Shining a fast light on diamonds: Conceptually, the electronic structure of matter is a fixed scaffold of energy levels, which electrons climb with the help of light absorption. In reality, the light's electromagnetic field distorts the scaffold, a phenomenon that becomes increasingly evident with rising field intensity. Lucchini et al. studied a manifestation of this phenomenon, termed the dynamical Franz Keldysh effect, in diamond substrates exposed to sudden, moderately intense infrared fields. Using attosecond probe pulses and accompanying theoretical simulations, they resolved and accounted for the extremely rapid ensuing electron dynamics. Science , this issue p. 916
The transfer of charge at the molecular level plays a fundamental role in many areas of chemistry, physics, biology and materials science. Today, more than 60 years after the seminal work of R. A. Marcus, charge transfer is still a very active field of research. An important recent impetus comes from the ability to resolve ever faster temporal events, down to the attosecond time scale. Such a high temporal resolution now offers the possibility to unravel the most elementary quantum dynamics of both electrons and nuclei that participate in the complex process of charge transfer. This review covers recent research that addresses the following questions. Can we reconstruct the migration of charge across a molecule on the atomic length and electronic time scales? Can we use strong laser fields to control charge migration? Can we temporally resolve and understand intramolecular charge transfer in dissociative ionization of small molecules, in transition-metal complexes and in conjugated polymers? Can we tailor molecular systems towards specific charge-transfer processes? What are the time scales of the elementary steps of charge transfer in liquids and nanoparticles? Important new insights into each of these topics, obtained from state-of-the-art ultrafast spectroscopy and/or theoretical methods, are summarized in this review.
Time and place of electron exit: Until about a decade ago, laser-induced ionization was considered instantaneous. Since then, applications of attosecond laser pulses have shown multiple subtle and complex factors that influence the precise timing of electron ejection from atoms and surfaces. Vos et al. measured the corresponding attosecond dynamics of dissociative photoionization in a diatomic molecule, carbon monoxide. By imaging the charged fragments, the timing could be correlated with the specific spatial portion of the molecule from which the electron wave packet emerged. Science , this issue p. 1326
Electron correlation and multielectron effects are fundamental interactions that govern many physical and chemical processes in atomic, molecular and solid state systems. The process of autoionization, induced by resonant excitation of electrons into discrete states present in the spectral continuum of atomic and molecular targets, is mediated by electron correlation. Here we investigate the attosecond photoemission dynamics in argon in the 20–40 eV spectral range, in the vicinity of the 3s−1np autoionizing resonances. We present measurements of the differential photoionization cross section and extract energy and angle-dependent atomic time delays with an attosecond interferometric method. With the support of a theoretical model, we are able to attribute a large part of the measured time delay anisotropy to the presence of autoionizing resonances, which not only distort the phase of the emitted photoelectron wave packet but also introduce an angular dependence.