Photoemission from atoms is assumed to occur instantly in response to incident radiation and provides the basis for setting the zero of time in clocking atomic-scale electron motion. We used attosecond metrology to reveal a delay of 21 +/- 5 attoseconds in the emission of electrons liberated from the 2p orbitals of neon atoms with respect to those released from the 2s orbital by the same 100-electron volt light pulse. Small differences in the timing of photoemission from different quantum states provide a probe for modeling many-electron dynamics. Theoretical models refined with the help of attosecond timing metrology may provide insight into electron correlations and allow the setting of the zero of time in atomic-scale chronoscopy with a precision of a few attoseconds.

Comprehensive knowledge of the dynamic behaviour of electrons in condensed-matter systems is pertinent to the development of many modern technologies, such as semiconductor and molecular electronics, optoelectronics, information processing and photovoltaics. Yet it remains challenging to probe electronic processes, many of which take place in the attosecond (1 as = 10(-18) s) regime. In contrast, atomic motion occurs on the femtosecond (1 fs = 10(-15) s) timescale and has been mapped in solids in real time using femtosecond X-ray sources. Here we extend the attosecond techniques previously used to study isolated atoms in the gas phase to observe electron motion in condensed-matter systems and on surfaces in real time. We demonstrate our ability to obtain direct time-domain access to charge dynamics with attosecond resolution by probing photoelectron emission from single-crystal tungsten. Our data reveal a delay of approximately 100 attoseconds between the emission of photoelectrons that originate from localized core states of the metal, and those that are freed from delocalized conduction-band states. These results illustrate that attosecond metrology constitutes a powerful tool for exploring not only gas-phase systems, but also fundamental electronic processes occurring on the attosecond timescale in condensed-matter systems and on surfaces.

Intense femtosecond laser excitation can produce transient states of matter that would otherwise be inaccessible to laboratory investigation. At high excitation densities, the interatomic forces that bind solids and determine many of their properties can be substantially altered. Here, we present the detailed mapping of the carrier density–dependent interatomic potential of bismuth approaching a solid-solid phase transition. Our experiments combine stroboscopic techniques that use a high-brightness linear electron accelerator–based x-ray source with pulse-by-pulse timing reconstruction for femtosecond resolution, allowing quantitative characterization of the interatomic potential energy surface of the highly excited solid.

Electrons emit light, carry electric current, and bind atoms together to form molecules. Insight into and control of their atomic-scale motion are the key to understanding the functioning of biological systems, developing efficient sources of x-ray light, and speeding up electronics. Capturing and steering this electron motion require attosecond resolution and control, respectively (1 attosecond = 10(-18) seconds). A recent revolution in technology has afforded these capabilities: Controlled light waves can steer electrons inside and around atoms, marking the birth of lightwave electronics. Isolated attosecond pulses, well reproduced and fully characterized, demonstrate the power of the new technology. Controlled few-cycle light waves and synchronized attosecond pulses constitute its key tools. We review the current state of lightwave electronics and highlight some future directions.

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The ability to fully characterize ultrashort, ultra-intense X-ray pulses at free-electron lasers (FELs) will be crucial in experiments ranging from single-molecule imaging to extreme-timescale X-ray science. This issue is especially important at current-generation FELs, which are primarily based on self-amplified spontaneous emission and radiate with parameters that fluctuate strongly from pulse to pulse. Using single-cycle terahertz pulses from an optical laser, we have extended the streaking techniques of attosecond metrology to measure the temporal profile of individual FEL pulses with 5 fs full-width at half-maximum accuracy, as well as their arrival on a time base synchronized to the external laser to within 6 fs r.m.s. Optical laser-driven terahertz streaking can be utilized at any X-ray photon energy and is non-invasive, allowing it to be incorporated into any pump–probe experiment, eventually characterizing pulses before and after interaction with most sample environments

We use time- and angle-resolved photoemission spectroscopy with sub-30-fs extreme-ultraviolet pulses to map the time- and momentum-dependent electronic structure of photoexcited 1T-TaS(2). This compound is a two-dimensional Mott insulator with charge-density wave ordering. Charge order, evidenced by splitting between occupied subbands at the Brillouin zone boundary, melts well before the lattice responds. This challenges the view of a charge-density wave caused by electron-phonon coupling and Fermi-surface nesting alone, and suggests that electronic correlations play a key role in driving charge order.

We report on laser-assisted attosecond photoemission from single-crystalline magnesium. In strong contrast to the previously investigated transition metal tungsten, photoelectron wave packets originating from the localized core level and delocalized valence-band states are launched simultaneously from the solid within the experimental uncertainty of 20 as. This phenomenon is shown to be compatible with a heuristic model based on free-particle-like propagation of the electron wave packets generated inside the crystal by the attosecond excitation pulse and their subsequent interaction with the assisting laser field at the metal-vacuum interface.