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Coherent dual-comb spectroscopy (DCS) enables high-resolution measurements at high speeds without the trade-off between resolution and update rate inherent to mechanical delay scanning approaches. However, high system complexity and limited measurement sensitivity remain major challenges for DCS. Here, we address these challenges via a wavelength-tunable dual-comb optical parametric oscillator (OPO) combined with an up-conversion detection method. The OPO is tunable in the short-wave infrared (1300-1670 nm range) and mid-infrared (2700- 5000 nm range) where many molecules have strong absorption bands. Both OPO pump beams are generated in a single spatially-multiplexed laser cavity, while both signal and idler beams are generated in a single spatially-multiplexed OPO cavity. The near-common path of the combs in this new configuration enables comb-line-resolved and aliasing-free measurements in free-running operation. By limiting the instantaneous idler bandwidth to below 1 THz, we obtain a high power per comb line in the mid-infrared of up to 160 $\mu$W. With a novel intra-cavity nonlinear up-conversion scheme based on cross-comb spectroscopy, we leverage these power levels while overcoming the sensitivity limitations of direct mid-infrared detection, leading to a high signal-to-noise ratio (50.2 dB Hz$^{1/2}$) and record-level dual-comb figure of merit (3.5\times 10^8 Hz$^{1/2}$). As a proof of concept, we demonstrate the detection of methane with 2-ppm concentration over 3-m path length. Our results demonstrate a new paradigm for DCS compatible with high-sensitivity and high-resolution measurements over a wide spectral range., Comment: Supplementary Information included

Dual-comb generation from a single laser cavity provides a simple and high-performance solution to time sampling applications. We demonstrate a compact single-cavity dual-comb laser operating at gigahertz repetition rates and high repetition rate differences up to more than 100 kHz with sub-100 fs pulse duration. The single cavity approach leads to passive common noise suppression resulting in ultra-low relative timing jitter and fully resolvable comb lines in free-running operation. We showcase the laser performance with two application demonstrations: (a) time-domain spectroscopy of acetylene in the near-infrared via computational comb line tracking and (b) free-space THz time domain spectroscopy and thickness-measurements via adaptive sampling. For (b) we use efficient state-of the art iron-doped InGaAs photoconductive antennas to generate and detect the THz light. Here we operate these devices with an efficient Yb-based gigahertz repetition rate laser for the first time. One optical comb generates the THz light, while the other probes it via equivalent time sampling. We obtain signal strengths comparable to reference measurements with MHz repetition rate Er-based laser systems while achieving close to 1 GHz spectral resolution (defined by the comb line spacing) and generating THz frequencies up to 3 THz. By carrying out a careful investigation of the noise properties of the laser we confirm that the free-running gigahertz dual-comb oscillator provides a rapid yet highly precise optical delay sweep from a simple setup. Therefore, our approach will be beneficial for high-update rate time sampling and time-domain spectroscopy applications.

Femtosecond dual-comb lasers have revolutionized linear Fourier-domain spectroscopy by offering a rapid motion-free, precise and accurate measurement mode with easy registration of the combs beat note in the RF domain. Extensions of this technique found already application for nonlinear time-resolved spectroscopy within the energy limit available from sources operating at the full oscillator repetition rate. Here, we present a technique based on time filtering of femtosecond frequency combs by pulse gating in a laser amplifier. This gives the required boost to the pulse energy and provides the flexibility to engineer pairs of arbitrarily delayed wavelength-tunable pulses for pump-probe techniques. Using a dual-channel millijoule amplifier, we demonstrate programmable generation of both extremely short, fs, and extremely long (>ns) interpulse delays. A predetermined arbitrarily chosen interpulse delay can be directly realized in each successive amplifier shot, eliminating the massive waiting time required to alter the delay setting by means of an optomechanical line or an asynchronous scan of two free-running oscillators. We confirm the versatility of this delay generation method by measuring chi^(2) cross-correlation and chi^(3) multicomponent population recovery kinetics.

Ultrafast laser systems operating with high-average power in the wavelength range from 1.9 um to 3 um are of interest for a wide range of applications for example in spectroscopy, material processing and as drivers for secondary sources in the XUV spectral region. In this area, laser systems based on holmium-doped gain materials directly emitting at 2.1 um have made significant progress over the past years, however so far only very few results were demonstrated in power-scalable high-power laser geometries. In particular, the thin-disk geometry is promising for directly modelocked oscillators with high average power levels that are comparable to amplifier systems at MHz repetition rate. In this paper, we demonstrate Semiconductor Saturable Absorber Mirror (SESAM) modelocked Ho:YAG thin-disk lasers (TDLs) emitting at 2.1 um wavelength with record-holding performance levels. In our highest average power configuration, we reach 50 W of average power, with 1.13 ps pulses, 2.11 uJ of pulse energy and ~1.9 MW of peak power. To the best of our knowledge, this represents the highest average power, as well as the highest output pulse energy so far demonstrated from a modelocked laser in the 2 um wavelength region. This record performance level was enabled by the recent development of high-power GaSb-based SESAMs with low loss, adapted for high intracavity power and pulse energy. We also explore the limitations in terms of reaching shorter pulse durations at high power with this gain material in the disk geometry and using SESAM modelocking, and present first steps in this direction, with the demonstration of 30 W of output power, with 692 fs pulses in another laser configuration., Comment: 12 pages, 10 figures

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. Furthermore, the proposed approach allows for continuous and precise tracking of the sampling rate. To demonstrate the technique, we perform a detailed characterization of a single-mode-diode pumped $\mathrm{Yb:CaF_2}$ dual-comb laser from a free-running polarization-multiplexed cavity. This new laser produces 115 fs pulses at 160 MHz repetition rate, with 130 mW of average power in each comb. The detection noise floor for the relative timing jitter between the two pulse trains reaches $8.0 \times 10^{-7} \, \mathrm{fs}^2/\mathrm{Hz} \; ( \sim 896 \: \mathrm{zs}/\sqrt{\mathrm{Hz}} )$, and the relative root mean square (rms) timing jitter is 13 fs when integrating from 100 Hz to 1 MHz. This performance indicates that the demonstrated laser is highly compatible with practical dual-comb spectroscopy, ranging, and sampling applications. Furthermore, our results show that the relative timing noise measurement technique can characterize dual-comb systems operating in free-running mode or with finite repetition rate differences while providing a sub-attosecond resolution, which was not feasible with any other approach before., Comment: 19 pages, 6 figures, 78 references; typos corrected, layout adjusted

We present a free-running 80-MHz dual-comb polarization-multiplexed solid-state laser which delivers 1.8 W of average power with 110-fs pulse duration per comb. With a high-sensitivity pump-probe setup, we apply this free-running dual-comb laser to picosecond ultrasonic measurements. The ultrasonic signatures in a semiconductor multi-quantum-well structure originating from the quantum wells and superlattice regions are revealed and discussed. We further demonstrate ultrasonic measurements on a thin-film metalized sample and compare these measurements to ones obtained with a pair of locked femtosecond lasers. Our data show that a free-running dual-comb laser is well-suited for picosecond ultrasonic measurements and thus it offers a significant reduction in complexity and cost for this widely adopted non-destructive testing technique.

Realistic attosecond wave packets have complex profiles that, in dispersive conditions, rapidly broaden or split into multiple components. Such behaviors are encoded in sharp features of the wave packet spectral phase. Here, we exploit the quantum beating between one- and two-photon transitions in an attosecond photoionization experiment to measure the photoelectron spectral phase continuously across a broad energy range. Supported by numerical simulations, we demonstrate that this experimental technique is able to reconstruct sharp fine-scale features of the spectral phase, continuously as a function of energy and across the full spectral range of the pulse train, thus beyond the capabilities of existing attosecond spectroscopies. In a proof-of-principle experiment, we retrieve the periodic modulations of the spectral phase of an attosecond pulse train due to the individual chirp of each harmonic.

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 level of 22.5 W, demonstrating pulses with a peak power greater than 21 GW. We demonstrate that at such high repetition rates, spatiotemporally flattened pump pulses can be achieved through a cascaded second-harmonic generation approach with an efficiency of more than 70%, providing a compelling OPCPA architecture for power-scaling ultra-broadband systems in the near-infrared. The output of this 800-nm OPCPA system was used to generate SXR radiation reaching 190 eV photon energy through high-harmonic generation in helium.

Attosecond measurements reveal new physical insights in photo ionization dynamics from atoms, molecules and condensed matter. However, on such time scales even small timing jitter can significantly reduce the time resolution in pump-probe measurements. Here, we propose a novel technique to retrieve attosecond delays from a well established attosecond interferometric technique, referred to as Reconstruction of Attosecond Beating By Interference of Two-photon Transition (RABBITT), which is unaffected by timing jitter and significantly improves the precision of state-of-the-art experiments. We refer to this new technique as the Timing-jitter Unaffected Rabbitt Time deLay Extraction method, in short TURTLE. Using this TURTLE technique we could measure the attosecond ionization time delay between Argon and Neon in full agreement with prior measurements. The TURTLE technique allows for attosecond time resolution without pump-probe time delay stabilization and without attosecond pulses because only a stable XUV frequency comb is required as a pump. This will more easily enable attosecond measurements at FELs for example and thus provide a valuable tool for attosecond science. Here we also make a MATLAB code available for the TURTLE fit with appropriate citation in return.

Coherent, broadband pulses of extreme ultraviolet (XUV) light provide a new and exciting tool for exploring attosecond electron dynamics. Using photoelectron streaking, interferometric spectrograms can be generated that contain a wealth of information about the phase properties of the photoionization process. If properly retrieved, this phase information reveals attosecond dynamics during photoelectron emission such as multielectron dynamics and resonance processes. However, until now, the full retrieval of the continuous electron wavepacket phase from isolated attosecond pulses has remained challenging. Here, after elucidating key approximations and limitations that hinder one from extracting the coherent electron wavepacket dynamics using available retrieval algorithms, we present a new method called Absolute Complex Dipole transmission matrix element reConstruction (ACDC). We apply the ACDC method to experimental spectrograms to resolve the phase and group delay difference between photoelectrons emitted from Ne and Ar. Our results reveal subtle dynamics in this group delay difference of photoelectrons emitted form Ar. These group delay dynamics were not resolvable with prior methods that were only able to extract phase information at discrete energy levels, emphasizing the importance of a complete and continuous phase retrieval technique such as ACDC. Here we also make this new ACDC retrieval algorithm available with appropriate citation in return.

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 {\mu}m and generating 16.5-fs pulses (2.2 oscillation cycles of the carrier wave) with 25 W of average power and a peak power exceeding 14 GW at 100-kHz pulse repetition rate. This corresponds to the highest reported peak power for high-repetition-rate mid-IR laser systems. The output of this 2.2-{\mu}m OPCPA system was used to generate a SXR continuum extending beyond 0.6 keV through HHG in a high-pressure gas cell.

Attosecond photoionisation time delays reveal information about the potential energy landscape an outgoing electron wavepacket probes upon ionisation. In this study we experimentally quantify, for the first time, the dependence of the time delay on the angular momentum of the liberated photoelectrons. For this purpose, electron quantum-path interference spectra have been resolved in energy and angle using a two-color attosecond pump-probe photoionisation experiment in helium. A fitting procedure of the angle-dependent interference pattern allows us to disentangle the relative phase of all four quantum pathways that are known to contribute to the final photoelectron signal. In particular, we resolve the dependence on the angular momentum of the delay of one-photon transitions between continuum states, which is an essential and universal contribution to the total photoionization delay observed in attosecond pump-probe measurements. For such continuum-continuum transitions, we measure a delay between outgoing s- and d-electrons as large as 12 as close to the ionisation threshold in helium. Both single-active-electron and first-principles ab initio simulations confirm this observation for helium and hydrogen, demonstrating the universality of the observed delays.

In strong-field ionization interferences between electron trajectories create a variety of interference structures in the final momentum distributions. Among them, the interferences between electron pathways that are driven directly to the detector and the ones that rescatter significantly with the parent ion lead to holography-type interference patterns that received great attention in recent years. In this work, we study the influence of the magnetic field component onto the holographic interference pattern, an effect beyond the electric dipole approximation, in experiment and theory. The experimentally observed nondipole signatures are analyzed via quantum trajectory Monte Carlo simulations. We provide explanations for the experimentally demonstrated asymmetry in the holographic interference pattern and its non-uniform photoelectron energy dependence as well as for the variation of the topology of the holography-type interference pattern along the laser field direction. Analytical scaling laws of the interference features are derived, and their direct relation to either the focal volume averaged laser intensities, or to the peak intensities are identified. The latter, in particular, provides a direct access to the peak intensity in the focal volume.

During multi-photon ionization of an atom it is well understood how the involved photons transfer their energy to the ion and the photoelectron. However, the transfer of the photon linear momentum is still not fully understood. Here, we present a time-resolved measurement of linear momentum transfer along the laser pulse propagation direction. Beyond the limit of the electric dipole approximation we observe a time-dependent momentum transfer. We can show that the time-averaged photon radiation pressure picture is not generally applicable and the linear momentum transfer to the photoelectron depends on the ionization time within the electromagnetic wave cycle using the attoclock technique. We can mostly explain the measured linear momentum transfer within a classical model for a free electron in a laser field. However, corrections are required due to the interaction of the outgoing photoelectron with the parent ion and due to the initial momentum when the electron appears in the continuum. The parent ion interaction induces a measurable negative attosecond time delay between the appearance in the continuum of the electron with minimal linear momentum transfer and the point in time with maximum ionization rate.

We theoretically investigate the role of intra-band transitions in laser-induced carrier-generation for different photon energy regimes: (i) strongly off-resonant, (ii) multi-photon resonant, and (iii) resonant conditions. Based on the analysis for the strongly off-resonant and multi-photon resonant cases, we find that intra-band transitions strongly enhance photo-carrier generation in both multi-photon absorption and tunneling excitation regimes, and thus, they are indispensable for describing the nonlinear photo-carrier generation processes. Furthermore, we find that intra-band transitions enhance photo-carrier generation even in the resonant condition, opening additional multi-photon excitation channels once the laser irradiation becomes sufficiently strong. The above findings suggest a potential for efficient control of photo-carrier generation via multi-color laser pulses through optimization of the contributions from intra-band transitions.

Time delays of electrons emitted from an isotropic initial state and leaving behind an isotropic ion are assumed to be angle-independent. Using an interferometric method involving XUV attosecond pulse trains and an IR probe field in combination with a detection scheme, which allows for full 3D momentum resolution, we show that measured time delays between electrons liberated from the $1s^2$ spherically symmetric ground state of helium depend on the emission direction of the electrons relative to the linear polarization axis of the ionizing XUV light. Such time-delay anisotropy, for which we measure values as large as 60 attoseconds, is caused by the interplay between final quantum states with different symmetry and arises naturally whenever the photoionization process involves the exchange of more than one photon in the field of the parent-ion. With the support of accurate theoretical models, the angular dependence of the time delay is attributed to small phase differences that are induced in the laser-driven continuum transitions to the final states. Since most measurement techniques tracing attosecond electron dynamics involve the exchange of at least two photons, this is a general, significant, and initially unexpected effect that must be taken into account in all such photoionization measurements., Comment: 17 pages, 4 figures

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. Compressing the full transmitted power through the fiber (118 W) could lead to a compressed output of >100 W of average power and >100 MW of peak power with an average power compression efficiency of 88%. This simple laser system with only one ultrafast laser oscillator and a simple single-pass fiber pulse compressor, generating both high peak power >100 MW and sub-100-fs pulses at megahertz repetition rate, is very interesting for many applications such as high harmonic generation and attosecond science with improved signal-to-noise performance.