We use two fiber-based femtosecond frequency combs and a low-noise carrier suppression phase detection system to characterize the optical to microwave synchronization achievable with such frequency divider systems. By applying specific noise reduction strategies, a residual phase noise as low as -120 dBc/Hz at 1 Hz offset frequency from a 11.55 GHz carrier is measured. The fractional frequency instability from a single optical-to-frequency divider is 1.1E-16 at 1 s averaging down to below 2E-19 after only 1000 s. The corresponding rms time deviation is lower than 100 attoseconds up to 1000 s averaging duration.
The interaction of strong near-infrared (NIR) laser pulses with wide-bandgap dielectrics produces high harmonics in the extreme ultraviolet (XUV) wavelength range. These observations have opened up the possibility of attosecond metrology in solids, which would benefit from a precise measurement of the emission times of individual harmonics with respect to the NIR laser field. Here we show that, when high-harmonics are detected from the input surface of a magnesium oxide crystal, a bichromatic probing of the XUV emission shows a clear synchronization largely consistent with a semiclassical mode…
Synchronous laser-microwave networks delivering attosecond timing precision are highly desirable in many advanced applications, such as geodesy, very-long-baseline interferometry, high-precision navigation and multi-telescope arrays. In particular, rapidly expanding photon science facilities like X-ray free-electron lasers and intense laser beamlines require system-wide attosecond-level synchronization of dozens of optical and microwave signals up to kilometer distances. Once equipped with such precision, these facilities will initiate radically new science by shedding light on molecular and a…
We demonstrate an all-optical approach for precise characterization of attosecond extreme ultraviolet pulses. Isolated attosecond pulse is produced from high order harmonics using intense driving pulse with proper gating technique. When a weak field is synchronized with the driver, it perturbs the harmonics generation process via altering the accumulated phase of the electron trajectories. The perturbed harmonic spectrum can be formulated as a convolution of the unperturbed dipole and a phase gate, implying the validity of complete reconstruction of isolated attosecond pulses using conventiona…
We study theoretically the effect of the giant resonance in Xe on the phase difference between the consecutive high order resonantly-enhanced harmonics and calculate the duration of the attosecond pulses produced by these harmonics. For certain conditions resonantly-induced dephasing compensates the phase difference which is intrinsic for the off-resonance harmonics. We find these conditions analytically and compare them with the numerical results. This harmonic synchronization allows attosecond pulse shortening in conjunction with the resonance-induced intensity increase by more than an order…
Time-domain sampling of arbitrary electric fields with sub-cycle resolution enables a complete time-frequency analysis of a system's response to electromagnetic illumination. This provides access to dynamic information that is not provided by absorption spectra alone, and has recently been shown through measurements in the infrared that time-domain optical-field sampling offers significant improvements with regard to molecular sensitivity and limits of detection compared to traditional spectroscopic methods. Despite the many scientific and technological motivations, time-domain, optical-field …
Many experiments in attosecond science will benefit from attosecond pulses at high repetition rates with sufficient photon flux for pump-probe experiments. We use 7fs, 800nm pulses from a non-collinear optical parametric chirped pulse amplification (NOPCPA) laser system to generate few-pulse attosecond pulse trains (APTs) in the extreme ultraviolet (XUV) at a repetition rate of 100kHz. The pulse trains have been fully characterized by recording FROG-CRAB (Frequency-Resolved Optical Gating for Complete Reconstruction of Attosecond Bursts) traces with a velocity map imaging spectrometer.
Pulse trains emitted from dual-comb systems are designed to have low relative timing jitter, making them useful for many optical measurement techniques such as optical ranging and spectroscopy. However, the characterization of low-jitter dual-comb systems is challenging because it requires measurement techniques with high sensitivity. Motivated by this challenge, we developed a technique based on an optical heterodyne detection approach for measuring the relative timing jitter of two pulse trains. The method is suitable for dual-comb systems with essentially any repetition rate difference. Fur…
In this paper we present proof of principle experiments of an optical gating concept for free electrons. We demonstrate a temporal resolution of 1.2+-0.3 fs via energy and transverse momentum modulation as a function of time. The scheme is based on the synchronous interaction between electrons and the near-field mode of a dielectric nano-grating excited by a femtosecond laser pulse with an optical period duration of 6.5 fs. The sub-optical cycle resolution demonstrated here is promising for use in laser-driven streak cameras for attosecond temporal characterization of bunched particle beams as…
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…
An ultrafast anisotropic electro-optic effect of the zinc sulfide crystal is predicted employing a numerical pump-probe simulation. The numerical results indicate that the time-dependence of the anisotropic response of ZnS exhibits a phase shift with respect to the pump laser field. The phase shift coincides with the time-resolved dynamical Franz-Keldysh effect, which is the modulation of the isotropic part of the dielectric function. While the probe frequency dependence around the band gap is not intense, it becomes intense at higher photon energies of approximately 42~eV.
RIKEN Center for Advanced Photonics, RIKEN（理化学研究所先进光子学中心）；Xi’an Institute of Optics and Precision Mechanics, Chinese Academy of Sciences（中国科学院西安光学精密机械研究所）；University of Chinese Academy of Sciences（中国科学院大学）
An electrical pulse E(t) is completely defined by its time-dependent amplitude and polarisation direction. For optical pulses the manipulation and characterisation of the light polarisation state is fundamental due to its relevance in several scientific and technological fields. In this work we demonstrate the complete temporal reconstruction of the electric field of few-cycle pulses with a complex time-dependent polarisation. Our experimental approach is based on extreme ultraviolet interferometry with isolated attosecond pulses and on the demonstration that the motion of an attosecond electr…
Characterizing an isolated attosecond pulse (IAP) is essential for its potential applications. A complete characterization of an IAP ultimately requires the determination of its electric field in both time and space domains. However, previous methods, like the widely-used RABBITT and attosecond streaking, only measure the temporal profile of the attosecond pulse. Here we demonstrate an all-optical method for the measurement of the space-time properties of an IAP. By introducing a non-collinear perturbing pulse to the driving field, the process of IAP generation is modified both spatially and t…
ICFO – Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology（光子科学研究所，巴塞罗那科学技术研究院）；Atominstitut, Technische Universität Wien（原子研究所，维也纳工业大学）；Department of Physics and Astronomy, University College London（伦敦大学学院物理与天文系）；Attosecond Quantum Physics Laboratory, Department of Physics, King’s College London（伦敦国王学院物理系阿托秒量子物理实验室）
Interferometry, as the key technique in modern precision measurements, has been used for length diagnosis in the fields of engineering metrology and astronomy. Analogous interferometric technique for time domain precision measurement is a significant complement to the spatial domain applications and requires the manipulation of the interference on the extreme time and energy scale. Here we present an all-optical interferometry for high precision measurement with attosecond temporal and hundreds of meV energy resolution. The interferometer is based on laser driven high order harmonics which pro…
An optical fast-scan delay exploiting the near-collinear interaction between a train of ultrashort optical pulses and an acoustic wave propagating in a birefringent crystal is introduced. In combination with a femtosecond Er:fiber laser, the scheme is shown to delay few-fs pulses by up to 6 ps with a precision of 15 as. A resolution of 5 fs is obtained for a single sweep at a repetition rate of 34 kHz. This value can be improved to 39 as for multiple scans at a total rate of 0.3 kHz.
Ultrashort electron bunches are useful for applications like ultrafast imaging and coherent radiation production. Currently, however, the shortest achievable bunches, at attosecond time scales, have only been realized in the single or very few electron regime, limited by Coulomb repulsion and electron energy spread. Using ab initio simulations and theoretical analysis, we show that highly-charged bunches are achievable by subjecting relativistic (few MeV-scale) electrons to a superposition of terahertz and optical pulses. Using realistic electron bunches and laser pulse parameters which are wi…
University of Arizona（亚利桑那大学）；James C. Wyant College of Optical Sciences, University of Arizona（亚利桑那大学詹姆斯·C·怀恩特光学科学学院）；ICFO–Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology（ICFO-光子科学研究所，巴塞罗那科学技术研究院）；Department of Physics & Astronomy, University College London（伦敦大学学院物理与天文学系）
Enabling a multifunctional telecommunications fiber optic network: Ultrastable optical frequency transfer and attosecond timing in deployed multicore fiber
The use of optical clocks/oscillators in future ultra-precise navigation, gravitational sensing, coherent arrays, and relativity experiments will require time comparison and synchronization over terrestrial or satellite free-space links. Here we demonstrate full unambiguous synchronization of two optical timescales across a free-space link. The time deviation between synchronized timescales is below 1 fs over durations from 0.1 s to 6500 s, despite atmospheric turbulence and kilometer-scale path length variations. Over several days, the time wander is 40 fs peak-to-peak. Our approach relies on…
Optical frequency division (OFD) via optical frequency combs (OFC) has enabled a leap in microwave metrology leading to noise performance never explored before. Extending the method to millimeter-wave (mmW) and terahertz (THz)-wave domain is of great interest. Dissipative Kerr solitons (DKSs) in integrated photonic chips offer a unique feature of delivering OFCs with ultrahigh repetition rates from 10 GHz to 1 THz making them relevant gears to perform OFD in the mmW and THz-wave domain. We experimentally demonstrate OFD of an optically-carried 3.6 THz reference down to 300 GHz through a DKS, p…
Isolated attosecond spatio-temporal optical vortices: Interplay between the topological charge and orbital angular momentum scaling in high harmonic generation
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…
Optical chirality (OC) - one of the fundamental quantities of electromagnetic fields - corresponds to the instantaneous chirality of light. It has been utilized for exploring chiral light-matter interactions in linear optics, but has not yet been applied to nonlinear processes. Motivated to explore the role of OC in the generation of helically polarized high-order harmonics and attosecond pulses, we first separate the OC of transversal and paraxial beams to polarization and orbital terms. We find that the polarization-associated OC of attosecond pulses corresponds to that of the pump in the qu…
Multiphoton-ionized electrons are born into a strong light field that will determine their short-term future. By controlling the infrared beam, we enable atoms or molecules to generate extreme ultraviolet (XUV) pulses and synthesize attosecond pulses - the shortest controlled events ever produced. Here we show that a weak obliquely incident beam imposes an optical grating on the fundamental beam, resulting in a spatially modulated attosecond pulse. We observe the modulation on a spectrally resolved near-field XUV image, encoding all information of the spectral phase of the recollision electron…
Sub-laser cycle time scale of electronic response to strong laser fields enables attosecond dynamical imaging in atoms, molecules and solids. Optical tunneling and high harmonic generation are the hallmarks of attosecond imaging in optical domain, including imaging of phase transitions in solids. Topological phase transition yields a state of matter intimately linked with electron dynamics, as manifested via the chiral edge currents in topological insulators. Does topological state of matter leave its mark on optical tunneling and sub-cycle electronic response? We identify distinct topological…
Free space optical (FSO) communication channels are typically used to transmit high-speed data between sites over the air. Here we repurpose an FSO digital communication system and use it directly for two-way time transfer. We demonstrate real-time synchronization between two sites over a turbulent air path of 4 km using binary phase modulated CW laser light. Under synchronization, the two sites exhibit a fractional frequency deviation below $10^{-15}$ and a time deviation below 1 picosecond at averaging times of seconds to hours. Over an 8-hour period the peak to peak wander is 16 ps.
Atomic motion dynamics during structural changes or chemical reactions have been visualized by picosecond and femtosecond pulsed electron beams via ultrafast electron diffraction and microscopy. Imaging the even faster dynamics of electrons in atoms, molecules and solids requires electron pulses with sub-femtosecond durations. We demonstrate here the all-optical generation of trains of attosecond free-electron pulses. The concept is based on the periodic energy modulation of a pulsed electron beam via an inelastic interaction with the ponderomotive potential of an optical travelling wave gener…
Light-phase-sensitive techniques, such as coherent multidimensional spectroscopy, are well-established in a broad spectral range, already spanning from radio-frequencies in nuclear magnetic resonance spectroscopy to visible and ultraviolet wavelengths in nonlinear optics with table-top lasers. Here, the ability to tailor the phases of electromagnetic waves with high precision is essential. In the present contribution we achieve phase control of extreme-ultraviolet pulses from a free-electron laser (FEL) on the attosecond timescale in a Michelson-type all-reflective interferometric autocorrelat…
Weizmann Institute of Science（魏茨曼科学研究所）；Technion - Israel Institute of Technology（以色列理工学院）；Max Planck Institute for the Structure and Dynamics of Matter（马克斯·普朗克物质结构与动力学研究所）；Guangdong Technion-Israel Institute of Technology（广东以色列理工学院）
In the last decade, the development of Ultrafast Electron Diffraction (UED) and Microscopy (UEM) has enabled the imaging of atomic motion in real time and space. These pivotal table-top tools opened the door for a vast range of applications in different areas of science spanning chemistry, physics, materials science, and biology. We first discuss the basic principles and recent advancements, including some of the important applications, of both UED and UEM. Then, we discuss the recent advances in the field that have enhanced the spatial and temporal resolutions, where the latter, however, is s…
Field-emission of electrons underlies major advances in science and technology, ranging from imaging the atomic-scale structure of matter to signal processing at ever-higher frequencies. The advancement of these applications to their ultimate limits of temporal resolution and frequency calls for techniques that can confine and probe the field emission on the sub-femtosecond time scale. We used intense, sub-cycle transients to induce optical field emission of electron pulses from tungsten nanotips and a weak replica of the same transient to directly probe the emission dynamics in real-time. Acc…
The ability of spatial light modulators (SLMs) to modify the amplitude and phase of light has proved them invaluable to the optics and photonics community. In many applications the bit-depth of SLMs is a major limiting factor dictated by the digital processor. As a result, there is usually a compromise between refresh speed and bit-depth. Here we present a method to increase the effective bit-depth of SLMs which utilizes a linear slope as is commonly applied to deal with the zeroth order effect. This technique was tested using two interferometric transient absorption spectroscopy setups. Throu…
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 …
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…
The electro-optical properties of most semiconductors and insulators of technological interest are dominated by the presence of electron-hole quasiparticles called excitons. The manipulation of these hydrogen-like quasi-particles in dielectrics, has received great interest under the name excitonics that is expected to be of great potential for a variety of applications, including optoelectronics and photonics. A crucial step for such exploitation of excitons in advanced technological applications is a detailed understanding of their dynamical nature. However, the ultrafast processes unfolding …
