Time-Resolved Multielectron Coincidence Spectroscopy of Double Auger-Meitner Decay Following Xe 4d Ionization.

We introduce time-resolved multielectron coincidence spectroscopy and apply it to the double Auger-Meitner (AM) emission process following xenon 4d photoionization. The photoelectron and AM electron(s) are measured in coincidence by using a magnetic-bottle time-of-flight spectrometer, enabling an unambiguous assignment of the complete cascade pathways involving two AM electron emissions. In the presence of a near-infrared (NIR) laser pulse, the intermediate Xe^{2+*} state embedded in the Xe^{3+} continuum is probed through single NIR photon absorption and the lifetime of this intermediate Xe^{2+*} state is directly obtained as (109±22) fs.

High-harmonic generation in liquids with few-cycle pulses: effect of laser-pulse duration on the cut-off energy.

High-harmonic generation (HHG) in liquids is opening new opportunities for attosecond light sources and attosecond time-resolved studies of dynamics in the liquid phase. In gas-phase HHG, few-cycle pulses are routinely used to create isolated attosecond pulses and to extend the cut-off energy. Here, we study the properties of HHG in liquids, including heavy water, ethanol and isopropanol, by continuously tuning the pulse duration of a mid-infrared driver from the multi- to the two-cycle regime. Similar to the gas phase, we observe the transition from discrete odd-order harmonics to continuous extreme-ultraviolet emission. However, the cut-off energy is shown to be entirely independent of the pulse duration. These observations are confirmed by ab-initio simulations of HHG in large liquid clusters. Our results support the notion that the cut-off energy is a fundamental property of the liquid, independent of the driving-pulse properties. Our work implies that few-cycle mid-infrared laser pulses are suitable drivers for generating isolated attosecond pulses from liquids and confirm the capability of high-harmonic spectroscopy to determine the mean-free paths of slow electrons in liquids.

Femtosecond proton transfer in urea solutions probed by X-ray spectroscopy.

Proton transfer is one of the most fundamental events in aqueous-phase chemistry and an emblematic case of coupled ultrafast electronic and structural dynamics1,2. Disentangling electronic and nuclear dynamics on the femtosecond timescales remains a formidable challenge, especially in the liquid phase, the natural environment of biochemical processes. Here we exploit the unique features of table-top water-window X-ray absorption spectroscopy3-6 to reveal femtosecond proton-transfer dynamics in ionized urea dimers in aqueous solution. Harnessing the element specificity and the site selectivity of X-ray absorption spectroscopy with the aid of ab initio quantum-mechanical and molecular-mechanics calculations, we show how, in addition to the proton transfer, the subsequent rearrangement of the urea dimer and the associated change of the electronic structure can be identified with site selectivity. These results establish the considerable potential of flat-jet, table-top X-ray absorption spectroscopy7,8 in elucidating solution-phase ultrafast dynamics in biomolecular systems.

Temperature measurements of liquid flat jets in vacuum.

Sub-µm thin samples are essential for spectroscopic purposes. The development of flat micro-jets enabled novel spectroscopic and scattering methods for investigating molecular systems in the liquid phase. However, the temperature of these ultra-thin liquid sheets in vacuum has not been systematically investigated. Here, we present a comprehensive temperature characterization using optical Raman spectroscopy of sub-micron flatjets produced by two different methods: colliding of two cylindrical jets and a cylindrical jet compressed by a high pressure gas. Our results reveal the dependence of the cooling rate on the material properties and the source characteristics, i.e., nozzle-orifice size, flow rate, and pressure. We show that materials with higher vapor pressures exhibit faster cooling rates, which is illustrated by comparing the temperature profiles of water and ethanol flatjets. In a sub-µm liquid sheet, the temperature of the water sample reaches around 268 K and the ethanol around 253 K close to the flatjet's terminus.

High-order harmonic source spanning up to the oxygen K-edge based on filamentation pulse compression.

We present a 0.2 TW sub-two-cycle 1.8 µm carrier-envelope-phase stable source based on two-stage pulse compression by filamentation for driving high-order harmonic generation extending beyond the oxygen K absorption edge. The 1 kHz repetition rate, high temporal resolution enabled by the short 11.8 fs driving pulse duration, and bright high-order harmonics generated in helium make this an attractive source for solid-state and molecular-dynamics studies.

Bismuth ferrite dielectric nanoparticles excited at telecom wavelengths as multicolor sources by second, third, and fourth harmonic generation.

We demonstrate the simultaneous generation of second, third, and fourth harmonics from a single dielectric bismuth ferrite nanoparticle excited using a telecom fiber laser at 1560 nm. We first characterize the signals associated with different nonlinear orders in terms of spectrum, excitation intensity dependence, and relative signal strengths. Successively, on the basis of the polarization-resolved emission curves of the three harmonics, we discuss the interplay of susceptibility tensor components at different orders and show how polarization can be used as an optical handle to control the relative frequency conversion properties.

Near- and Extended-Edge X-Ray-Absorption Fine-Structure Spectroscopy Using Ultrafast Coherent High-Order Harmonic Supercontinua.

Recent advances in high-order harmonic generation have made it possible to use a tabletop-scale setup to produce spatially and temporally coherent beams of light with bandwidth spanning 12 octaves, from the ultraviolet up to x-ray photon energies >1.6 keV. Here we demonstrate the use of this light for x-ray-absorption spectroscopy at the K- and L-absorption edges of solids at photon energies near 1 keV. We also report x-ray-absorption spectroscopy in the water window spectral region (284-543 eV) using a high flux high-order harmonic generation x-ray supercontinuum with 10^{9} photons/s in 1% bandwidth, 3 orders of magnitude larger than has previously been possible using tabletop sources. Since this x-ray radiation emerges as a single attosecond-to-femtosecond pulse with peak brightness exceeding 10^{26} photons/s/mrad^{2}/mm^{2}/1% bandwidth, these novel coherent x-ray sources are ideal for probing the fastest molecular and materials processes on femtosecond-to-attosecond time scales and picometer length scales.

High-energy pulse stacking via regenerative pulse-burst amplification.

Here we present a coherent pulse stacking approach for upscaling the energy of a solid-state femtosecond chirped pulse amplifier. We demonstrate pulse splitting into four replicas, amplification in a burst-mode regenerative Yb:CaF2 amplifier, designed to overcome intracavity optical damage by colliding pulse replicas, and coherent combining into a single millijoule level pulse. The thresholds of pulse-burst-induced damage of optical elements are experimentally investigated. The scheme allows achieving an enhancement factor of 2.62 using a single-stage stacker cavity and, potentially, much higher enhancement factors using cascaded stacking.

Direct carrier-envelope phase control of an amplified laser system.

Direct carrier-envelope phase stabilization of an Yb:KGW MOPA laser system is demonstrated with a residual phase jitter reduced to below 100 mrad, which compares favorably with previous stabilization reports, both of amplified laser systems as well as of ytterbium-based oscillators. This novel stabilization scheme relies on a frequency synthesis scheme and a feed-forward approach. The direct stabilization of a sub-MHz frequency comb from a CPA amplifier not only reduces the phase noise but also greatly simplifies the stabilization setup.

Ultrafast multi-wavelength switch based on dynamics of spectrally-shifted solitons in a dual­core photonic crystal fiber.

Nonlinear propagation of ultrafast near infrared pulses in anomalous dispersion region of dual-core photonic crystal fiber was studied. Polarization tunable soliton-based nonlinear switching at multiple non-excitation wavelengths was demonstrated experimentally for fiber excitation by 100 fs pulses at 1650 nm. The highest-contrast switching was obtained with the fiber length of just 14 mm, which is significantly shorter compared to the conventional non-solitonic in-fiber switching based on nonlinear optical loop mirror. Advanced numerical simulations show good agreement with the experimental results, suggesting that the underlying dual-core soliton fission process supports nonlinear optical switching and simultaneous pulse compression to few-cycle durations at the level of 20 fs.

Bright coherent ultrahigh harmonics in the keV x-ray regime from mid-infrared femtosecond lasers.

High-harmonic generation (HHG) traditionally combines ~100 near-infrared laser photons to generate bright, phase-matched, extreme ultraviolet beams when the emission from many atoms adds constructively. Here, we show that by guiding a mid-infrared femtosecond laser in a high-pressure gas, ultrahigh harmonics can be generated, up to orders greater than 5000, that emerge as a bright supercontinuum that spans the entire electromagnetic spectrum from the ultraviolet to more than 1.6 kilo-electron volts, allowing, in principle, the generation of pulses as short as 2.5 attoseconds. The multiatmosphere gas pressures required for bright, phase-matched emission also support laser beam self-confinement, further enhancing the x-ray yield. Finally, the x-ray beam exhibits high spatial coherence, even though at high gas density the recolliding electrons responsible for HHG encounter other atoms during the emission process.

Carrier envelope phase stabilization of a Yb:KGW laser amplifier.

In this paper we report on the active stabilization of the carrier envelope phase (CEP) of a Yb:KGW chirped pulse amplifier laser system seeded by a Yb-doped solid-state Kerr-lens mode-locked oscillator. The regenerative amplifier delivers 180 fs CEP stable pulses of 30 µJ-1 mJ energy at a repetition rate tunable from 1 to 200 kHz. The bandwidth of the feedback loop was extended by a factor of 5 using a specially designed high-pass filter, which resulted in a dramatic decrease of CEP jitter below 0.45 rad after the amplifier.

90 GW peak power few-cycle mid-infrared pulses from an optical parametric amplifier.

We demonstrate a compact 20 Hz repetition-rate mid-IR OPCPA system operating at a central wavelength of 3900 nm with the tail-to-tail spectrum extending over 600 nm and delivering 8 mJ pulses that are compressed to 83 fs (<7 optical cycles). Because of the long optical period (∼13 fs) and a high peak power, the system opens a range of unprecedented opportunities for tabletop ultrafast science and is particularly attractive as a driver for a highly efficient generation of ultrafast coherent x-ray continua for biomolecular and element specific imaging.

Time-resolved off-axis digital holography for characterization of ultrafast phenomena in water.

We present the application of time-resolved off-axis digital holography for the investigation of refractive index/transmission properties of laser-induced plasma filaments in water. Time evolution of both amplitude- and phase-contrast images of the self-focused beam in water was characterized with temporal resolution better than 50 fs. To the best of our knowledge, this is the first attempt to characterize the propagation of femtosecond laser pulse in nonlinear media using off-axis digital holography.