In attosecond and strong-field physics, the acquisition of data in an acceptable time demands the combination of high peak power with high average power. We report a 21 W mid-IR optical parametric chirped pulse amplifier (OPCPA) that generates 131 μJ and 97 fs (sub-9-cycle) pulses at a 160 kHz repetition rate and at a center wavelength of 3.25 μm. Pulse-to-pulse stability of the carrier envelope phase (CEP)-stable output is excellent with a 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 antiresonant-guiding photonic crystal fiber. 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 3.9 GW in combination with the near-single-cycle duration and intrinsic CEP stability makes our OPCPA a key-enabling technology for the next generation of extreme photonics, strong-field attosecond research, and coherent x-ray science.

Probing matter with light in the mid-infrared provides unique insight into molecular composition, structure, and function with high sensitivity. However, laser spectroscopy in this spectral region lacks the broadband or tunable light sources and efficient detectors available in the visible or near-infrared. We overcome these challenges with an approach that unites a compact source of phase-stable, single-cycle, mid-infrared pulses with room temperature electric field–resolved detection at video rates. The ultrashort pulses correspond to laser frequency combs that span 3 to 27 μm (370 to 3333 cm⁻¹), and are measured with dynamic range of >10⁶ and spectral resolution as high as 0.003 cm⁻¹. We highlight the brightness and coherence of our apparatus with gas-, liquid-, and solid-phase spectroscopy that extends over spectral bandwidths comparable to thermal or infrared synchrotron sources. This unique combination enables powerful avenues for rapid detection of biological, chemical, and physical properties of matter with molecular specificity.

We present a state-of-the-art compact high-energy mid-infrared (mid-IR) laser system for TW-level eight-cycle pulses at 7 μm. This system consists of an Er:Tm:Ho:fiber MOPA which serves as the seeder for a ZGP-based optical parametric chirped pulse amplification (OPCPA) chain, in addition to a Ho:YLF amplifier which is Tm:fiber pumped. Featuring all-optical synchronization, the system delivers 260 mJ pump energy at 2052 nm and 16 ps duration at 100 Hz with a stability of 0.8% rms over 20 min. We show that chirp inversion in the OPCPA chain leads to excellent energy extraction and aids in compression of the 7 μm pulses to eight optical cycles (188 fs) in bulk ${\mathrm{BaF}}_2$ with 93.5% efficiency. Using 21.7 mJ of the available pump energy, we generate 0.75 mJ energy pulses at 7 μm due to increased efficiency with a chirp inversion scheme. The pulse quality of the system’s output is shown by generating high harmonics in ZnSe which span up to harmonic order 13 with excellent contrast. The combination of the passive carrier-envelope phase stable mid-IR seed pulses and the high-energy 2052 nm picosecond pulses makes this compact system a key enabling tool for the next generation of studies on extreme photonics, strong field physics, and table-top coherent X-ray science.

B a G a 2 G e S e 6 (BGGSe) is a newly developed nonlinear material that is attractive for ultrabroad frequency mixing and ultrashort pulse generation due to its comparably low dispersion and high damage threshold. A numerical study shows the material’s capacity for octave-spanning mid-infrared pulse generation up to 18 µm. In a first experiment, we show that a long crystal length of 2.6 mm yields a pulse energy of 21 pJ at 100 MHz with a spectral bandwidth covering 5.8 to 8.5 µm. The electric field of the carrier-envelope-phase stable pulse is directly measured with electro-optical sampling and reveals a pulse duration of 91 fs, which corresponds to sub-four optical cycles, thus confirming some of the prospects of the material for ultrashort pulse generation and mid-infrared spectroscopy.

We study and describe the reshaping of ultrashort and broadband mid-IR optical pulses in an ambient atmosphere. While all pulse propagation undergoes dispersion and absorption, which causes pulse reshaping, the effects are strongly pronounced for broadband radiation in the mid-IR due to the orders of magnitude greater oscillator strengths of molecular constituents of our atmosphere. A noticeable macroscopic impact is a transition of the measured autocorrelation function from squared hyperbolic secant to Lorentzian, which we fully explain based on pulse propagation, including molecular free induction decay. Electro-optical sampling directly reveals the light wave response to atmospheric molecular free induction decay, and a Kramers–Kronig-based propagation model thoroughly explains the observation. The findings are essential for applications in sensing, standoff detection, high-energy pulse propagation, and energy delivery.