99 research outputs found
Attosecond imaging
The natural timescale for electron dynamics reaches down to the attosecond
domain. Following the discovery of attosecond laser pulses, about a decade
ago, attosecond science has developed into a vibrant, new research field,
where the motion of single or multiple electrons and, in molecules, the
coupling of electronic and nuclear motion, can be investigated, on attosecond
to few-femtosecond timescales. Attosecond experiments require suitable
observables. This review describes how “attosecond imaging”, basing itself on
kinetic energy and angle-resolved detection of photoelectrons and fragment
ions using a velocity map imaging (VMI) spectrometer, has been exploited in a
number of pump–probe experiments. The use of a VMI spectrometer in attosecond
experiments has allowed the characterization of attosecond pulse trains and
isolated attosecond pulses, the elucidation of continuum electron dynamics and
wave packet interferometry in atomic photoionization and the observation of
electron localization in dissociative molecular photoionization
Spatio-temporal characterisation of a 100 kHz 24 W sub-3-cycle NOPCPA laser system
In recent years, OPCPA and NOPCPA laser systems have shown the potential to supersede Ti:sapphire plus post-compression based laser systems to drive next generation attosecond light sources via direct amplification of few-cycle pulses to high pulse energies at high repetition rates. In this paper, we present a sub 3-cycle, 100 kHz, 24 W NOPA laser system and characterise its spatio-temporal properties using the SEA-F-SPIDER technique. Our results underline the importance of spatio-temporal diagnostics for these emerging laser systems
Tracing transient charges in expanding clusters
We study transient charges formed in methane clusters following ionization by intense near-infrared laser pulses. Cluster ionization by 400-fs (I=1Ă—1014 W/cm2) pulses is highly efficient, resulting in the observation of a dominant C3+ ion contribution. The C4+ ion yield is very small but is strongly enhanced by applying a time-delayed weak near-infrared pulse. We conclude that most of the valence electrons are removed from their atoms during the laser-cluster interaction and that electrons from the nanoplasma recombine with ions and populate Rydberg states when the cluster expands, leading to a decrease of the average charge state of individual ions. Furthermore, we find clear bound-state signatures in the electron kinetic energy spectrum, which we attribute to Auger decay taking place in expanding clusters. Such nonradiative processes lead to an increase of the final average ion charge state that is measured in experiments. Our results suggest that it is crucial to include both recombination and nonradiative decay processes for the understanding of recorded ion charge spectra
Numerical study of spatiotemporal distortions in noncollinear optical parametric chirped-pulse amplifiers
During amplification in a noncollinear optical parametric amplifier the spatial and temporal coordinates of the amplified field are inherently coupled. These couplings or distortions can limit the peak intensity, among other things. In this work, a numerical study of the spatiotemporal distortions in BBO-based noncollinear optical parametric chirped-pulse amplifiers (NOPCPAs) is presented for a wide range of parameters and for different amplification conditions. It is shown that for Gaussian pump beams, gain saturation introduces strong distortions and high conversion efficiency always comes at the price of strong spatiotemporal couplings which drastically reduce the peak intensity even when pulse fronts of the pump and the signal are matched. However, high conversion efficiencies with minimum spatiotemporal distortions can still be achieved with flat-top pump beam profiles
Ionization avalanching in clusters ignited by extreme-ultraviolet driven seed electrons
We study the ionization dynamics of Ar clusters exposed to ultrashort
near-infrared (NIR) laser pulses for intensities well below the threshold at
which tunnel ionization ignites nanoplasma formation. We find that the emission
of highly charged ions up to Ar can be switched on with unit contrast by
generating only a few seed electrons with an ultrashort extreme ultraviolet
(XUV) pulse prior to the NIR field. Molecular dynamics simulations can explain
the experimental observations and predict a generic scenario where efficient
heating via inverse bremsstrahlung and NIR avalanching are followed by resonant
collective nanoplasma heating. The temporally and spatially well-controlled
injection of the XUV seed electrons opens new routes for controlling
avalanching and heating phenomena in nanostructures and solids, with
implications for both fundamental and applied laser-matter science.Comment: 5 pages, 4 figure
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Spatio-temporal characterisation of a 100 kHz 24 W sub-3-cycle NOPCPA laser system
In recent years, OPCPA and NOPCPA laser systems have shown the potential to supersede Ti:sapphire plus post-compression based laser systems to drive next generation attosecond light sources via direct amplification of few-cycle pulses to high pulse energies at high repetition rates. In this paper, we present a sub 3-cycle, 100 kHz, 24 W NOPA laser system and characterise its spatio-temporal properties using the SEA-F-SPIDER technique. Our results underline the importance of spatio-temporal diagnostics for these emerging laser systems
Interference stabilization of autoionizing states in molecular studied by time- and angular-resolved photoelectron spectroscopy
An autoionizing resonance in molecular N is excited by an ultrashort XUV
pulse and probed by a subsequent weak IR pulse, which ionizes the contributing
Rydberg states. Time- and angular-resolved photoelectron spectra recorded with
a velocity map imaging spectrometer reveal two electronic contributions with
different angular distributions. One of them has an exponential decay rate of
fs, while the other one is shorter than 10 fs. This observation is
interpreted as a manifestation of interference stabilization involving the two
overlapping discrete Rydberg states. A formalism of interference stabilization
for molecular ionization is developed and applied to describe the autoionizing
resonance. The results of calculations reveal, that the effect of the
interference stabilization is facilitated by rotationally-induced couplings of
electronic states with different symmetry.Comment: 8 pages, 6 figure
Sequential and direct ionic excitation in the strong-field ionization of 1-butene molecules
We study the Strong-Field Ionization (SFI) of the hydrocarbon 1-butene as a function of wavelength using photoion-photoelectron covariance and coincidence spectroscopy. We observe a striking transition in the fragment-associated photoelectron spectra: from a single Above Threshold Ionization (ATI) progression for photon energies less than the cation D0–D1 gap to two ATI progressions for a photon energy greater than this gap. For the first case, electronically excited cations are created by SFI populating the ground cationic state D0, followed by sequential post-ionization excitation. For the second case, direct sub-cycle SFI to the D1 excited cation state contributes significantly. Our experiments access ionization dynamics in a regime where strong-field and resonance-enhanced processes can interplay
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