Generation and characterization of tailored MIR waveforms for steering molecular dynamics

The dream of physico-chemists to control molecular reactions with light beyond electronic excitations pushes the development of laser pulse shaping capabilities in the mid-infrared (MIR) spectral range. Here, we present a compact optical parametric amplifier platform for the generation and shaping of MIR laser pulses in the wavelength range between 8 μm and 15 μm. Opportunities for judiciously tailoring the electromagnetic waveform are investigated, demonstrating light field control with a spectral resolution of 59 GHz at a total spectral bandwidth of 5 THz. In experiments focusing on spectral amplitude manipulation these parameters result in a time window of 1.8 ps available for shaping the temporal pulse envelope and a phase modulation resolution of 100 mrad for several picosecond delays

XUV fluorescence as a probe of laser-induced helium nanoplasma dynamics

XUV fluorescence spectroscopy provides information on energy absorption and dissipation processes taking place in the interaction of helium clusters with intense femtosecond laser pulses. The present experimental results complement the physical picture derived from previous electron and ion spectroscopic studies of the generated helium nanoplasma. Here, the broadband XUV fluorescence emission from high-lying Rydberg states that covers the spectral region from $6p \to 1s$ at 53.0 eV all the way to photon energies corresponding to the ionization potential of He$^+$ ions at 54.4 eV is observed directly. The cluster size-dependent population of these states in the expanding nanoplasma follows the well-known bottleneck model. The results support previous findings and highlight the important role of Rydberg states in the energetics and dynamics of laser-generated nanoplasma

Generation and Control of Ultrafast 10 μm Laser Pulses for Driving Chemical Dynamics

We demonstrate pulse shaping via acousto-optic modulation at a tunable mid-infrared source between wavelengths of 8–15 µm. e optimised pulse shapes aim at modification of molecular wavepackets in the electronic ground state

Versatile few-cycle high-energy MID-IR OPCPA for nonlinear optics, spectroscopy and imaging

High-power, high-energy, ultrashort, mid-infrared (MID-IR) laser systems operating at high repetition rates are of considerable interest for many science applications, such as coherent vibrational spectroscopy, label-free imaging, time-resolved pump-probe and high-harmonic generation studies. We developed an optical parametric chirped-pulse amplifier (OPCPA) system employing a difference-frequency generation in a lithium gallium sulfide nonlinear crystal in the final amplifier stage, which provides in principle the possibility for passive carrier-envelop-phase (CEP) stability. The OPCPA efficiently down-converts a 1 μm 200 $μ$J Yb-YAG pump pulse into the MID-IR spectral range generating $μ$J-level pulses at a repetition rate of 200 kHz. Two modes of operations providing complimentary MID-IR pulse properties are presented. Depending on the envisaged application, one can switch between (a) a wavelength-tunable (4.2–11 μm) source and (b) a broadband source centered at ≈8.5 μm by controlling the group-delay dispersion of the signal pulse. The broadband, high-energy MID-IR pulses have a short pulse duration of 74±2 fs, which corresponds to only ≈3 optical cycles at the central wavelength of 8.5 μm

Full characterization of a phase-locked DUV double pulse generated in an all-reflective shaping setup working under grazing incidence in a broad spectral range

Controlling the temporal and spectral properties of ultrashort laser pulses in the visible and near-infrared spectral range by means of a femtosecond pulse-shaping device is a powerful tool with many applications in ultrafast spectroscopy. A major and successful concept is known as the 4f design, which has a symmetric zero-dispersion-compressor geometry. Most 4f pulse shapers rely on using transmissive optics in their beam path limiting the operational wavelength ranges. In the present contribution, we use an all-reflective shaping setup to generate a phase-locked 266 nm double pulse to benchmark its performance in the limit of short wavelengths. The setup comprises the complete spectral amplitude and phase diagnostics for quantitative analysis of the pulse properties before and after the shaper using the technique of frequency-resolved optical gating. The measured time–frequency spectra are in good agreement with optical simulations. The geometry and hardware of the device including the optical components are designed, such that all harmonics of the deep UV pulses travel the same path, giving the instrument the ability to work with soft X-ray pulses, under vacuum conditions, down to the few-nanometer wavelength scale