Marcus Ossiander

Carrier-envelope-phase-stable, 1.2 mJ, 1.5 cycle laser pulses at 2.1 μm

We produce 1.5 cycle (10.5 fs), 1.2 mJ, 3 kHz carrier-envelope-phase-stable pulses at 2.1 μm carrier wavelength, from a three-stage optical parametric chirped-pulse amplifier system, pumped by an optically synchronized 1.6 ps Yb:YAG thin disk laser. A chirped periodically poled lithium niobate crystal is used to generate the ultrabroad spectrum needed for a 1.5 cycle pulse through difference frequency mixing of spectrally broadened pulse from a Ti:sapphire amplifier. It will be an ideal tool for producing isolated attosecond pulses with high photon energies.

Active stabilization for optically synchronized optical parametric chirped pulse amplification

The development of new high power laser sources tends toward optical parametric chirped pulse amplification (OPCPA) in recent years. One of the difficulties in OPCPA is the the temporal overlap between pump and seed pulses. In this work we characterize our timing jitter on a single-shot basis using spectrally resolved cross-correlation in combination with a position sensitive detector. A commercial beam stabilization is adapted to actively enhance temporal overlap. This delay-stabilizer reduces the RMS jitter from σ = 127 fs down to σ = 24 fs. The enhanced temporal overlap is demonstrated in our frontend and we propose the scheme to be applicable in many optically synchronized high-repetition-rate OPCPA systems.

Chromium/scandium multilayer mirrors for isolated attosecond pulses at 145 eV

Recent advances in the development of attosecond soft x-ray sources toward photon wavelengths below 10 nm are also driving the development of suited broadband multilayer optics for steering and shaping attosecond pulses. We demonstrate that current attosecond experiments in the sub-200-eV range benefit from these improved optics. We present our achievements in utilizing ion-beam-deposited chromium/scandium (Cr/Sc) multilayer mirrors, optimized by tailored material dependent deposition and interface polishing, for the generation of single attosecond pulses from a high-harmonic cut-off spectrum at a central energy of 145 eV. Isolated attosecond pulses have been measured by soft x-ray-pump/NIR-probe electron streaking experiments and characterized using frequency-resolved optical gating for complete reconstruction of attosecond bursts (FROG/CRAB). The results demonstrate that Cr/Sc multilayer mirrors can be used as efficient attosecond optics for reflecting 600-attosecond pulses at a photon energy of 145 eV, which is a prerequisite for present and future attosecond experiments in this energy range.

Absolute timing of the photoelectric effect

Photoemission spectroscopy is central to understanding the inner workings of condensed matter, from simple metals and semiconductors to complex materials such as Mott insulators and superconductors1. Most state-of-the-art knowledge about such solids stems from spectroscopic investigations, and use of subfemtosecond light pulses can provide a time-domain perspective. For example, attosecond (10−18 seconds) metrology allows electron wave packet creation, transport and scattering to be followed on atomic length scales and on attosecond timescales2–7. However, previous studies could not disclose the duration of these processes, because the arrival time of the photons was not known with attosecond precision. Here we show that this main source of ambiguity can be overcome by introducing the atomic chronoscope method, which references all measured timings to the moment of light-pulse arrival and therefore provides absolute timing of the processes under scrutiny. Our proof-of-principle experiment reveals that photoemission from the tungsten conduction band can proceed faster than previously anticipated. By contrast, the duration of electron emanation from core states is correctly described by semiclassical modelling. These findings highlight the necessity of treating the origin, initial excitation and transport of electrons in advanced modelling of the attosecond response of solids, and our absolute data provide a benchmark. Starting from a robustly characterized surface, we then extend attosecond spectroscopy towards isolating the emission properties of atomic adsorbates on surfaces and demonstrate that these act as photoemitters with instantaneous response. We also find that the tungsten core-electron timing remains unchanged by the adsorption of less than one monolayer of dielectric atoms, providing a starting point for the exploration of excitation and charge migration in technologically and biologically relevant adsorbate systems.The absolute timing of the photoelectric effect has proved difficult to measure, but the delay between photon arrival at a tungsten surface and ejection of photoelectrons has now been determined.

Carrier frequency tuning of few-cycle light pulses by a broadband attenuating mirror

We demonstrate the performance of a novel multilayer dielectric reflective thin-film attenuator capable of reshaping the super-octave spectrum of near-single-cycle visible laser pulses without deteriorating the phase properties of the reflected light. These novel broadband attenuating mirrors reshape in a virtually dispersion-free manner the incident spectrum such that the carrier wavelength of the reflected pulses shifts from ∼700  nm (Eγ=1.77  eV) to ∼540  nm (Eγ=2.25  eV) or beyond while maintaining their initial near-single-cycle pulse duration. This constitutes a viable approach to convert a number of established few-cycle ultrafast laser systems into sources with a selectable excitation wavelength to meet the requirements of single-color/multicolor high temporal resolution spectroscopic experiments.