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تسجيل مستخدم جديدExtreme-ultraviolet pump-probe studies of one femtosecond scale electron dynamics
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Studies of ultrafast dynamics along with femtosecond-pulse metrology rely on non-linear processes, induced solely by the exciting/probing pulses or the pulses to be characterized. Extension of these approaches to the extreme-ultraviolet (XUV) spectral region opens up a new, direct route to attosecond scale dynamics. Limitations in available intensities of coherent XUV continua kept this prospect barren. The present work overcomes this barrier. Reaching condition at which simultaneous ejection of two bound electrons by two-XUV-photon absorption becomes more efficient than their one-by-one removal it is succeeded to probe atomic coherences, evolving at the 1fs scale, and determine the XUV-pulse duration. The investigated rich and dense in structure autoionizing manifold ascertains applicability of the approach to complex systems. This initiates the era of XUV-pump-XUV-probe experiments with attosecond resolution.
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Coherent light pulses of few to hundreds of femtoseconds (fs) duration have prolifically served the field of ultrafast phenomena. While fs pulses address mainly dynamics of nuclear motion in molecules or lattices in the gas, liquid or condensed matte
r phase, the advent of attosecond pulses has in recent years provided direct experimental access to ultrafast electron dynamics. However, there are processes involving nuclear motion in molecules and in particular coupled electronic and nuclear motion that possess few fs or even sub-fs dynamics. In the present work we have succeeded in addressing simultaneously vibrational and electronic dynamics in molecular Hydrogen. Utilizing a broadband extreme-ultraviolet (XUV) continuum the entire, Frank-Condon allowed spectrum of H2 is coherently excited. Vibrational, electronic and ionization 1fs scale dynamics are subsequently tracked by means of XUV-pump-XUV-probe measurements. These reflect the intrinsic molecular behavior as the XUV probe pulse hardly distorts the molecular potential.
Ultrafast dynamical processes in photoexcited molecules can be observed with pump-probe measurements, in which information about the dynamics is obtained from the transient signal associated with the excited state. Background signals provoked by pump
and/or probe pulses alone often obscure these excited state signals. Simple subtraction of pump-only and/or probe-only measurements from the pump-probe measurement, as commonly applied, results in a degradation of the signal-to-noise ratio and, in the case of coincidence detection, the danger of overrated background subtraction. Coincidence measurements additionally suffer from false coincidences. Here we present a probabilistic approach based on Bayesian probability theory that overcomes these problems. For a pump-probe experiment with photoelectron-photoion coincidence detection we reconstruct the interesting excited-state spectrum from pump-probe and pump-only measurements. This approach allows to treat background and false coincidences consistently and on the same footing. We demonstrate that the Bayesian formalism has the following advantages over simple signal subtraction: (i) the signal-to-noise ratio is significantly increased, (ii) the pump-only contribution is not overestimated, (iii) false coincidences are excluded, (iv) prior knowledge, such as positivity, is consistently incorporated, (v) confidence intervals are provided for the reconstructed spectrum, and (vi) it is applicable to any experimental situation and noise statistics. Most importantly, by accounting for false coincidences, the Bayesian approach allows to run experiments at higher ionization rates, resulting in a significant reduction of data acquisition times. The application to pump-probe coincidence measurements on acetone molecules enables novel quantitative interpretations about the molecular decay dynamics and fragmentation behavior.
The capability of generating two intense, femtosecond x-ray pulses with controlled time delay opens the possibility of performing time-resolved experiments for x-ray induced phenomena. We have applied this capability to study the photoinduced dynamic
s in diatomic molecules. In molecules composed of low-Z elements, textit{K}-shell ionization creates a core-hole state in which the main decay mode is an Auger process involving two electrons in the valence shell. After Auger decay, the nuclear wavepackets of the transient two-valence-hole states continue evolving on the femtosecond timescale, leading either to separated atomic ions or long-lived quasi-bound states. By using an x-ray pump and an x-ray probe pulse tuned above the textit{K}-shell ionization threshold of the nitrogen molecule, we are able to observe ion dissociation in progress by measuring the time-dependent kinetic energy releases of different breakup channels. We simulated the measurements on N$_2$ with a molecular dynamics model that accounts for textit{K}-shell ionization, Auger decay, and the time evolution of the nuclear wavepackets. In addition to explaining the time-dependent feature in the measured kinetic energy release distributions from the dissociative states, the simulation also reveals the contributions of quasi-bound states.
This paper employs Bayesian probability theory for analyzing data generated in femtosecond pump-probe photoelectron-photoion coincidence (PEPICO) experiments. These experiments allow investigating ultrafast dynamical processes in photoexcited molecul
es. Bayesian probability theory is consistently applied to data analysis problems occurring in these types of experiments such as background subtraction and false coincidences. We previously demonstrated that the Bayesian formalism has many advantages, amongst which are compensation of false coincidences, no overestimation of pump-only contributions, significantly increased signal-to-noise ratio, and applicability to any experimental situation and noise statistics. Most importantly, by accounting for false coincidences, our approach allows running experiments at higher ionization rates, resulting in an appreciable reduction of data acquisition times. In addition to our previous paper, we include fluctuating laser intensities, of which the straightforward implementation highlights yet another advantage of the Bayesian formalism. Our method is thoroughly scrutinized by challenging mock data, where we find a minor impact of laser fluctuations on false coincidences, yet a noteworthy influence on background subtraction. We apply our algorithm to data obtained in experiments and discuss the impact of laser fluctuations on the data analysis.
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