Spatio-temporal coupling of attosecond pulses

The shortest light pulses produced to date are of the order of a few tens of attoseconds, with central frequencies in the extreme ultraviolet range and bandwidths exceeding tens of eV. They are often produced as a train of pulses separated by half the driving laser period, leading in the frequency domain to a spectrum of high, odd-order harmonics. As light pulses become shorter and more spectrally wide, the widely-used approximation consisting in writing the optical waveform as a product of temporal and spatial amplitudes does not apply anymore. Here, we investigate the interplay of temporal and spatial properties of attosecond pulses. We show that the divergence and focus position of the generated harmonics often strongly depend on their frequency, leading to strong chromatic aberrations of the broadband attosecond pulses. Our argumentation uses a simple analytical model based on Gaussian optics, numerical propagation calculations and experimental harmonic divergence measurements. This effect needs to be considered for future applications requiring high quality focusing while retaining the broadband/ultrashort characteristics of the radiation

A versatile velocity map ion-electron covariance imaging spectrometer for high-intensity XUV experiments

We report on the design and performance of a velocity map imaging (VMI) spectrometer optimized for experiments using high-intensity extreme ultraviolet (XUV) sources such as laser-driven high-order harmonic generation (HHG) sources and free-electron lasers (FELs). Typically exhibiting low repetition rates and high single-shot count rates, such experiments do not easily lend themselves to coincident detection of photo-electrons and -ions. In order to obtain molecular frame or reaction channel-specific information, one has to rely on other correlation techniques, such as covariant detection schemes. Our device allows for combining different photo-electron and -ion detection modes for covariance analysis. We present the expected performance in the different detection modes and present the first results using an intense high-order harmonic generation (HHG) source

Two-Photon Double Ionization of Neon Studied with Intense Attosecond Pulse Trains

We focused an intense attosecond pulse train into a neon gas target and observed Ne2+ resulting from two-photon double ionization. By modifying the photon spectrum we find that the process is dominated by the sequential ionization via the Ne+ ion

Single-shot extreme-ultraviolet wavefront measurements of high-order harmonics

We perform wavefront measurements of high-order harmonics using an extreme-ultraviolet (XUV) Hartmann sensor and study how their spatial properties vary with different generation parameters, such as pressure in the nonlinear medium, fundamental pulse energy and duration as well as beam size. In some conditions, excellent wavefront quality (up to λ/11) was obtained. The high throughput of the intense XUV beamline at the Lund Laser Centre allows us to perform single-shot measurements of both the full harmonic beam generated in argon and individual harmonics selected by multilayer mirrors. We theoretically analyze the relationship between the spatial properties of the fundamental and those of the generated high-order harmonics, thus gaining insight into the fundamental mechanisms involved in high-order harmonic generation (HHG). © 2019 Optical Society of America

Dissociation dynamics of the diamondoid adamantane upon photoionization by XUV femtosecond pulses

International audienceAbstract This work presents a photodissociation study of the diamondoid adamantane using extreme ultraviolet femtosecond pulses. The fragmentation dynamics of the dication is unraveled by the use of advanced ion and electron spectroscopy giving access to the dissociation channels as well as their energetics. To get insight into the fragmentation dynamics, we use a theoretical approach combining potential energy surface determination, statistical fragmentation methods and molecular dynamics simulations. We demonstrate that the dissociation dynamics of adamantane dications takes place in a two-step process: barrierless cage opening followed by Coulomb repulsion-driven fragmentation

Simultaneous remote monitoring of atmospheric methane and water vapor using an integrated path DIAL instrument based on a widely tunable optical parametric source

International audienceWe report on the remote sensing capability of an integrated path differential absorption lidar (IPDIAL) instrument, for multi-species gas detection and monitoring in the 3.3-3.7 µm range. This instrument is based on an optical parametric source composed of a master oscillator-power amplifier scheme--whose core building block is a nested cavity optical parametric oscillator--emitting up to 10 µJ at 3.3 µm. Optical pumping is realized with an innovative single-frequency, 2-kHz repetition rate, nanosecond microchip laser, amplified up to 200 µJ per pulse in a single-crystal fiber amplifier. Simultaneous monitoring of mean atmospheric water vapor and methane concentrations was performed over several days by use of a topographic target, and water vapor concentration measurements show good agreement compared with an in situ hygrometer measurement. Performances of the IPDIAL instrument are assessed in terms of concentration measurement uncertainties and maximum remote achievable range

3.3 - 3.7µm OPO/OPA optical source for multi-species 200m range Integrated Path DIfferential Absorption Lidar

International audienceWe report on an integrated path Differential Absorption Lidar instrument based on a 3.3 - 3.7 µm range transmitter for multi-species atmospheric gas detection and quantification. Detection demonstration for atmospheric methane and water vapor is realized

Low-temperature nanoscale heat transport in a gadolinium iron garnet heterostructure probed by ultrafast x-ray diffraction

Time-resolved x-ray diffraction has been used to measure the low-temperature thermal transport properties of a Pt/Gd3Fe5O12//Gd3Ga5O12 metal/oxide heterostructure relevant to applications in spin caloritronics. A pulsed femtosecond optical signal produces a rapid temperature rise in the Pt layer, followed by heat transport into the Gd3Fe5O12 (GdIG) thin film and the Gd3Ga5O12 (GGG) substrate. The time dependence of x-ray diffraction from the GdIG layer was tracked using an accelerator-based femtosecond x-ray source. The ultrafast diffraction measurements probed the intensity of the GdIG (1 -1 2) x-ray reflection in a grazing-incidence x-ray diffraction geometry. The comparison of the variation of the diffracted x-ray intensity with a model including heat transport and the temperature dependence of the GdIG lattice parameter allows the thermal conductance of the Pt/GdIG and GdIG//GGG interfaces to be determined. Complementary synchrotron x-ray diffraction studies of the low-temperature thermal expansion properties of the GdIG layer provide a precise calibration of the temperature dependence of the GdIG lattice parameter. The interfacial thermal conductance of the Pt/GdIG and GdIG//GGG interfaces determined from the time-resolved diffraction study is of the same order of magnitude as previous reports for metal/oxide and epitaxial dielectric interfaces. The thermal parameters of the Pt/GdIG//GGG heterostructure will aid in the design and implementation of thermal transport devices and nanostructures

Micro-Focusing of Broadband High-Order Harmonic Radiation by a Double Toroidal Mirror

We present an optical system based on two toroidal mirrors in a Wolter configuration to focus broadband extreme ultraviolet (XUV) radiation. Optimization of the focusing optics alignment is carried out with the aid of an XUV wavefront sensor. Back-propagation of the optimized wavefront to the focus yields a focal spot of 3.6 × 4.0 µm2 full width at half maximum, which is consistent with ray-tracing simulations that predict a minimum size of 3.0 × 3.2 µm2. This work is important for optimizing the intensity of focused high-order harmonics in order to reach the nonlinear interaction regime