Extreme ultraviolet (XUV) transient absorption (TA) and transient reflectivity (TR) spectroscopies enable element-specific insights into attosecond-timescale processes in solids. XUV transient grating spectroscopy (TGS) is an emerging tool that combines the advantages of both absorption and reflectivity while offering intrinsically background-free detection. Here, we implement XUV-TGS by generating a transient grating in germanium solid using two few-cycle near-infrared pulses and probing it with an attosecond XUV pulse, produced via tabletop high-harmonic generation. The spectrally resolved, diffracted XUV pulses directly visualize the separate ultrashort decay times of both photoexcited electrons and holes, without the need for iterative deconvolution. By combining XUV-TA and -TG spectroscopy, we extract the evolution of the complex refractive index, ñ, without the need for Kramers-Kronig reconstruction, as required in XUV-TR, allowing us to extract the roots of the induced optical response. We find reflectivity changes of up to 34% via the real part of ñ, whereas changes in the imaginary part only result in a variation in reflectivity of around 0.5%.
We introduce a method for using Fizeau interferometry to measure the intrinsic resolving power of a diffraction grating. This method is more accurate than traditional techniques based on a long-trace profiler (LTP), since it is sensitive to long-distance phase errors not revealed by a d-spacing map. We demonstrate 50,400 resolving power for a mechanically ruled XUV grating from Inprentus, Inc.
Time- and Angle-resolved photoelectron spectroscopy from surfaces can be used to record the dynamics of electrons and holes in condensed matter on ultrafast time scales. However, ultrafast photoemission experiments using extreme-ultraviolet (XUV) light have previously been limited by either space-charge effects, low photon flux, or limited tuning range. In this article, we describe space-charge-free XUV photoelectron spectroscopy experiments with up to 5 nA of average sample current using a tunable cavity-enhanced high-harmonic source operating at 88 MHz repetition rate. The source delivers $ …
We present a table-top extreme ultraviolet (XUV) beamline for measuring time- and frequency-resolved XUV excited optical luminescence (XEOL) with additional femtosecond-resolution XUV transient absorption spectroscopy functionality. XUV pulses are generated via high-harmonic generation using a near-infrared pulse in a noble gas medium, and focused to excite luminescence from a solid sample. The luminescence is collimated and guided into a streak camera, where its spectral components are temporally resolved with picosecond temporal resolution. We time-resolve XUV excited luminescence and compar…
Active Control of Extreme Ultraviolet Photon Flux and Resolution with a Plane Ruled Reflection Grating Spectrometer that Measures Diverging High-Harmonics
We present a theoretical study of transient absorption and reshaping of extreme ultraviolet (XUV) pulses by helium atoms dressed with a moderately strong infrared (IR) laser field. We formulate the atomic response using both the frequency-dependent absorption cross section and a time-frequency approach based on the time-dependent dipole induced by the light fields. The latter approach can be used in cases when an ultrafast dressing pulse induces transient effects, and/or when the atom exchanges energy with multiple frequency components of the XUV field. We first characterize the dressed atom r…
The high-order harmonic generation (HHG), if phase matched, opens a unique way to produce coherent ultrafast extreme-UV (XUV) or soft x-ray light sources. Here we describe a robust and tunable method for scaling and narrowing the bandwidth of high-order harmonics in different transversal modes based on femtosecond dynamic grating in a gas jet. This technique has potential of self-phase controlled XUV generation by adjusting the intersect angle and the intensity ratio of interfering fundamental beams. The limitations of using high intensity laser fundamental pulses in gas, such as non-negligibl…
We present the main features of CITIUS, a new light source for ultrafast science, generating tunable, intense, femtosecond pulses in the spectral range from IR to XUV. The XUV pulses (about 10^5-10^8 photons/pulse in the range 14-80 eV) are produced by laser-induced high-order harmonic generation in gas. This radiation is monochromatized by a time-preserving monochromator, allowing also to work with high-resolution bandwidth selection. The tunable IR-UV pulses (10^{12}-10^{15} photons/pulse in the range 0.4-5.6 eV) are generated by an optical parametric amplifier, which is driven by a fraction…
Ultrafast light sources have become an indispensable tool to access and understand transient phenomenon in material science. However, a simple and easy-to-implement method for harmonic selection, with high transmission efficiency and pulse duration conservation, is still a challenge. Here we showcase and compare two approaches for selecting the desired harmonic from a high harmonic generation source while achieving the above goals. The first approach is the combination of extreme ultraviolet spherical mirrors with transmission filters and the second approach uses a normal-incidence spherical g…
Ultrafast excitation of Bloch plasmon polaritons in hyperbolic metamaterials with an extreme ultra-violet transient grating
Umeå University（于默奥大学）；Elettra Sincrotrone Trieste（的里雅斯特同步辐射中心）；CIC nanoGUNE BRTA（nanoGUNE研究中心）；Ikerbasque, Basque Foundation for Science（伊卡巴斯克，巴斯克科学基金会）；Università degli Studi di Modena e Reggio Emilia（摩德纳和雷焦艾米利亚大学）；Wallenberg Initiative Materials Science for Sustainability（瓦伦堡可持续材料科学倡议）
Experiments on the excitation of propagating surface plasmons (SPs) by ultrashort, high intensity laser interaction with "grating" targets are reviewed. At intensities exceeding $10^{19}~\mbox{W cm}^{-2}$ on target, i.e. in the strongly relativistic regime of electron dynamics, multi-MeV electrons are accelerated by the SP field as dense bunches collimated in a near-tangent direction. By the use of a suitable blazed grating, the bunch charge can be increased up to $\simeq $660 picoCoulomb. Intense XUV high harmonics (HH) diffracted by the grating are observed when a plasma with sub-micrometer …
We have developed low-dispersion (1480 l/mm), resonance-free, diffraction gratings made of dielectric materials resistant to femtosecond laser damage $(SiO_{2}/HfO_{2})$. A 14 cm diameter sample was fabricated resulting in a mean diffraction efficiency of 99.1% at λ = 810 nm with 0.4% uniformity using equipment which can fabricate gratings up to 1m diagonal. The implementation of these gratings in the compression of 30 fs pulses in an out-of-plane geometry can result in compressor efficiencies of ~95%. The measured laser absorption is 500x lower than current ultrafast petawatt-class compressor…
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…
Diffusion of heat in metals is a fundamental process which is crucial for a variety of applications of metal nanostructures. Surprisingly, however, {\em ultrafast} heat diffusion received only limited attention so far. Here, we show that heat diffusion can be made faster than $e-ph$ energy transfer rate, in which case, it dominates the spatio-temporal dynamics of the temperature. This enables the metals to overcome the conventional limitations of the nonlinear optical response of materials - it can be simultaneously fast and strong. As a specific example, we identify the underlying (femtosecon…
Modern nonlinear optical materials allow light of one wavelength be efficiently converted into light at another wavelength. However, designing nonlinear optical materials to operate with ultrashort pulses is difficult, because it is necessary to match both the phase velocities and group velocities of the light. Here we show that self-organized nonlinear gratings can be formed with femtosecond pulses propagating through nanophotonic waveguides, providing simultaneous group-velocity matching and quasi-phase-matching for second harmonic generation. We record the first direct microscopy images of …
Ultrafast phenomena on a femtosecond timescale are commonly examined by pump-probe experiments. This implies multiple measurements where the sample under investigation is pumped with a short light pulse and then probed with a second pulse at various time delays to follow its dynamics. Recently, the principle of streaking extreme ultraviolet (XUV) pulses in the temporal domain has enabled recording the dynamics of a system within a single pulse. However, separate pump-probe experiments at different absorption edges still lack a unified timing, when comparing the dynamics in complex systems. Her…
The peak power improvement and running safety of petawatt (PW) lasers are limited by laser-induced damage of optical components with limited sizes and damage thresholds. Diffraction gratings in pulse compressors have been the shortest stave of PW lasers up to now, as to manufacture a high quality meter-sized grating remains particularly challenging. Here, the asymmetric four-grating compressor (AFGC) with asymmetric configuration is proposed for PW lasers to increase the maximum bearable output pulse energy and running safety without neither additional optical component nor extra control in co…
High harmonic generation (HHG) enables coherent extreme-ultraviolet (XUV) radiation with ultra-short pulse duration in a table-top setup. This has already enabled a plethora of applications. Nearly all of these applications would benefit from a high photon flux to increase the signal-to-noise ratio and decrease measurement times. In addition, shortest pulses are desired to investigate fastest dynamics in fields as diverse as physics, biology, chemistry and material sciences. In this work, the up-to-date most powerful table-top XUV source with 12.9 mW in a single harmonic line at 26.5 eV is dem…
Ultrafast laser inscription (ULI) is a rapidly maturing technique which uses focused ultrashort laser pulses to locally modify the refractive index of dielectric materials in three-dimensions (3D). Recently, ULI has been applied to the fabrication of astrophotonic devices such as integrated beam combiners, 3D integrated waveguide fan-outs and multimode-to-single mode convertors (photonic lanterns). Here, we outline our work on applying ULI to the fabrication of volume phase gratings (VPGs) in fused silica and gallium lanthanum sulphide (GLS) glasses. The VPGs we fabricated had a spatial freque…
Integrated, ultrafast all-optical polariton transistors with sub-wavelength grating microcavities
IBM Research Europe – Zurich（IBM欧洲苏黎世研究中心）；ETH Zürich（苏黎世联邦理工学院）；AMO GmbH（AMO有限公司）；RWTH Aachen University（亚琛工业大学）；Bergische Universität Wuppertal（伍珀塔尔大学）
The release of conduction-band electrons from a metal surface by a sub-femtosecond extreme ultraviolet (XUV) pulse, and their propagation through the solid, provokes a dielectric response in the solid that acts back on the photoelectron wave packet. We calculated the (wake) potential associated with this photoelectron self-interaction in terms of bulk and surface plasmon excitations and show that it induces a considerable, XUV-frequency-dependent temporal shift in laser-streaked XUV photoemission spectra, suggesting the observation of the ultrafast solid-state dielectric response in contempora…
The phase, amplitude, speed, and polarization, in addition to many other properties of light, can be modulated by photonic Bragg structures. In conjunction with nonlinearity and quantum effects, a variety of ensuing micro- or nano-photonic applications can be realized. This paper reviews various optical phenomena in several exemplary 1D Bragg gratings. Important examples are resonantly absorbing photonic structures, chirped Bragg grating, and cholesteric liquid crystals; their unique operation capabilities and key issues are considered in detail. These Bragg structures are expected to be used …
Nonlinear spectroscopy in the extreme ultraviolet (EUV) and soft x-ray spectral range offers the opportunity for element selective probing of ultrafast dynamics using core-valence transitions (Mukamel et al., Acc. Chem. Res. 42, 553 (2009)). We demonstrate a step on this path showing core-valence sensitivity in transient grating spectroscopy with EUV probing. We study the optically induced insulator-to-metal transition (IMT) of a VO2 film with EUV diffraction from the optically excited sample. The VO2 exhibits a change in the 3p-3d resonance of V accompanied by an acoustic response. Due to the…
Square-wave pulse generation with a variable duty ratio can be realized with the help of ideas of Talbot array illuminators formulated for binary phase gratings. A binary temporal phase modulation of CW laser field propagating through a group-delay-dispersion circuit of the fractional Talbot length $P/Q$ results in a well defined sequence of square-wave-form pulses. When $P=1$ a duty ratio of the pulses $D$ is $1/2$ for $Q=4$ and $1/3$ for $Q=3$ and 6. Maximum intensity of the pulses doubles and triples compared to the CW intensity for $D=1/2$ and $1/3$, respectively. These pulses can be used …
We demonstrate an ultrafast reversible modulation of resonant terahertz (THz) response in strongly photoexcited metamaterials. The transient spectral-temporal response of the dipole transition ~1.6 THz exhibits a distinct non-monotonic variation as a function of pump fluence. The transition energy shift, strength, spectral width and density-dependent ultrafast relaxation manifest a remarkable re-emergence of the resonances after initial quenching. Our simulation, incorporating the first-order diffraction from the photoinduced transient grating, reproduces the salient features, providing a new …
A High Intensity Attosecond Light Source in Compact Geometry at ELI ALPS User Facility
ELI ALPS, The Extreme Light Infrastructure ERIC（ELI ALPS，极端光基础设施欧洲研究基础设施有限公司）；Institute of Physics, University of Szeged（塞格德大学物理研究所）；Foundation for Research and Technology - Hellas, Institute of Electronic Structure & Laser（希腊研究与技术基金会电子结构与激光研究所）
The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within a XUV p…
Few-picosecond pulse generation featuring ultrafast spectral dynamics in gain-switched surface-grating DFB lasers via impulsive optical pumping
Institute for Solid State Physics, The University of Tokyo（东京大学固体物理研究所）；State Key Laboratory of Precision Spectroscopy, Department of Electronic Engineering, East China Normal University（华东师范大学精密光谱科学国家重点实验室电子工程系）；LDseed Co., Ltd.（LDseed有限公司）
Strong retardation of ultrashort optical pulses, including their deceleration and stoppage in the form of Bragg solitons in a cascaded Bragg-grating (BG) structure, is proposed. The manipulations of the pulses are carried out, using nonlinear effects, in a chirped BG segment which is linked, via a defect, to a uniform grating. The storage of the ultrashort pulses is shown to be very robust with respect to variations of the input field intensity, suggesting the feasibility of storing ultrafast optical pulses in such a structure. Physical estimates are produced for the BGs written in silicon.
Single-shot ultrafast spectroscopy based on the frequency encoding of transient absorbance kinetics (FDSS) is demonstrated. These kinetics are sampled spectrally using linearly chirped pulses derived from a Ti:sapphire laser. A variable length grating pair compressor is used to provide group velocity dispersion out to -1.6 ps^2 and achieve the sampling of 512 channels per a 2-to-160 ps window with sensitivity > 5e-4. The possibilities of FDSS are illustrated with studies of three photon ionization of liquid water and one-photon excitation of a thin-film
Infrared and visible light beams carrying orbital angular momentum (OAM) are currently thoroughly studied for their extremely broad applicative prospects, among which are quantum information, micromachining and diagnostic tools. Here we extend these prospects, presenting a comprehensive study for the synthesis and full characterization of optical vortices carrying OAM in the extreme ultraviolet (XUV) domain. We confirm the upconversion rules of a femtosecond infrared helically phased beam into its high-order harmonics, showing that each harmonic order carries the total number of OAM units abso…
In the Kapitza-Dirac effect, atoms, molecules, or swift electrons are diffracted off a standing wave grating of the light intensity created by two counter-propagating laser fields. In ultrafast electron optics, such a coherent beam splitter offers interesting perspectives for ultrafast beam shaping. Here, we study, both analytically and numerically, the effect of the inclination angle between two laser fields on the diffraction of pulsed, low-energy electron beams. For sufficiently high light intensities, we observe a rich variety of complex diffraction patterns. These do not only reflect inte…
Noncollinear wave-mixing spectroscopies with attosecond extreme ultraviolet (XUV) pulses provide unprecedented insight into electronic dynamics. In infrared and visible regimes, heterodyne detection techniques utilize a reference field to amplify wave-mixing signals while simultaneously allowing for phase-sensitive measurements. Here, we implement a self-heterodyned detection scheme in noncollinear wave-mixing measurements with a short attosecond XUV pulse train and two few-cycle near infrared (NIR) pulses. The initial spatiotemporally overlapped XUV and NIR pulses generate a coherence of both…
The self-referenced spectral interferometry (SRSI) technique, which is usually used for microjoule-level femtosecond pulses characterization, is improved to characterize weak femtosecond pulses with nanojoule based on the transient-grating effect. Both femtosecond pulses from an amplifier with 3 nJ per pulse at 1 kHz repetition rates and femtosecond pulses from an oscillator with less than 0.5 nJ per pulse at 84 MHz repetition rates are successfully characterized. Furthermore, through a special design, the optical setup of the device is even smaller than a palm which will makes it simple and c…
The use of few-femtosecond, extreme ultraviolet (XUV) pulses, produced by high-order harmonic generation, in combination with few-femtosecond infrared (IR) pulses in pump-probe experiments has great potential to disclose ultrafast dynamics in molecules, nanostructures and solids. A crucial prerequisite is a reliable characterization of the temporal properties of the XUV and IR pulses. Several techniques have been developed. The majority of them applies phase reconstruction algorithms to a photoelectron spectrogram obtained by ionizing an atomic target in a pump-probe fashion. If the ionizing r…
Laser-induced transient opacity in helium nanodroplets probed by single-shot coherent diffraction
ETH Zurich（苏黎世联邦理工学院）；University of Rostock（罗斯托克大学）；Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy（马克斯·玻恩非线性光学和超快光谱研究所）；Technical University of Berlin（柏林工业大学）
Ultrafast imaging is essential in physics and chemistry to investigate the femtosecond dynamics of nonuniform samples or of phenomena with strong spatial variations. It relies on observing the phenomena induced by an ultrashort laser pump pulse using an ultrashort probe pulse at a later time. Recent years have seen the emergence of very successful ultrafast imaging techniques of single non-reproducible events with extremely high frame rate, based on wavelength or spatial frequency encoding. However, further progress in ultrafast imaging towards high spatial resolution is hampered by the lack o…
Optical-domain Transient Grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique used to probe vibrational, magnetic and electronic degrees of freedom in the time domain. The newly developed coherent X-ray Free Electron Laser sources allow its extension to the X-ray regime. Xrays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element-specificity can address core-excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. We …
High-resolution Fourier-transform spectroscopy using table-top sources in the extreme ultraviolet (XUV) spectral range is still in its infancy. In this contribution a significant advance is presented based on a Michelson-type all-reflective split-and-delay autocorrelator operating in a quasi amplitude splitting mode. The autocorrelator works under a grazing incidence angle in a broad spectral range $\mathrm{(10\,nm - 1\,μm)}$ providing collinear propagation of both pulse replicas and thus a constant phase difference across the beam profile. The compact instrument allows for XUV pulse autocorre…
Ultrafast control of magnetization on the nanometer length scale, in particular all-optical switching, is key to putting ultrafast magnetism on the path towards future technological application in data storage technology. However, magnetization manipulation with light on this length scale is challenging due to the wavelength limitations of optical radiation. Here, we excite transient magnetic gratings in a GdFe alloy with a periodicity of 87 nm by interference of two coherent femtosecond light pulses in the extreme ultraviolet spectral range at the free electron laser facility FERMI. The subse…
