Compact realization of all-attosecond pump-probe spectroscopy.

The ability to perform attosecond-pump attosecond-probe spectroscopy (APAPS) is a longstanding goal in ultrafast science. While first pioneering experiments demonstrated the feasibility of APAPS, the low repetition rates (10 to 120 Hz) and the large footprints of existing setups have so far hindered the widespread exploitation of APAPS. Here, we demonstrate two-color APAPS using a commercial laser system at 1 kHz, straightforward post-compression in a hollow-core fiber, and a compact high-harmonic generation (HHG) setup.

Phase-locking of time-delayed attosecond XUV pulse pairs.

We present a setup for the generation of phase-locked attosecond extreme ultraviolet (XUV) pulse pairs. The attosecond pulse pairs are generated by high harmonic generation (HHG) driven by two phase-locked near-infrared (NIR) pulses that are produced using an actively stabilized Mach-Zehnder interferometer compatible with near-single cycle pulses. The attosecond XUV pulses can be delayed over a range of 400 fs with a sub-10-as delay jitter.

Experimental Control of Quantum-Mechanical Entanglement in an Attosecond Pump-Probe Experiment.

Entanglement is one of the most intriguing aspects of quantum mechanics and lies at the heart of the ongoing second quantum revolution, where it is a resource that is used in quantum key distribution, quantum computing, and quantum teleportation. We report experiments demonstrating the crucial role that entanglement plays in pump-probe experiments involving ionization, which are a hallmark of the novel research field of attosecond science. We demonstrate that the degree of entanglement in a bipartite ion + photoelectron system, and, as a consequence, the degree of vibrational coherence in the ion, can be controlled by tailoring the spectral properties of the attosecond extreme ultraviolet laser pulses that are used to create them.

8 fs laser pulses from a compact gas-filled multi-pass cell.

Compression of 42 fs, 0.29 mJ pulses from a Ti:Sapphire amplifier down to 8 fs (approximately 3 optical cycles) is demonstrated by means of spectral broadening in a compact multi-pass cell filled with argon. The efficiency of the nonlinear pulse compression is limited to 45 % mostly by losses in the mirrors of the cell.

27 W 2.1 µm OPCPA system for coherent soft X-ray generation operating at 10 kHz.

We developed a high power optical parametric chirped-pulse amplification (OPCPA) system at 2.1 µm harnessing a 500 W Yb:YAG thin disk laser as the only pump and signal generation source. The OPCPA system operates at 10 kHz with a single pulse energy of up to 2.

Photoemission from non-polar aromatic molecules in the gas and liquid phase.

The photoelectron spectra of both liquid and gas phase aromatic molecules are reported. The spectra were obtained using a 34.1 eV source produced by high harmonic generation and analysed with the help of high-level ab initio simulations using the reflection principle combined with path integral molecular dynamics simulations accounting for nuclear quantum effects for the gas phase.

Single-step fabrication of surface waveguides in fused silica with few-cycle laser pulses.

Direct laser writing of surface waveguides with ultrashort pulses is a crucial achievement towards all-laser manufacturing of photonic integrated circuits sensitive to their environment. In this Letter, few-cycle laser pulses (with a sub-10 fs duration) are used to produce subsurface waveguides in a non-doped, non-coated fused-silica substrate. The fabrication technique relies on laser-induced microdensification below the threshold for nanopore formation.

State-Resolved Probing of Attosecond Timescale Molecular Dipoles.

We report an experimental study of iodomethane attosecond transient absorption spectroscopy (ATAS) in the region of iodine 4d core-to-valence/Rydberg excitation. Similar to previous atomic experiments, extreme ultraviolet near-infrared (XUV-NIR) delay-dependent absorbance changes reflect a light-induced phase due to an NIR-field driven AC Stark shift of the excited states, as well as pathway interferences arising from couplings between neighboring states. As a novel aspect of molecular ATAS, we observe pronounced differences between the ATAS signatures of valence and Rydberg states.

Extreme-ultraviolet refractive optics.

Refraction is a well-known optical phenomenon that alters the direction of light waves propagating through matter. Microscopes, lenses and prisms based on refraction are indispensable tools for controlling light beams at visible, infrared, ultraviolet and X-ray wavelengths. In the past few decades, a range of extreme-ultraviolet and soft-X-ray sources has been developed in laboratory environments and at large-scale facilities.

Chirp-control of resonant high-order harmonic generation in indium ablation plumes driven by intense few-cycle laser pulses.

We have studied high-order harmonic generation (HHG) in an indium ablation plume driven by intense few-cycle laser pulses centered at 775 nm as a function of the frequency chirp of the laser pulse. We found experimentally that resonant emission lines between 19.7 eV and 22.

Continuous every-single-shot carrier-envelope phase measurement and control at 100 kHz.

With the emergence of high-repetition-rate few-cycle laser pulse amplifiers aimed at investigating ultrafast dynamics in atomic, molecular, and solid-state science, the need for ever faster carrier-envelope phase (CEP) detection and control has arisen. Here we demonstrate a high-speed, continuous, every-single-shot measurement and fast feedback scheme based on a stereo above-threshold ionization time-of-flight spectrometer capable of detecting the CEP and pulse duration at a repetition rate of up to 400 kHz. This scheme is applied to a 100 kHz optical parametric chirped pulse amplification few-cycle laser system, demonstrating improved CEP stabilization and allowing for CEP tagging.

Sub-4 fs laser pulses at high average power and high repetition rate from an all-solid-state setup.

The generation of high average power, carrier-envelope phase (CEP) stable, near-single-cycle pulses at a repetition rate of 100 kHz is demonstrated using an all solid-state setup. By exploiting self-phase modulation in thin quartz plates and air, the spectrum of intense pulses from a high-power, high repetition rate non-collinear optical parametric chirped pulse amplifier (NOPCPA) is extended to beyond one octave, and pulse compression down to 3.7 fs is achieved.

Role of Intrapulse Coherence in Carrier-Envelope Phase Stabilization.

The concept of coherence is of fundamental importance for describing the physical characteristics of light and for evaluating the suitability for experimental application. In the case of pulsed laser sources, the pulse-to-pulse coherence is usually considered for a judgment of the compressibility of the pulse train. This type of coherence is often lost during propagation through a highly nonlinear medium, and pulses prove incompressible despite multioctave spectral coverage.

CEP-stable few-cycle pulses with more than 190 μJ of energy at 100 kHz from a noncollinear optical parametric amplifier.

Noncollinear optical parametric amplifiers (NOPAs) have become the leading technique for the amplification of carrier-envelope phase (CEP)-stable, few-cycle pulses at high repetition rate and high average power. In this Letter, a NOPA operating at a repetition rate of 100 kHz delivering more than 24 W of average power before compression is reported. The amplified bandwidth supports sub-7 fs pulse durations and pulse compression close to the transform limit is realized.

Interferometric time-domain ptychography for ultrafast pulse characterization.

A novel pulse characterization method is presented, favorably combining interferometric frequency-resolved optical gating (FROG) and time-domain ptychography. This new variant is named ptychographic-interferometric frequency-resolved optical gating (πFROG). The measurement device is simple, bearing similarity to standard second-harmonic FROG, yet with a collinear beam geometry and an added bandpass filter in one of the correlator arms.

Angle-resolved coherent wave mixing using a 4 fs ultra-broad bandwidth laser.

We demonstrate angle-resolved coherent (ARC) wave mixing using 4 fs light pulses derived from a laser source that spans 550-1000 nm. We believe this to be the shortest pulse duration used to date in coherent multi-dimensional spectroscopy. The marriage of this ultra-broad band, few-cycle coherent source with the ARC technique will permit new investigations of the interplay between energy transfers and quantum superposition states spanning 8200  cm.

Attosecond physics at the nanoscale.

Recently two emerging areas of research, attosecond and nanoscale physics, have started to come together. Attosecond physics deals with phenomena occurring when ultrashort laser pulses, with duration on the femto- and sub-femtosecond time scales, interact with atoms, molecules or solids. The laser-induced electron dynamics occurs natively on a timescale down to a few hundred or even tens of attoseconds (1 attosecond  =  1 as  =  10 s), which is comparable with the optical field.

Strong-field ionization of clusters using two-cycle pulses at 1.8 μm.

The interaction of intense laser pulses with nanoscale particles leads to the production of high-energy electrons, ions, neutral atoms, neutrons and photons. Up to now, investigations have focused on near-infrared to X-ray laser pulses consisting of many optical cycles. Here we study strong-field ionization of rare-gas clusters (10 to 10 atoms) using two-cycle 1.

Spatio-temporal characterization of intense few-cycle 2 μm pulses.

We present a variant of spatially encoded spectral shearing interferometry for measuring two-dimensional spatio-temporal slices of few-cycle pulses centered around 2 μm. We demonstrate experimentally that the device accurately retrieves the pulse-front tilt caused by angular dispersion of two-cycle pulses. We then use the technique to characterize 500-650 μJ pulses from a hollow fiber pulse compressor, with durations as short as 7.

Time-domain ptychography of over-octave-spanning laser pulses in the single-cycle regime.

We report, to the best of our knowledge, the first application of time-domain ptychography for the characterization of few-cycle laser pulses. Our method enables zero-additional phase measurements of over-octave-spanning laser pulses in the single cycle regime. The spectral phase is recovered using a robust ptychography algorithm that requires no input apart from the measured data trace.

X-SEA-F-SPIDER characterization of over octave spanning pulses in the infrared range.

We show a practical implementation of a pulse characterization method for sub-cycle pulse measurements in the infrared spectral range based on spectral shearing interferometry. We employ spatially-encoded arrangement filter-based spectral phase interferometry for direct electric field reconstruction with external ancila pulses (X-SEA-F-SPIDER). We show merits and limitations of the setup and an in-depth comparison to another widely used temporal characterization technique - Second-Harmonic Generation Frequency Resolved Optical Gating (SHG-FROG).

Self-referenced characterization of space-time couplings in near-single-cycle laser pulses.

We report on the characterization of space-time couplings in high-energy sub-2-cycle 770 nm laser pulses using a self-referencing single-frame method. Using spatially encoded arrangement filter-based spectral phase interferometry for direct electric field reconstruction, we characterize few-cycle pulses with a wavefront rotation of 2.8×10  rev/s (1.

Single-shot implementation of dispersion-scan for the characterization of ultrashort laser pulses.

We demonstrate a single-shot ultrafast diagnostic, based on the dispersion-scan (d-scan) technique. In this implementation, rather than translating wedges to vary the dispersion as in scanning d-scan, the pulse to be measured experiences a spatially varying amount of dispersion in a prism. The resulting beam is then imaged into a second-harmonic generation crystal and an imaging spectrometer is used to measure the two-dimensional trace, which is analyzed using the d-scan retrieval algorithm.

A strong-field driver in the single-cycle regime based on self-compression in a kagome fibre.

Over the past decade intense laser fields with a single-cycle duration and even shorter, subcycle multicolour field transients have been generated and applied to drive attosecond phenomena in strong-field physics. Because of their extensive bandwidth, single-cycle fields cannot be emitted or amplified by laser sources directly and, as a rule, are produced by external pulse compression-a combination of nonlinear optical spectral broadening followed up by dispersion compensation. Here we demonstrate a simple robust driver for high-field applications based on this Kagome fibre approach that ensures pulse self-compression down to the ultimate single-cycle limit and provides phase-controlled pulses with up to a 100 μJ energy level, depending on the filling gas, pressure and the waveguide length.

A simple electron time-of-flight spectrometer for ultrafast vacuum ultraviolet photoelectron spectroscopy of liquid solutions.

We present a simple electron time of flight spectrometer for time resolved photoelectron spectroscopy of liquid samples using a vacuum ultraviolet (VUV) source produced by high-harmonic generation. The field free spectrometer coupled with the time-preserving monochromator for the VUV at the Artemis facility of the Rutherford Appleton Laboratory achieves an energy resolution of 0.65 eV at 40 eV with a sub 100 fs temporal resolution.