Abstract
Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. These experiments employ attosecond pulses or pulse trains and explore dynamical processes in a pump–probe scheme that is selectively sensitive to electronic state of matter via photoelectron or XUV absorption spectroscopy or that includes changes of the ionic state detected via photo-ion mass spectrometry. Here, we demonstrate how the implementation of combined photo-ion and absorption spectroscopy with attosecond resolution enables tracking the complex multidimensional excitation and decay cascade of an Auger auto-ionization process of a few femtoseconds in highly excited krypton. In tandem with theory, our study reveals the role of intermediate electronic states in the formation of multiply charged ions. Amplitude tuning of a dressing laser field addresses different groups of decay channels and allows exerting temporal and quantitative control over the ionization dynamics in rare gas atoms.
Highlights
Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids
Photoelectron detection techniques generally suffer from electron backgrounds produced by strong laser fields or secondary electrons that do not carry any information about the dynamics under inspection
Transient absorption spectroscopy (TAS) in contrast is not limited to phenomena liberating electrons and is the method of choice for investigating bound–bound transitions[19,20]
Summary
Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. Instead of measuring the yield of generated charge carriers, TAS measures the spectrally resolved absorption of an attosecond extreme ultraviolet (XUV) pulse in a medium that has been coherently excited by an XUV pulse or dressed by an intense, time-delayed near-infrared (NIR) few-cycle laser pulse.
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