Search

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.

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.

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.

A new Monte Carlo algorithm for phase-space sampling, named (MC)**3, is presented. It is based on Markov Chain Monte Carlo techniques but at the same time incorporates prior knowledge about the target distribution in the form of suitable phase-space mappings from a corresponding Multi-Channel importance sampling Monte Carlo. The combined approach inherits the benefits of both techniques while typical drawbacks of either solution get ameliorated., Comment: version accepted for publication in CPC, largely extended examples section