Practical aspects of the robust method we recently proposed for producing few-cycle attosecond pulses with arbitrary waveform in the extreme ultraviolet spectral range are studied numerically. It is based on the undulator radiation of relativistic ultrathin electron layers produced by inverse free-electron laser process. Optimal conditions for nanobunching are given; attosecond pulse energy and waveform, and their stability are studied. For K=0.8 undulator parameter, carrier-envelope-phase stable pulses with >45 nJ energy and 80 as duration at 20 nm, and >250 nJ energy and 240 as duration at 60 nm are predicted with 31 mrad and 13 mrad phase stability, respectively.
An intuitive physical mechanism for single attosecond pulse generation in multi-cycle pulse regime is proposed. We suggest that the continuum spectra of HHG can be controlled through the modulation of carrier wave, while keeping the multi-cycle envelope unchanged approximately. By increasing the time interval between the adjacent maximum return kinetic energy peaks, the kinetic energy of the side peaks will be apparently suppressed by the multi-cycle envelope. The photons with energies near the cutoff burst only at the pulse center with high coherence, which contribute to the generation of sin…
Advancing table-top attosecond sources in brightness and pulse duration is of immense interest and importance for an expanding sphere of applications. Recent theoretical studies [New J. Phys., 22 093030 (2020)] have found that high-order frequency mixing (HFM) in a two-color laser field can be much more efficient than high-order harmonic generation (HHG). Here we study the attosecond properties of the coherent XUV generated via HFM analytically and numerically, focusing on the practically important case when one of the fields has much lower frequency and much lower intensity than the other one…
Two- and multi-dimensional spectroscopy is used in physics and chemistry to obtain structural and dynamical information that would otherwise be invisible by the projection into a one-dimensional data set such as a single emission or absorption spectrum. Here, we introduce a qualitatively new two-dimensional spectroscopy method by employing the carrier-envelope phase (CEP). Instead of measuring spectral vs. spectral information, the combined application of spectral interferometry and CEP control allows the measurement of otherwise inseparable temporal events on an attosecond time scale. As a sp…
A proposal for a novel source of isolated attosecond XUV -- soft X-ray pulses with a well controlled carrier-envelope phase difference (CEP) is presented in the framework of nonlinear Thomson-backscattering. Based on the analytic solution of the Newton-Lorentz equations, the motion of a relativistic electron is calculated explicitly, for head-on collision with an intense fs laser pulse. By using the received formulae, the collective spectrum and the corresponding temporal shape of the radiation emitted by a mono-energetic electron bunch can be easily computed. For certain suitable and realisti…
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…
Infrared femtosecond laser pulses are important tools both in strong-field physics, driving X-ray high-harmonic generation, and as the basis for widely tuneable, if inefficient, ultrafast sources in the visible and ultraviolet. Although anomalous material dispersion simplifies compression to few-cycle pulses, attosecond pulses in the infrared have remained out of reach. We demonstrate soliton self-compression of 1800 nm laser pulses in hollow capillary fibers to sub-cycle envelope duration (2 fs) with 27 GW peak power, corresponding to attosecond field transients. In the same system, we genera…
Laser-plasma accelerators (LPAs), producing high-quality electron beams, provide an opportunity to reduce the size of free-electron lasers (FELs) to only a few meters. A complete system is proposed here, which is based on FEL technology and consists of an LPA, two undulators, and other magnetic devices. The system is capable to generate carrier-envelope phase stable attosecond pulses with engineered waveform. Pulses with up to~60~nJ energy and 90 to~400~attosecond duration in the 30 to 120~nm wavelength range are predicted by numerical simulation. These pulses can be used to investigate ultraf…
We have investigated the polarization of attosecond light bursts generated by nanobunches of electrons from relativistic few-cycle laser pulse interaction with the surface of overdense plasmas. Particle-in-cell simulation shows that the polarization state of the generated attosecond burst depends on the incident-pulse polarization, duration, carrier envelope phase, as well as the plasma scale length. Through laser and plasma parameter control, without compromise of generation efficiency, a linearly polarized laser pulse with azimuth $θ^i=10^\circ$ can generate an elliptically polarized attosec…
The ability to measure and control the carrier envelope phase (CEP) of few-cycle laser pulses is of paramount importance for both frequency metrology and attosecond science. Here, we present a phase meter relying on the CEP-dependent photocurrents induced by circularly polarized few-cycle pulses focused between electrodes in ambient air. The new device facilitates compact single-shot, CEP measurements under ambient conditions and promises CEP tagging at repetition rates orders of magnitude higher than most conventional CEP detection schemes as well as straightforward implementation at longer w…
Non-perturbative and phase-sensitive light-matter interactions have led to the generation of attosecond pulses of light and the control electrical currents on the same timescale. Traditionally, probing these effects via high harmonic generation has involved complicated lasers and apparatuses to generate the few-cycle and high peak power pulses needed to obtain and measure spectra that are sensitive to the phase of the light wave. Instead, we show that nonlinear effects dependent on the carrier-envelope phase can be accessed in solid state crystals with simple low-energy frequency combs that we…
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…
We report theoretical calculations of high-order harmonic generation (HHG) of Xe with the inclusion of multi-electron effects and macroscopic propagation of the fundamental and harmonic fields in an ionizing medium. By using the time-frequency analysis we show that the reshaping of the fundamental laser field is responsible for the continuum structure in the HHG spectra. We further suggest a method for obtaining an isolated attosecond pulse (IAP) by using a filter centered on axis to select the harmonics in the far field with different divergence. We also discuss the carrier-envelope-phase dep…
Based on the dual-chirped optical parametric amplification and type-I BiB$_3$O$_6$(BiBO) crystals, the generation of $>$100 mJ, 10.4 fs, 10 Hz, carrier-to-envelope phase (CEP)-stable laser pulses, which are centered at 1.7 $μ$m, is demonstrated; it produces a peak power of 10 TW. CEP-dependent high harmonic generation is implemented to confirm the sub-two-cycle pulse duration and CEP stabilization of infrared (IR) laser pulses. As far as we know, the obtained pulse energy and peak power represent the highest values for sub-two-cycle CEP-stable IR optical parametric amplification. Additionally,…
Relativistic surface high harmonics have been considered a unique source for the generation of intense isolated attosecond pulses in the extreme ultra-violet (XUV) and X-ray spectral range. However, its experimental realization is still a challenging task requiring identification of the optimum conditions for the generation of isolated attosecond pulses as well as their temporal characterization. Here, we demonstrate measurements in both directions. Particularly, we have made a first step towards the temporal characterization of the emitted XUV radiation by adapting the attosecond streak camer…
Sharp metallic nanotapers irradiated with few-cycle laser pulses are emerging as a source of highly confined coherent electron wavepackets with attosecond duration and strong directivity. The possibility to steer, control or switch such electron wavepackets by light is expected to pave the way towards direct visualization of nanoplasmonic field dynamics and real-time probing of electron motion in solid state nanostructures. Such pulses can be generated by strong-field induced tunneling and acceleration of electrons in the near-field of sharp gold tapers within one half-cycle of the driving las…
Occupation-Driven emission asynchronous as a Fundamental Constraint on Solid-State Attosecond Pulses
State Key Laboratory of Semiconductor Physics and Chip Technologies, Institute of Semiconductors, Chinese Academy of Sciences（中国科学院半导体研究所）；Center of Material Science and Optoelectronics Engineering, University of Chinese Academy of Sciences（中国科学院大学物质科学与光电技术学院）
We present experimental results showing the appearance of a near-continuum in the high-order harmonic generation (HHG) spectra of atomic and molecular species as the driving laser intensity of an infrared pulse increases. Detailed macroscopic simulations reveal that these near-continuum spectra are capable of producing IAPs in the far field if a proper spatial filter is applied. Further, our simulations show that the near-continuum spectra and the IAPs are a product of strong temporal and spatial reshaping (blue shift and defocusing) of the driving field. This offers a possibility of producing…
Full coherent soft X-ray attosecond pulses are now available through high-order harmonic generation (HHG); however, its insufficient output energy hinders various applications, such as attosecond-scale soft X-ray nonlinear experiments, the seeding of soft X-ray free-electron lasers, attosecond-pump-attosecond-probe spectroscopies, and single-shot imaging. In this paper, towards the implementation of these exciting studies, we demonstrate a soft X-ray harmonic beam that is more than two orders of magnitudes stronger up to the water window region compared to previous works. This was achieved by …
Shot-noise-limited few-cycle mid-infrared frequency comb with attosecond phase stability
Wrocław University of Science and Technology（弗罗茨瓦夫理工大学）；University of Warsaw（华沙大学）；Center for Molecular Fingerprinting Research（分子指纹研究中心）；Max-Planck-Institute of Quantum Optics（马克斯·普朗克量子光学研究所）
Photoemission driven by a strong electric field of near-infrared or visible light, referred to as strong-field photoemission, produces attosecond electron pulses that are synchronized to the waveform of the incident light, and this principle lies at the heart of current attosecond technologies. However, full access to strong-field photoemission regimes at near-infrared wavelengths based on solid-state materials is restricted by space-charge screening and material damage at high optical-field strengths, which significantly hampers the realization of predicted attosecond technologies, such as ul…
Reducing the Carrier-Envelope-Phase-dependence of High-Harmonic-Generation by Vectorial-Time-Polarization-Gating
Raymond and Beverly Sackler Faculty of Exact Sciences, School of Chemistry, Tel Aviv University（特拉维夫大学理学院化学系）；Tel-Aviv University Center for Light-Matter-Interaction（特拉维夫大学光物质相互作用中心）
Carrier-envelope phase (CEP) detection of ultrashort optical pulses and low-energy waveform field sampling have recently been demonstrated using direct time-domain methods that exploit optical-field photoemission from plasmonic nanoantennas. These devices make for compact and integratable solid-state detectors operating at optical frequency that work in ambient conditions and require minute pulse energies (picojoule-level). Applications include frequency-comb stabilization, visible to near-infrared time-domain spectroscopy, compact tools for attosecond science and metrology and, due to the hig…
Attosecond pulses in the soft-X-ray (SXR) to water-window energy region offer the tools for creating and studying target specific localized inner-shell electrons or holes in materials, enable monitoring or controlling charge and energy flows in a dynamic system on attosecond timescales. Recently, a number of laboratories have reported generation of continuum harmonics in the hundred-electron-volt to kilovolt region with few-cycle long-wavelength mid-infrared lasers. These harmonics have the bandwidth to support pulses with duration of few- to few-ten attoseconds. But harmonics generated in a g…
We report on tunnel ionization of Xe by 2-cycle, intense, infrared laser pulses and its dependence on carrier-envelope-phase (CEP). At low values of optical field ($E$), the ionization yield is maximum for cos-like pulses with the dependence becoming stronger for higher charge states. At higher $E$-values, the CEP dependence either washes out or flips. A simple phenomenological model is developed that predicts and confirms the observed results. CEP effects are seen to persist for 8-cycle pulses. Unexpectedly, electron rescattering plays an unimportant role in the observed CEP dependence. Our r…
The bottleneck for an attosecond science experiment is concluded to be the lack of a high-peak-power isolated attosecond pulse source. Therefore, currently, generating an intense attosecond pulse would be one of the highest priority goals. In this paper, we review a TW-class parallel three-channel waveform synthesizer for generating a gigawatt-scale soft-x-ray isolated attosecond pulse (IAP) using high-order harmonics generation (HHG). Simultaneously, using several stabilization methods, namely, the low-repetition-rate laser carrier-envelope phase stabilization, Mach-Zehnder interferometer, ba…
Few-cycle pulsed laser technology highlights the need for control and stabilization of the carrier-envelope phase (CEP) for applications requiring shot-to-shot timing and phase consistency. This general requirement has been achieved successfully in a number of free space and fiber lasers via feedback and feed-forward methods. Expanding upon existing results, we demonstrate CEP stabilization through the feed-forward method applied to a SESAM mode-locked Er:Yb:glass laser at 1.55 um with a measured ultralow timing jitter of 2.9 as (1 Hz - 3 MHz) and long-term stabilization over a duration of eig…
A stable 50 mJ three-channel optical waveform synthesizer is demonstrated and used to reproducibly generate a high-order harmonics supercontinuum in the soft-x-ray region. This synthesizer is composed of pump pulses from a 10-Hz-repetition-rate Ti:sapphire pump laser and signal and idler pulses from an infrared two-stage optical parametric amplifier driven by this pump laser. With the full active stabilization of all relative time delays, relative phases, and the carrier-envelope phase, a shot-to-shot stable intense continuum harmonic spectrum is obtained around 60 eV with pulse energy above 0…
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 …
Measuring the time it takes to remove an electron from an atom or molecule during photoionization using newly developed attosecond spectroscopies has been a focus of many recent experiments. However, the outcome of such measurement depends on measurement protocols and specific observables available in each particular experiment. One of such protocols relies on high harmonic generation. First, we derive rigorous and general expressions for ionization and recombination times in high harmonic generation experiments. We show that these times are different from, but related to ionization times meas…
Given the quasi-static nature of optical-field emission and the nontrivial dependence of the emission rate on the instantaneous electric field strength, the CEP-sensitive component of the emitted photocurrent is highly sensitive to the energy of the optical pulse, and should carry information about the underlying sub-cycle dynamics of electron emission. Here we examine CEP-sensitive photoemission from plasmonic gold nanoantennas excited with few-cycle optical pulses of increasing energy. We observe antiresonance-like features in the CEP-sensitive photocurrent; specifically, at a critical pulse…
Carrier-Envelope Phase Control of Orbital Angular Momentum in Solid-State High-Harmonic Generation
Eastern Institute of Technology（东方理工学院）；ELI ALPS, The Extreme Light Infrastructure ERIC（ELI ALPS，极端光基础设施欧洲利益相关者实体）；Theoretisch-Physikalisches Institut, Friedrich-Schiller-Universität Jena（耶拿弗里德里希·席勒大学理论物理研究所）；Laboratoire Photonique Numérique et Nanosciences (LP2N), UMR 5298, CNRS-IOGS-Université Bordeaux（数字光子学与纳米科学实验室（LP2N），UMR 5298，法国国家科学研究中心-高等光学学校-波尔多大学）；Centro de Investigaciones en Óptica, A.C.（光学研究中心）
The interaction of ultra-intense laser pulses with an underdense plasma is used in laser-plasma acceleration to create compact sources of ultrashort pulses of relativistic electrons and X-rays. The accelerating structure is a plasma wave, or wakefield, that is excited by the laser ponderomotive force, a force that is usually assumed to depend solely on the laser envelope and not on its exact waveform. Here, we use near-single-cycle laser pulses with a controlled carrier-envelope-phase (CEP) to show that the actual waveform of the laser field has a clear impact on the plasma response. We measur…
Ultrafast light-matter interactions lead to optical-field-driven photocurrents with an attosecond-level temporal response. These photocurrents can be used to detect the carrier-envelope-phase (CEP) of short optical pulses, and could be utilized to create optical-frequency, petahertz (PHz) electronics for information processing. Despite recent reports on optical-field-driven photocurrents in various nanoscale solid-state materials, little has been done in examining the large-scale integration of these devices. In this work, we demonstrate enhanced, on-chip CEP detection via optical-field-driven…
We report a newly designed mid-infrared-pump visible-probe measurement system, which can measure phase-sensitive responses to a mid-infrared pulse along the oscillating electromagnetic field. In this system, the pump light is a phase-locked mid-infrared pulse with temporal width of 100 fs, which is produced via difference frequency generation (DFG) from two idler pulses of two optical parametric amplifiers (OPAs) that are excited by the same Ti:sapphire regenerative amplifier. The probe pulse is a visible pulse with temporal width of 9 fs, and it is generated from a custom-built non-collinear …
BGGSe is a newly developed nonlinear material that is attractive for ultrabroad frequency mixing and ultrashort pulse generation due to its comparably low dispersion and high damage threshold.In a first experiment, we show that a long crystal length of 2.6 mm yields a pulse energy of 21 pJ at 100 MHz with a spectral bandwidth covering 5.8 to 8.5 microns. The electric field of the carrier-envelope-phase stable pulse is directly measured with electro-optical sampling and reveals a pulse duration of 91 fs, which corresponds to sub-four optical cycles, thus confirming some of the prospects of the …
Neural networks are a prominent tool for identifying and modeling complex patterns, which are otherwise hard to detect and analyze. While machine learning and neural networks have been finding applications across many areas of science and technology, their use in decoding ultrafast dynamics of quantum systems driven by strong laser fields has been limited so far. Here we use deep neural networks to analyze simulated noisy spectra of highly nonlinear optical response of a 2-dimensional gapped graphene crystal to intense few-cycle laser pulses. We show that a computationally simple 1-dimensional…
The availability of intense, ultrashort coherent radiation sources in the infrared region of the spectrum is enabling the generation of attosecond X-ray pulses via high harmonic generation, pump-probe experiments in the "molecular fingerprint" region and opening up the area of relativistic-infrared nonlinear optics of plasmas. These applications would benefit from multi-millijoule single-cycle pulses in the mid to long wavelength infrared (LW-IR) region. Here we present a new scheme capable of producing tunable relativistically intense, single-cycle infrared pulses from 5-14$μ$m with a 1.7% co…
Studies of strong field ionization have historically relied on the strong field approximation, which neglects all spatial dependence in the forces experienced by the electron after ionization. More recently, the small spatial inhomogeneity introduced by the long-range Coulomb potential has been linked to a number of important features in the photoelectron spectrum, such as Coulomb asymmetry, Coulomb focusing, and the low energy structure (LES). Here, we demonstrate by combined quantum and classical simulations that a small time-varying spatial dependence in the laser electric field creates a p…
