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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 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.

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.

We present a 1.75-GHz self-referenceable frequency comb from a vertical external-cavity surface-emitting laser (VECSEL) passively modelocked with a semiconductor saturable absorber mirror (SESAM). The VECSEL delivers 231-fs pulses with an average power of 100 mW and is optimized for stable and reliable operation. The optical spectrum was centered around 1038 nm and nearly transform-limited with a full width half maximum (FWHM) bandwidth of 5.5 nm. The pulses were first amplified to an average power of 5.5 W using a backward-pumped Yb-doped double-clad large mode area (LMA) fiber and then compressed to 85 fs with 2.2 W of average power with a passive LMA fiber and transmission gratings. Subsequently, we launched the pulses into a highly nonlinear photonic crystal fiber (PCF) and generated a coherent octave-spanning supercontinuum (SC). We then detected the carrier-envelope offset (CEO) frequency (fCEO) beat note using a standard f-to-2f-interferometer. The fCEO exhibits a signal-to-noise ratio of 17 dB in a 100-kHz resolution bandwidth and a FWHM of 10 MHz. To our knowledge, this is the first report on the detection of the fCEO from a semiconductor laser, opening the door to fully stabilized compact frequency combs based on modelocked semiconductor disk lasers.

We demonstrate a new regime for mid-infrared optical parametric chirped pulse amplification (OPCPA) based on achromatic quasi-phase-matching. Our mid-infrared OPCPA system is based on collinear aperiodically poled lithium niobate (APPLN) pre-amplifiers and a non-collinear PPLN power amplifier. The idler output has a bandwidth of 800 nm centered at 3.4 $\mu$m. After compression, we obtain a pulse duration of 44.2 fs and a pulse energy of 21.8 $\mu$J at a repetition rate of 50 kHz. We explain the wide applicability of the non-collinear QPM amplification scheme we used, including how it can enable octave-spanning OPCPA in a single device when combined with an aperiodic QPM grating.