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Dissociation of the ethylene cation is a prototypical multistep pathway in which the exact mechanisms leading to internal energy conversions are not fully known. For example, it is still unclear how the energy is exactly redistributed among the internal modes and which step is rate-determining. Here we use few-femtosecond extreme-ultraviolet pulses of tunable energy to excite a different superposition of the four lowest states of C 2 H 4 + and probe the subsequent fast relaxation with a short infrared pulse. Our results demonstrate that the infrared pulse photoexcites the cationic ground state (GS) to higher excited states, producing a hot GS upon relaxation, which enhances the fragmentation yield. As the photoexcitation probability of the GS strongly depends on the molecular geometry, the probing by the IR pulse provides information about the ultrafast excited-state dynamics and the type of conical intersection (planar or twisted) involved in the first 20 fs of the nonradiative relaxation.

The electro-optical properties of most semiconductors and insulators of technological interest are dominated by the presence of electron-hole quasi-particles, called excitons. The manipulation of excitons in dielectrics has recently received great attention, with possible applications in different fields including optoelectronics and photonics. Here, we apply attosecond transient reflection spectroscopy in a sequential two-foci geometry and observe sub-femtosecond dynamics of a core-level exciton in bulk MgF 2 single crystals. Furthermore, we access absolute phase delays, which allow for an unambiguous comparison with theoretical calculations. Our results show that excitons surprisingly exhibit a dual atomic- and solid-like character, which manifests itself on different time scales. While the former is responsible for a femtosecond optical Stark effect, the latter dominates the attosecond excitonic response. Further theoretical investigation reveals a link with the exciton sub-femtosecond nanometric motion and allows us to envision a new route to control exciton dynamics in the close-to-petahertz regime.

We present an innovative beamline for extreme ultraviolet (XUV)-infrared (IR) pump-probe reflection spectroscopy in solids with attosecond temporal resolution. The setup uses an actively stabilized interferometer, where attosecond pulse trains or isolated attosecond pulses are produced by high-order harmonic generation in gases. After collinear recombination, the attosecond XUV pulses and the femtosecond IR pulses are focused twice in sequence by toroidal mirrors, giving two spatially separated interaction regions. In the first region, the combination of a gas target with a time-of-flight spectrometer allows for attosecond photoelectron spectroscopy experiments. In the second focal region, an XUV reflectometer is used for attosecond transient reflection spectroscopy (ATRS) experiments. Since the two measurements can be performed simultaneously, precise pump-probe delay calibration can be achieved, thus opening the possibility for a new class of attosecond experiments on solids. Successful operation of the beamline is demonstrated by the generation and characterization of isolated attosecond pulses, the measurement of the absolute reflectivity of SiO 2 , and by performing simultaneous photoemission/ATRS in Ge.

Frequency-resolved optical gating for the complete reconstruction of attosecond bursts (FROG-CRAB) is a well-known technique for the complete temporal characterization of ultrashort extreme ultraviolet (XUV) pulses, with durations down to a few tens of attoseconds. Recently, this technique was extended to few-femtosecond XUV pulses, produced by high-order harmonic generation (HHG) in gases, thanks to the implementation of a robust iterative algorithm: the extended ptychographic iterative engine (ePIE). We demonstrate, by using numerical simulations, that the ptychographic reconstruction technique is characterized by an excellent degree of convergence and robustness. We analyse the effects on pulse reconstruction of various experimental imperfections, namely, the jitter of the relative temporal delay between the XUV pulse and a suitably delayed infrared (IR) pulse and the noise of the measured FROG-CRAB spectrograms. We also show that the ePIE approach is particularly suitable for the reconstruction of incomplete FROG-CRAB spectrograms (i.e., spectrograms with a reduced number of measured time delays) and of spectrograms acquired with a reduced spectral resolution, particularly when relatively high-intensity IR pulses are employed.

Sub-10-fs pulses tunable in the extreme-ultraviolet (XUV) spectral region are particularly important in many research fields: from atomic and molecular spectroscopy to the study of relaxation processes in solids and transition phase processes, from holography to free-electron laser injection. A crucial prerequisite for all applications is the accurate measurement of the temporal characteristics of these pulses. To fulfill this purpose, many phase retrieval algorithms have been successfully applied to reconstruct XUV attosecond pulses. Nevertheless, their extension to XUV femtosecond pulses is not trivial and has never been investigated/reported so far. We demonstrate that ultrashort XUV pulses, produced by high-order harmonic generation, spectrally filtered by a time-delay compensated monochromator, can be fully characterized, in terms of temporal intensity and phase, by employing the ptychographic reconstruction technique while other common reconstruction algorithms fail. This allows us to report on the generation and complete temporal characterization of XUV pulses with duration down to 5 fs, which constitute the shortest XUV pulse ever achieved via a time-delay compensated monochromator.