Generation and characterization of few-pulse attosecond pulse trains at 100kHz repetition rate
Mikhail Osolodkov, Federico J. Furch, Felix Schell, Peter Susnjar, Fabio Cavalcante, Carmen S. Menoni, Claus P. Schulz, Tobias Witting, Marc J. J. Vrakking
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.
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 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.
High-repetition-rate attosecond pulse sources are indispensable tools of time-resolved studies of electron dynamics, such as coincidence spectroscopy and experiments with high demands on statistics or signal-to-noise ratio, especially in case of solid and big molecule samples in chemistry and biology. Although with the high-repetition-rate lasers such attosecond pulses in a pump-probe configuration are possible to achieve, until now only a few such light sources have been demonstrated. Here, by shaping the driving laser to an annular beam, a 100-kHz attosecond pulse train (APT) is reported wit…
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…
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 new routes to generating a train of attosecond pulses. The methods are extremely simple and robust; we need to place only a few thin dispersive materials in the optical path. We numerically demonstrate the generation of a train of attosecond pulses with a transform-limited pulse duration of 728 as and a repetition period of 8.03 fs in gaseous parahydrogen.
Liquid dye lasers have long been considered as ideal tunable laser sources in the visible range but are bulky, expensive, and require a complex system for dye circulation. Here, we present a system that relies on a low-cost blue laser diode as the pump source and a sealed dye cell with no flowing circuitry, resulting in a device that combines the convenience and size of a solid-state device with the stability of a liquid organic laser. A very high photo-stability is obtained (up to 1.2 x 10$^9$ pulses or 12 days at 1 kHz), which is five orders of magnitude higher than a solid-state dye laser o…
We demonstrate a compact source of energetic and phase-locked multi-terahertz pulses at a repetition rate of 190 kHz. Difference frequency mixing of the fundamental output of an Yb:KGW amplifier with the idler of an optical parametric amplifier in GaSe and LiGaS2 crystals yields a passively phase-locked train of waveforms tunable between 12 and 42 THz. The shortest multi-terahertz pulses contain 1.8 oscillation cycles within the intensity FWHM. Pulse energies of up to 0.16 μJ and peak electric fields of 13 MV/cm are achieved. Electro-optic sampling reveals a phase stability better than 0.1 $π$…
Coherent soft x-ray (SXR) sources enable fundamental studies in the important water window spectral region. Until now, such sources have been limited to repetition rates of 1 kHz or less, which limits count rates and signal-to-noise ratio for a variety of experiments. SXR generation at high repetition rate has remained challenging because of the missing high-power mid-infrared (mid-IR) laser sources to drive the high-harmonic generation (HHG) process. Here we present a mid-IR optical parametric chirped pulse amplifier (OPCPA) centered at a wavelength of 2.2 μm and generating 16.5-fs pulses (2.…
A high repetition rate, picosecond THz parametric amplifier (TPA) with a LiNbO3 (LN) crystal has been demonstrated in this work. At 10 kHz repetition rate, a peak power of 200 W and an average power of 12 μW have been obtained over a wide range around 2 THz; at 100 kHz repetition rate, a maximum peak power of 18 W and average power of 10.8 μW have been obtained. The parametric gain of the LN crystal was also investigated and a modified Schwarz-Maier model was introduced to interpret the experimental results.
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.
We demonstrate 14.3-attosecond timing jitter [integrated from 10 kHz to 94 MHz offset frequency] optical pulse trains from 188-MHz repetition-rate mode-locked Yb-fiber lasers. In order to minimize the timing jitter, we shorten the non-gain fiber length to shorten the pulsewidth and reduce excessive higher-order nonlinearity and nonlinear chirp in the fiber laser. The measured jitter spectrum is limited by the amplified spontaneous emission limited quantum noise in the 100 kHz - 1 MHz offset frequency range, while it was limited by the relative intensity noise-converted jitter in the lower offs…
We demonstrate ultra-low timing jitter optical pulse trains from free- running, 80 MHz repetition rate, mode-locked Yb-fiber lasers. Timing jitter of various mode-locking conditions at close-to-zero intra-cavity dispersion (-0.004 to +0.002 ps2 range at 1040 nm center wavelength) is characterized using a sub-20-attosecond-resolution balanced optical cross-correlation method. The measured lowest rms timing jitter is 175 attoseconds when integrated from 10 kHz to 40 MHz (Nyquist frequency) offset frequency range, which corresponds to the record-low timing jitter from free-running mode-locked fib…
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…
We report on a multi-mJ 2.1-$μ$m OPCPA system operating at a 1-kHz repetition rate, pumped by a picosecond cryogenic Yb:YAG pump laser, and the phase-matched high-flux high-harmonic soft X-ray generation.
We present a rapid-scan, time-domain terahertz spectrometer employing femtosecond Er:fiber technology and an acousto-optic delay with attosecond precision, enabling scanning of terahertz transients over a 12.4 ps time window at a waveform refresh rate of 36 kHz, and a signal-to-noise ratio of $1.7 \times 10^5/\sqrt{\rm Hz}$. Our approach enables real-time monitoring of dynamic THz processes at unprecedented speeds, which we demonstrate through rapid 2D thickness mapping of a spinning teflon disc at a precision of $10\,\rm nm/\sqrt{\rm Hz}$. The compact, all-optical design ensures alignment-fre…
We have produced a soft x-ray supercontinuum with a pulse energy of 0.24-$μ$J using high-order harmonics from a multiterawatt, 10-Hz, stable, three-channel waveform synthesizer [Sci. Adv. eaay2802 (2020)]. We report here an attosecond streaking scheme, which is designed for measuring low-repetition-rate, high-energy, isolated attosecond pulses. The retrieved pulse duration is 226 as, which conclusively demonstrates the realization of 1.1-gigawatt isolated attosecond pulses at the generation point. The gigawatt-level peak power of this tabletop, isolated-attosecond-pulse light source is equival…
We report on an environmentally stable, Yb-doped, all-normal dispersion, mode-locked fibre laser that is capable of creating broadband pulses with ultra-low repetition rates. Specifically, through careful positioning of fibre sections in an all-PM-fibre cavity mode-locked with a nonlinear amplifying loop mirror, we achieve stable pulse trains with repetition rates as low as 506 kHz. The pulses have several nanojules of energy and are compressible down to ultrashort (< 500 fs) durations.
Time-resolved femtosecond stimulated Raman spectroscopy (FSRS) is a powerful tool for investigating ultrafast structural and vibrational dynamics in light absorbing systems. However, the technique generally requires exposing a sample to high laser pulse fluences and long acquisition times to achieve adequate signal-to-noise ratios. Here, we describe a timeresolved FSRS instrument built around a Yb ultrafast amplifier operating at 200 kHz, and address some of the unique challenges that arise at high repetition-rates. The setup includes detection with a 9 kHz CMOS camera and an improved dual-cho…
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…
Bright, coherent soft X-ray (SXR) radiation is essential to a variety of applications in fundamental research and life sciences. So far, high photon flux in this spectral region can only be delivered by synchrotrons, free electron lasers or high-order harmonic generation (HHG) sources, which are driven by kHz-class repetition rate lasers with very high peak powers. Here, we establish a novel route toward powerful and easy-to-use SXR sources by presenting a compact experiment, in which nonlinear pulse self-compression to the few-cycle regime is combined with phase-matched HHG in a single, heliu…
A compact pulsed Nd:LuAG laser at 1064 nm based on the self-Q-switching technique is reported, having the output power as high as 6.61 W at the incident pump power of 21.32 W, corresponding to the optical conversion efficiency of ~31 %. The temporal width of the pulse was in the range from 532.2 ns to 652.6 ns, and the repetition rate varied between 488.6 kHz and 551.9 kHz. To the best of our knowledge, this is the first report on the self-Q-switching Nd:LuAG laser. Possible reasons for the self-Q-switching of Nd:LuAG were also provided, and the factor leading to the high repetition rate was a…
We present a near-infrared optical parametric chirped-pulse amplifier (OPCPA) and soft X-ray (SXR) high-harmonic generation system. The OPCPA produces few-cycle pulses at a center wavelength of 800 nm and operates at a high repetition rate of 100 kHz. It is seeded by fully programmable amplitude and phase controlled ultra-broadband pulses from a Ti:sapphire oscillator. The output from the OPCPA system was compressed to near-transform-limited 9.3-fs pulses. High-power operation up to an average power of 35 W was achieved, and a fully characterized pulse compression was recorded for a power leve…
We experimentally demonstrate that the transmission of a 1030~nm, 1.3~ps laser beam of 100 mJ energy through fog increases when its repetition rate increases to the kHz range. Due to the efficient energy deposition by the laser filaments in the air, a shockwave ejects the fog droplets from a substantial volume of the beam, at a moderate energy cost. This process opens prospects for applications requiring the transmission of laser beams through fogs and clouds.
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…
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 report a 21-W mid-IR OPCPA that generates 131-μJ and 97 fs (sub-9-cycle) pulses at 160 kHz repetition rate and at a centre wavelength of 3.25 μm. Pulse-to-pulse stability of the CEP-stable output is excellent with 0.33% rms over 288 million pulses (30 min) and compression close to a single optical cycle was achieved through soliton self- compression inside a gas-filled mid-IR anti-resonant-guiding photonic crystal fibre. Without any additional compression device, stable generation of 14.5 fs (1.35-optical-cycle) pulses was achieved at an average power of 9.6 W. The resulting peak power of 3…
We present a 100 kHz optical parametric chirped pulse amplifier (OPCPA) developed for strong-field attosecond physics and soft-X-ray transient absorption experiments. The system relies on noncollinear potassium titanyl arsenate (KTA) booster OPCPAs and is pumped by a 240 W, 1.1 ps Yb:YAG Innoslab chirped pulse laser amplifier. Two optically synchronized infrared output beams are simultaneously available: a 430 μJ, 51 fs, carrier-envelope phase (CEP) stable beam at 1.55 μm and an angular-dispersion-compensated, 125 μJ, 73 fs beam at 3.1 μm.
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…
The output of a 200 kHz, 34 W, 300 fs Yb amplifier is compressed to 31 fs with > 88 % efficiency to reach a peak power of 2.5 GW, which to date is a record for a single-stage bulk multi-pass cell. Despite operation 80 times above the critical power for self-focusing in bulk material, the setup demonstrates excellent preservation of the input beam quality. Extensive beam and pulse characterizations are performed to show that the compressed pulses are promising drivers for high harmonic generation and nonlinear optics in gases or solids.
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…
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 …
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 demonstrate a femtosecond pump-probe spectrometer which utilizes a white light supercontinuum as input, and relies on mutual synchronization of acousto-optical chopper, pump-probe delay stage and the CCD camera to record shot-to-shot pump-probe spectra while the pump-probe delay is scanned synchronously with the laser repetition rate. The unique combination of technologies implemented here allows for electronically controllable and repetition-rate scalable detection throughput that is only limited by the camera frame rate. Despite RMS white-light probe fluctuations of ~5.5%, fully leveragin…
