Ultrafast element-resolved magneto-optics using a fiber-laser-driven extreme ultraviolet light source
Christina Möller, Henrike Probst, Johannes Otto, Karen Stroh, Carsten Mahn, Sabine Steil, Vasily Moshnyaga, G. S. Matthijs Jansen, Daniel Steil, Stefan Mathias
发表信息：
Review of Scientific Instruments 92, 065107 (2021)
We present a novel setup to measure the transverse magneto-optical Kerr effect in the extreme ultraviolet spectral range at exceptionally high repetition rates based on a fiber laser amplifier system. This affords a very high and stable flux of extreme ultraviolet light, which we use to measure element-resolved demagnetization dynamics with unprecedented depth of information. Furthermore, the setup is equipped with a strong electromagnet and a cryostat, allowing measurements between 10 and 420 K using magnetic fields up to 0.86 T. The performance of our setup is demonstrated by a set of temperature- and time-dependent magnetization measurements showing distinct element-dependent behavior.
Deep ultraviolet (DUV) laser pulses with tuneable wavelength and very short duration are a key enabling technology for next-generation technology and ultrafast science. Their generation has been the subject of extensive experimental effort, but no technique demonstrated thus far has been able to meet all requirements in one light source. Here we demonstrate a bright, efficient, and compact source of tuneable deep ultraviolet ultrafast laser pulses based on resonant dispersive wave emission in hollow capillary fibre. In a total footprint of only 120 x 75 cm, including the ytterbium-based drive …
We report on the development of a high-order harmonic generation (HHG)-based ultrafast high-repetition-rate (250 kHz) monochromatic extreme ultraviolet (21.6 eV) source with polarization tunability, specifically designed for multi-modal dichroism in time- and angle-resolved photoemission spectroscopy. Driving HHG using an annular beam allows us to spatially separate the high-power 515 nm driving laser from the XUV beamlet while preserving the linear polarization axis angle tunability. This enables controlling the polarization state of the XUV radiation with a fixed all-reflective phase-shifter…
We experimentally demonstrate the efficient generation of circularly polarized pulses tunable from the vacuum to deep ultraviolet (160-380 nm) through resonant dispersive wave emission from optical solitons in a gas-filled hollow capillary fiber. In the deep ultraviolet we measure up to 13 microjoule of pulse energy, and from numerical simulations, we estimate the shortest output pulse duration to be 8.5 fs. We also experimentally verify that simply scaling the pulse energy by 3/2 between linearly and circularly polarized pumping closely reproduces the soliton and dispersive wave dynamics. Bas…
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…
Ultrafast nonlinear photonics enables a host of applications in advanced on-chip spectroscopy and information processing. These rely on a strong intensity dependent (nonlinear) refractive index capable of modulating optical pulses on sub-picosecond timescales and on length scales suitable for integrated photonics. Currently there is no platform that can provide this for the UV spectral range where broadband spectra generated by nonlinear modulation can pave the way to new on-chip ultrafast (bio-) chemical spectroscopy devices. We demonstrate the giant nonlinearity of UV hybrid light-matter sta…
We demonstrate, for the first time, the application of rare-gas filled hollow-core photonic crystal fibres (HC-PCFs) as tuneable ultraviolet light sources in femtosecond pump-probe spectroscopy. The time-resolved photoelectron imaging technique reveals non-adiabatic dynamical processes operating on three distinct timescales in the styrene molecule following excitation over the 242-258 nm region. These include ultrafast (<100 fs) internal conversion between the S2(pipi*) and S1(pipi*) electronic states and subsequent intramolecular vibrational energy redistribution within S1(pipi*). Compact, co…
A comprehensive experimental analysis of spatio-temporal coupling effects inherent to the acousto-optic programmable dispersive filter (AOPDF) is presented. Phase and amplitude measurements of the AOPDF transfer function are performed using spatially and spectrally resolved interferometry. Spatio-temporal and spatio-spectral coupling effects are presented for a range of shaped pulses that are commonly used in quantum control experiments. These effects are shown to be attributable to a single mechanism: a group-delay--dependent displacement of the shaped pulse. The physical mechanism is explain…
Trapped ions are one of the most promising approaches for the realization of a universal quantum computer. Faster quantum logic gates could dramatically improve the performance of trapped-ion quantum computers, and require the development of suitable high repetition rate pulsed lasers. Here we report on a robust frequency upconverted fiber laser based source, able to deliver 2.5 ps ultraviolet (UV) pulses at a stabilized repetition rate of 300.00000 MHz with an average power of 190 mW. The laser wavelength is resonant with the strong transition in Ytterbium (Yb+) at 369.53 nm and its repetitio…
Vacuum ultraviolet (VUV) light is critical for the study of molecules and materials, but the generation of femtosecond pulses in the VUV region at high repetition rates has proven difficult. Here, we demonstrate the efficient generation of VUV light at MHz repetition rates using highly cascaded four-wave mixing processes in a negative-curvature hollow-core fiber. Both even and odd order harmonics are generated up to the 15th harmonic (69 nm, 18.0 eV), with high energy resolution of ~40 meV. In contrast to direct high harmonic generation, this highly cascaded harmonic generation process require…
Here we report on a novel High Harmonic Generation (HHG) light source designed for space charge free ultrafast photoelectron spectroscopy (PES) on solids. The ultimate overall energy resolution achieved on a polycrystalline Au sample is ~22 meV at 40 K. These results have been obtained at a photon energy of 16.9 eV with a pulse bandwidth of ~19 meV, by varying, up to 200 kHz, the photon pulses repetition rate and the photon fluence on the sample. These features set a new benchmark for tunable narrowband HHG sources. By comparing the PES energy resolution and the photon pulse bandwidth with a p…
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 induce ultrafast magneto-photocurrents in a GaAs crystal employing interband excitation with femtosecond laser pulses at room temperature and non-invasively separate surface and bulk contributions to the overall current response. The separation between the different symmetry contributions is achieved by measuring the simultaneously emitted terahertz radiation for different sample orientations. Excitation intensity and photon energy dependences of the magneto-photocurrents for linearly and circularly polarized excitations reveal an involvement of different microscopic origins, one of which w…
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…
Ultraviolet frequency combs enable applications ranging from precision spectroscopy to atomic clocks by addressing the electronic transitions of atoms and molecules. Access to ultraviolet light via integrated nonlinear optics is usually hampered by the strong material dispersion and large waveguide attention in the ultraviolet region. Here we demonstrate a simple route to chip-scale ultraviolet comb generators, simultaneously showing a gap-free frequency span of ~128 terahertz and supercontinuum sourced by an ultrafast fiber laser. The simultaneous cubic and quadratic nonlinear processes are i…
We report about the existence of magneto-acoustic pulses propagating in a 200-nm-thick ferromagnetic nickel film excited with 120 fs laser pulses. They result from the coupling between the magnetization of the ferromagnetic film and the longitudinal acoustic waves associated to the propagation of the lattice deformation induced by the femtosecond laser pulses. The magneto-acoustic pulses are detected from both the front and back sides of the film, using the time-resolved magneto-optical Kerr technique, measuring both the time dependent rotation and ellipticity. We show that the propagating aco…
We induce ultrafast photocurrents in a GaAs crystal exposed to a magnetic field by optical femtosecond excitation. The magneto-photocurrents are studied by time-resolved detection of the simultaneously emitted THz radiation. We find that their dynamics differ considerably from the dynamics of other photocurrents which are expected to follow the temporal shape of the optical intensity. We attribute this difference to the influence of carrier-anisotropy relaxation on the magneto-photocurrents. Our measurements show that the anisotropy relaxation for carrier densities ranging between $10^{16}$ cm…
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…
We consider light scattering by a coated magneto-plasmonic nanoparticle (MPNP) with a Kerr-type nonlinear plasmonic shell and a magneto-optic core. Such structure features two plasmon dipole modes, associated with electronic oscillations on the inner and outer surfaces of the shell. Driven in a nonlinear regime, each mode exhibits a bistable response. Bistability of an inner plasmon leads to switching between this state and a Fano resonance (Fano switching). Once the external light intensity exceeds the critical value, the bistability zones of both eigen modes overlap yielding optical tristabi…
Ultrafast broadband ultraviolet radiation is of importance in spectroscopy and photochemistry, since high photon energies enable single-photon excitations and ultrashort pulses allow time-resolved studies. Here we report the use of gas-filled hollow-core photonic crystal fibers (HC-PCFs) for efficient ultrafast nonlinear optics in the ultraviolet. Soliton self-compression of 400 nm pulses of (unprecedentedly low) ~500 nJ energies down to sub-6-fs durations is achieved, as well as resonant emission of tunable dispersive waves from these solitons. In addition, we discuss the generation of a flat…
Antisymmetric chirp transfer to high-energy ultraviolet pulses via gas-based chirped four-wave mixing
University of California Los Angeles（加州大学洛杉矶分校）；California NanoSystems Institute（加州纳米系统研究所）；SLAC National Accelerator Laboratory, Stanford University（斯坦福大学SLAC国家加速器实验室）
Light-matter interactions in layered materials and heterostructures: from moiré physics and magneto-optical effects to ultrafast dynamics and hybrid meta-photonics
High harmonic generation is a convenient way to obtain extreme ultraviolet light from table-top laser systems and the experimental tools to exploit this simple and powerful light source for time-resolved spectroscopy are being developed by several groups. For these applications, brightness and stability of the high harmonic generation is a key feature. This article focuses on practical aspects in the generation of extreme ultraviolet pulses with ultrafast commercial lasers, namely generation parameters and online monitoring as well as analysis of generation yield and stability.
Noble metal nanoparticles exhibit localized plasmon resonance modes that span the visible and near-infrared spectral ranges and have many applications. Modifying the size, shape, and composition of the nanoparticles changes the number of modes and their properties. The characteristics of these modes are transiently affected when illuminating the nano-objects with ultrashort laser pulses. Here, we synthesize core-shell gold-silver nanocuboids and measure their spectral signature in the stationary and ultrafast transient regimes. Their dipolar transverse mode vanishes with increasing Ag-shell th…
We report on the experimental evidence of magnetic helicoidal dichroism, observed in the interaction of an extreme ultraviolet vortex beam carrying orbital angular momentum with a magnetic vortex. Numerical simulations based on classical electromagnetic theory show that this dichroism is based on the interference of light modes with different orbital angular momenta, which are populated after the interaction between the light phase chirality and the magnetic topology. This observation gives insight into the interplay between orbital angular momentum and magnetism, and sets the framework for th…
In this study the generation of energetic coherent extreme ultraviolet (XUV) radiation with controlled polarization, is reported. The XUV radiation results from the process of high harmonic generation (HHG), in a gas phase atomic medium, driven by an intense two-color circularly polarized counter-rotating laser field, under loose focusing geometry conditions. The energy of the XUV radiation emitted per laser pulse is found to be of the order of ~100 nJ with the spectrum spanning from 17 to 26 eV. The demonstrated energy values along with tight focusing geometries is sufficient to induce nonlin…
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…
Surface plasmon polaritons (SPP or SP) are electromagnetic waves propagating along metal dielectric interfaces and existing over a wide range of frequencies. They have become popular because of their sub-wavelength confinement and the possibility to perform ultrasensitive optical measurements. Driven by tremendous progress in nanofabrication techniques and ultrafast laser technologies the applications of SP nanooptics extend beyond the border of nanoplasmonics. Here we review how using novel hybrid multilayer structures combining different functionalities allows to develop active plasmonic dev…
High-energy ultraviolet pulse generation in gas-filled hollow capillary fibers (HCFs) through dispersive-wave-emission process, has attracted considerable attentions in recent several years due to its great application potentials in ultraviolet spectroscopy and photochemistry. While the ability of this technique to deliver high-energy, ultrafast ultraviolet pulses is widely recognized, few-fs duration of μJ-level dispersive-wave (DW) pulses has, however, escaped direct measurements. In this letter, we demonstrate that using several chirped mirrors, few-fs ultraviolet DW pulses can be obtained …
The industrial maturity of ultrashort pulsed lasers has triggered the development of a plethora of material processing strategies. Recently, the combination of these remarkable temporal pulse properties with advanced structured light concepts has led to breakthroughs in the development of novel laser application methods, which will now gradually reach industrial environments. We review the efficient generation of customized focus distributions from the near infrared down to the deep ultraviolet, e.g., based on non-diffracting beams and 3D-beam splitters, and demonstrate their impact for micro-…
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…
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…
Novel table-top sources of extreme-ultraviolet light based on high-harmonic generation yield unique insight into the fundamental properties of molecules, nanomaterials, or correlated solids, and enable advanced applications in imaging or metrology. Extending high-harmonic generation to high repetition rates portends great experimental benefits, yet efficient extreme-ultraviolet conversion of correspondingly weak driving pulses is challenging. Here, we demonstrate a highly efficient source of femtosecond extreme-ultraviolet pulses at 50-kHz repetition rate, utilizing the ultraviolet second-harm…
In magnetoplasmonics, it is possible to tailor the magneto-optical properties of nanostructures by exciting surface plasmon polaritons (SPPs). Thus far, magnetoplasmonic effects have been considered static. Here, we describe ultrafast manifestations of magnetoplasmonics by observing the non-trivial evolution of the transverse magneto-optic Kerr effect within 45-fs pulses reflected from an iron-based magnetoplasmonic crystal. The effect occurs for resonant SPP excitations, displays opposite time derivative signs for different slopes of the resonance, and is explained with the magnetization-depe…
Optical soliton dynamics can cause the extreme alteration of the temporal and spectral shape of a propagating light pulse. They occur at up to kilowatt peak powers in glass-core optical fibres and the gigawatt level in gas-filled microstructured hollow-core fibres. Here we demonstrate optical soliton dynamics in large-core hollow capillary fibres. This enables scaling of soliton effects by several orders of magnitude to the multi-mJ energy and terawatt peak power level. We experimentally demonstrate two key soliton effects. First, we observe self-compression to sub-cycle pulses and infer the c…
We present the results of an experimental and numerical investigation into temporally non-local coherent interactions between ultrashort pulses, mediated by Raman coherence, in gas-filled kagomé-style hollow-core photonic crystal fiber. A pump pulse first set up the Raman coherence, creating a refractive index grating in the gas that travels at the group velocity of the pump pulse. Varying the arrival time of a second probe pulse allows high degree of control over its evolution as it propagates along the fiber, in particular soliton self-compression and dispersive wave (DW) emission. In the ex…
The ultrafast switching of magnetization in multiferroic materials by a femtosecond laser could provide various advantages in photonics and magnonics. An efficient approach to control the light matter interaction is the modulation of ultrafast coherent magnons and phonons in the high frequency range. Spontaneous Raman and infrared spectra reveal the excitation of magnons and optical phonons in multiferroic BiFeO3 in the sub few terahertz range. However, coherent control of such quasiparticles has not been achieved yet. In this study, we demonstrate that linearly polarized laser pulses simultan…
We investigate the interaction of femtosecond laser pulses with spins including relativistic corrections. The time-ordered magneto-optical signals corresponding to a pump-probe configuration are calculated in the case of one electron submitted to a magnetic field and evolving in eight levels of the fine structure of a hydrogen-like atom. Our simulations explain the origin of the coherent magneto-optical response and ultrafast spin dynamics in ferromagnets excited by intense laser pulses as recently reported in Ni and CoPt3 ferromagnetic thin films. Our detailed analysis allows identifying the …
