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 demonstrated via HHG of a frequency-doubled and post-compressed fibre laser. At the same time sub-6 fs XUV pulse duration allows accessing ultrafast dynamics with an order of magnitude higher photon flux than previously demonstrated. This concept will greatly advance and facilitate applications of XUV radiation in science and technology and enable photon-hungry ultrafast studies.
High harmonic generation (HHG) enables extreme ultraviolet radiation with table-top setups. Its exceptional properties, such as coherence and (sub)-femtosecond pulse durations, have led to a diversity of applications. Some of these require a high photon flux and megahertz repetition rates, e.g. to avoid space charge effects in photoelectron spectroscopy. To date this has only been achieved with enhancement cavities. Here, we establish a novel route towards powerful HHG sources. By achieving phase-matched HHG of a megahertz fibre laser we generate a broad plateau (25 eV - 40 eV) of strong harmo…
Pulse-to-pulse spectral phase characterization of mid-infrared pulses at megahertz rates
The University of Tokyo（东京大学）；Polytechnique Montréal（蒙特利尔理工大学）；University of New Mexico（新墨西哥大学）；RIKEN Center for Advanced Photonics, RIKEN（理化学研究所先进光子中心）
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…
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…
We propose sub-harmonic resonant optical excitation with femtosecond lasers as a new method for the characterization of phononic and nanomechanical systems in the gigahertz to terahertz frequency range. This method is applied for the investigation of confined acoustic modes in a free-standing semiconductor membrane. By tuning the repetition rate of a femtosecond laser through a sub-harmonic of a mechanical resonance we amplify the mechanical amplitude, directly measure the linewidth with megahertz resolution, infer the lifetime of the coherently excited vibrational states, accurately determine…
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…
We report generation of a femtosecond supercontinuum extending from the ultraviolet to the near-infrared and detection of its carrier-envelope phase variation by f-to-2f interferometry. The spectrum is generated in a gas-filled hollow-core photonic crystal fiber where soliton dynamics allows CEP-stable self-compression of OPCPA pump pulses at 800 nm to a duration of 1.7 optical cycles, followed by dispersive wave emission. The source provides up to 1 μJ of pulse energy at 800 kHz repetition rate resulting in 0.8 W of average power, and can be extremely useful for example in strong-field physic…
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…
Time- and angle-resolved photoelectron spectroscopy (trARPES) employing a 500 kHz extreme-ultravioled (XUV) light source operating at 21.7 eV probe photon energy is reported. Based on a high-power ytterbium laser, optical parametric chirped pulse amplification (OPCPA), and ultraviolet-driven high-harmonic generation, the light source produces an isolated high-harmonic with 110 meV bandwidth and a flux of more than $10^{11}$ photons/second on the sample. Combined with a state-of-the-art ARPES chamber, this table-top experiment allows high-repetition rate pump-probe experiments of electron dynam…
A compact high repetition rate attosecond light source based on a standard laser oscillator combined with plasmonic enhancement is presented. At repetition rates of tens of MHz, we predict focusable pulses with durations of ~< 300 attoseconds, and collimation angles ~< 5 degrees. Attosecond pulse parameters are robust with respect variations of driver pulse focus and duration.
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.
After decades of supremacy of the Titanium:Sapphire technology, Ytterbium-based high-order harmonic sources are emerging as an interesting alternative for experiments requiring high flux of ultrashort extreme ultraviolet (XUV) radiation. In this article we describe a versatile experimental setup delivering XUV photons in the 10-50 eV range. The use of cascaded high-harmonic generation enables us to reach 1.8 mW of average power at 18 eV. Several spectral focusing schemes are presented, to select either a single harmonic or group of high-harmonics and thus an attosecond pulse train. In the pers…
Many atomic and molecular systems of fundamental interest possess resonance frequencies in the extreme ultraviolet (XUV) where laser technology is limited and radiation sources have traditionally lacked long-term phase coherence. Recent breakthroughs in XUV frequency comb technology have demonstrated spectroscopy with unprecedented resolution at the megahertz level, but even higher resolutions are desired for future applications in precision measurement. By characterizing heterodyne beats between two XUV comb sources, we demonstrate the capability for sub-hertz spectral resolution. This corres…
Although ultraviolet (UV) light is important in many areas of science and technology, there are very few if any lasers capable of delivering wavelength-tunable ultrashort UV pulses at MHz repetition rates. Here we report the generation of deep-UV laser pulses at MHz repetition rates and μJ-energies by means of dispersive wave (DW) emission from self-compressed solitons in gas-filled single-ring hollow-core photonic crystal fiber (SR-PCF). Pulses from an ytterbium fiber laser (~300 fs) are first compressed to ~25 fs in a SR-PCF-based nonlinear compression stage, and subsequently used to pump a …
Laser-driven high-order harmonic generation (HHG) provides tabletop sources of broadband extreme-ultraviolet (XUV) light with excellent spatial and temporal coherence. These sources are typically operated at low repetition rates, $f_{rep}\lesssim$100 kHz, where phase-matched frequency conversion into the XUV is readily achieved. However, there are many applications that demand the improved counting statistics or frequency-comb precision afforded by operation at high repetition rates, $f_{rep}$ > 10 MHz. Unfortunately, at such high $f_{rep}$, phase matching is prevented by the accumulated stead…
We present nonlinear pulse compression of a high-power SESAM-modelocked thin-disk laser (TDL) using an Ar-filled hypocycloid-core Kagome Hollow-Core Photonic Crystal Fiber (HC-PCF). The output of the modelocked Yb:YAG TDL with 127 W average power, a pulse repetition rate of 7 MHz, and a pulse duration of 740 fs was spectrally broadened 16-fold while propagating in a Kagome HC-PCF containing 13 bar of static Argon gas. Subsequent compression tests performed using 8.4% of the full available power resulted in a pulse duration as short as 88 fs using the spectrally broadened output from the fiber.…
Extreme ultraviolet frequency combs are a versatile tool with applications including precision measurement, strong-field physics, and solid-state physics. Here we report on an application of extreme ultraviolet frequency combs and their driving lasers for studying strong-field effects in molecular systems. We perform field-free molecular alignment and high-order harmonic generation with aligned molecules in a gas jet at a repetition rate of 154 MHz using a high-powered optical frequency comb inside a femtosecond enhancement cavity. The cavity-enhanced system provides a means to reach suitable …
Extreme ultraviolet (XUV) lasers are essential for the investigation of fundamental physics. Especially high repetition rate, high photon flux sources are of major interest for reducing acquisition times and improving signal to noise ratios in a plethora of applications. Here, an XUV source based on cascaded frequency conversion is presented, which delivers due to the drastic better single atom response for short wavelength drivers, an average output power of (832 +- 204) μW at 21.7 eV. This is the highest average power produced by any HHG source in this spectral range surpassing precious demo…
A novel scheme for stabilizing the carrier-envelope phase (CEP) of low-repetition rate lasers was demonstrated using a 350 mJ, 14 fs Ti:Sapphire laser operating at 10 Hz. The influence of the CEP on the generation of a continuum in the extreme ultraviolet (XUV) was observed.
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 temper…
Tunable coherent light sources operating in the vacuum ultraviolet (VUV) region in 100-200-nm (6-12 eV) wavelength range have important spectroscopic applications in many research fields, including time-resolved angle-resolved photoemission spectroscopy (ARPES). Recent advances in laser technology have enabled the upconversion of visible femtosecond lasers to the vacuum and extreme ultraviolet regions. However, the complexity of their experimental setups and the scarcity of bulk nonlinear crystals for VUV generation have hampered its widespread use. Here, we propose the use of a free-standing …
A compact Kerr-lens mode-locked thin-disk oscillator delivering 110 MW output peak power, the highest among all oscillators, is reported. A pulse train with a repetition rate of 14 MHz carries 115 fs long, 14.4 uJ pulses resulting in 202 W of average power. This compact, simple, and stable oscillator is a suitable driver and an important milestone for further high harmonics generation and the development of extreme ultraviolet transportable frequency comb sources.
Recent progress in laser-based high-repetition rate extreme ultraviolet (EUV) lightsources and multidimensional photoelectron spectroscopy enable the build-up of a new generation of time-resolved photoemission experiments. Here, we present a setup for time-resolved momentum microscopy driven by a 1 MHz femtosecond EUV table-top light source optimized for the generation of 26.5 eV photons. The setup provides simultaneous access to the temporal evolution of the photoelectron's kinetic energy and in-plane momentum. We discuss opportunities and limitations of our new experiment based on a series o…
The generation of coherent light pulses in the extreme ultraviolet (XUV) spectral region with attosecond pulse durations constitutes the foundation of the field of attosecond science. Twenty years after the first demonstration of isolated attosecond pulses, they continue to be a unique tool enabling the observation and control of electron dynamics in atoms, molecules and solids. It has long been identified that an increase in the repetition rate of attosecond light sources is necessary for many applications in atomic and molecular physics, surface science, and imaging. Although high harmonic g…
A recently developed source of ultraviolet radiation, based on optical soliton propagation in a gas-filled hollow-core photonic crystal fiber, is applied here to angle-resolved photoemission spectroscopy (ARPES). Near-infrared femtosecond pulses of only few μJ energy generate vacuum ultraviolet (VUV) radiation between 5.5 and 9 eV inside the gas-filled fiber. These pulses are used to measure the band structure of the topological insulator Bi2Se3 with a signal to noise ratio comparable to that obtained with high order harmonics from a gas jet. The two-order-of-magnitude gain in efficiency promi…
Characterizing and controlling electronic properties of quantum materials require direct measurements of non-equilibrium electronic band structures over large regions of momentum space. Here, we demonstrate an experimental apparatus for time- and angle-resolved photoemission spectroscopy using high-order harmonic probe pulses generated by a robust, moderately high power (20 W) Yb:KGW amplifier with tunable repetition rate between 50 and 150 kHz. By driving high-order harmonic generation (HHG) with the second harmonic of the fundamental 1025 nm laser pulses, we show that single-harmonic probe p…
High-harmonic generation (HHG) provides short-wavelength light that is useful for precision spectroscopy and probing ultrafast dynamics. We report efficient, phase-coherent harmonic generation up to 9th-order (333 nm) in chirped periodically poled lithium niobate waveguides driven by phase-stable $\leq$12-nJ, 100 fs pulses at 3 $μ$m with 100 MHz repetition rate. A mid-infrared to ultraviolet-visible conversion efficiency as high as 10% is observed, amongst an overall 23% conversion of the fundamental to all harmonics. We verify the coherence of the harmonic frequency combs despite the complex …
We present efficient high-order harmonic generation (HHG) based on a high-repetition rate, few-cycle, near infrared (NIR), carrier-envelope phase stable, optical parametric chirped pulse amplifier (OPCPA), emitting 6fs pulses with 9μJ pulse energy at 200kHz repetition rate. In krypton, we reach conversion efficiencies from the NIR to the extreme ultraviolet (XUV) radiation pulse energy on the order of ~10^{-6} with less than 3μJ driving pulse energy. This is achieved by optimizing the OPCPA for a spatially and temporally clean pulse and by a specially designed high-pressure gas target. In the …
We demonstrate a femtosecond enhancement cavity with a crossed-beam geometry for efficient generation and extraction of extreme-ultraviolet (XUV) frequency combs at a 154 MHz repetition rate. We achieve a record-high out-coupled power of 600 μW, directly usable for spectroscopy, at a wavelength of 97 nm. This corresponds to a >60% out-coupling efficiency. The XUV power scaling and generation efficiency are similar to that achieved with a single Gaussian-mode fundamental beam inside a collinear enhancement cavity. The noncollinear geometry also opens the door for the generation of isolated atto…
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…
We demonstrate that high-harmonic generation (HHG) in solids dominantly originates from strongly localized surface states through non-perturbative processes. Measurements reveal that HHG from bulk states is suppressed by at least 1-2 orders of magnitude due to the lack of phase matching, when generated perturbatively, or by at least 3-4 orders of magnitude, when generated non-perturbatively. We derive a theory that fully supports this observation and quantitatively describes the generation of harmonics from the surface states as well as from interfaces between solids; it also predicts a much w…
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 $ …
Optical waveguides made from periodically poled materials provide high confinement of light and enable the generation of new wavelengths via quasi-phase-matching, making them a key platform for nonlinear optics and photonics. However, such devices are not typically employed for high-harmonic generation. Here, using 200-fs, 10-nJ-level pulses of 4100 nm light at 1 MHz, we generate high harmonics up to the 13th harmonic (315 nm) in a chirped, periodically poled lithium niobate (PPLN) waveguide. Total conversion efficiencies into the visible--ultraviolet region are as high as 10 percent. We find …
Here we present a high repetition rate, narrow band-width, extreme ultraviolet (XUV) photon source for time- and angle-resolved photoemission spectroscopy (tr-ARPES). The narrow band width pulses $ΔE=9, 14, 18$ meV for photon energies $hν=10.8, 18.1, 25.3$ eV are generated through High Harmonic Generation (HHG) using ultra-violet (UV) drive pulses with relatively long pulse lengths (461 fs). The HHG setup employs an annuluar drive beam in a tight focusing geometry at a repetition rate of 250 kHz. Photon energy selection is provided by a series of selectable multilayer bandpass mirrors and thin…
Development of the optical frequency comb has revolutionised metrology and precision spectroscopy due to its ability to provide a precise and direct link between microwave and optical frequencies. A novel application of frequency comb technology that leverages both the ultrashort duration of each laser pulse and the exquisite phase coherence of a train of pulses is the generation of frequency combs in the extreme ultraviolet (XUV) via high harmonic generation (HHG) in a femtosecond enhancement cavity. Until now, this method has lacked sufficient average power for applications, which has also h…
We review the current state of tabletop extreme ultraviolet (XUV) sources based on high harmonic generation (HHG) in femtosecond enhancement cavities (fsEC). Recent developments have enabled generation of high photon flux (1014 photons/sec) in the XUV, at high repetition rates (>50 MHz) and spanning the spectral region from 40 nm - 120 nm. This level of performance has enabled precision spectroscopy with XUV frequency combs and promises further applications in XUV spectroscopic and photoemission studies. We discuss the theory of operation and experimental details of the fsEC and XUV generation…
We report on the development of a high-power mid-infrared frequency comb with 100 MHz repetition rate and 100 fs pulse duration. Difference frequency generation is realized between two branches derived from an Er:fiber comb, amplified separately in Yb:fiber and Er:fiber amplifiers. Average powers of 6.7 W and 14.9 W are generated in the 2.9 $μ$m idler and 1.6 $μ$m signal, respectively. With high average power, excellent beam quality, and passive carrier-envelope phase stabilization, this light source is a promising platform for generating broadband frequency combs in the far infrared, visible,…
