streaking, tempora…
Attosecond science promises to reveal the most fundamental electronic dynamics occurring in matter and it can develop further by meeting two linked technological goals related to high-order harmonic sources: higher photon flux (permitting to measure low cross-section processes) and improved spectral tunability (allowing selectivity in addressing specific electronic transitions). New developments come through parametric waveform synthesis, which provides control over the shape of high-energy electric field transients, enabling the creation of highly-tunable isolated attosecond pulses via high-h…
Numerical simulations are used to study how fiber supercontinuum generation seeded by picosecond pulses can be actively controlled through the use of input pulse modulation. By carrying out multiple simulations in the presence of noise, we show how tailored supercontinuum Spectra with increased bandwidth and improved stability can be generated using an input envelope modulation of appropriate frequency and depth. The results are discussed in terms of the non-linear propagation dynamics and pump depletion.
A method is proposed for arbitrarily engineering the high-order harmonic generation phase achieved by shaping a laser pulse and employing xuv light or x rays for ionization. This renders the production of bandwidth-limited attosecond pulses possible while avoiding the use of filters for chirp compensation. By adding the first 8 Fourier components to a sinusoidal field of $10^{16}$W/cm$^2$, the bandwidth-limited emission of 8 as is shown to be possible from a Li$^{2+}$ gas. The scheme is extendable to the zs-scale.
Broadband hard X-ray attosecond pulses from extremely chirped electron beams
SLAC National Accelerator Laboratory（斯坦福直线加速器中心）；Department of Applied Physics, Stanford University（斯坦福大学应用物理系）；Stanford PULSE Institute, SLAC National Accelerator Laboratory（斯坦福PULSE研究所，斯坦福直线加速器中心）
High-brightness sources of coherent and few-cycle-duration light waveforms with spectral coverage from the UV to the THz would offer unprecedented versatility and opportunities for a spectacular range of applications from bio-chemical sensing, to time-resolved and nonlinear spectroscopy, to attosecond light-wave electronics. Combinations of various sources with frequency conversion and supercontinuum generation can provide relatively large spectral coverage, but many applications require much broader spectral range and low-jitter synchronization for time-domain measurements. Here, we present a…
Controlling the wave function of free electrons is important to improve the spatial resolution of electron microscopes, the efficiency of electron interaction with sample modes of interest, and our ability to probe ultrafast materials dynamics at the nanoscale. In this context, attosecond electron compression has been recently demonstrated through interaction with the near fields created by scattering of ultrashort laser pulses at nanostructures followed by free electron propagation. Here, we show that control over electron pulse shaping, compression, and statistics can be improved by replacin…
Applications ranging from nonlinear terahertz spectroscopy to remote sensing require broadband and intense THz radiation which can be generated by focusing two-color laser pulses into a gas. In this setup, THz radiation originates from the buildup of the electron density in sharp steps of attosecond duration due to tunnel ionization, and subsequent acceleration of free electrons in the laser field. We show that the spectral shape of the THz pulses generated by this mechanism is determined by superposition of contributions from individual ionization events. This provides a straightforward analo…
XUV and X-ray Free Electron Lasers (FELs) produce short wavelength pulses with high intensity, ultrashort duration, well-defined polarization and transverse coherence, and have been utilised for many experiments previously possible at long wavelengths only: multiphoton ionization, pumping an atomic laser, and four-wave mixing spectroscopy. However one important optical technique, coherent control, has not yet been demonstrated, because Self- Amplified Spontaneous Emission FELs have limited longitudinal coherence. Single-colour pulses from the FERMI seeded FEL are longitudinally coherent, and t…
High harmonic generation (HHG) provides a flexible framework for the development of coherent light sources in the extreme-ultraviolet and soft x-ray regimes. However it suffers from low conversion efficiencies as the control of the HHG spectral and temporal characteristics requires manipulating electron trajectories on attosecond time scale. The phase matching mechanism has been employed to selectively enhance specific quantum paths leading to HHG. A few important fundamental questions remain open, among those how much of the enhancement can be achieved by the single-emitter and what is the ro…
High-Density Monocular 3D Particle Image Velocimetry by Wavefront Shaping and Deep Learning
Technion - Israel Institute of Technology（以色列理工学院）；Russell Berrie Nanotechnology Institute, Technion–Israel Institute of Technology（拉塞尔·贝里纳米技术研究所，以色列理工学院）
Laser-based preparation, manipulation, and readout of the states of quantum particles has become a powerful research tool that has enabled the most precise measurements of time, fundamental constants, and electromagnetic fields. Laser control of free electrons can improve the detection of electrons' interaction with material objects, thereby advancing the exploration of matter on the atomic scale. For example, temporal modulation of electron waves with light has enabled the study of transient processes with attosecond resolution. In contrast, laser-based spatial shaping of the electron wave fu…
