Matteo Lucchini

Energy-dependent photoemission delays from noble metal surfaces by attosecond interferometry

How quanta of energy and charge are transported on both atomic spatial and ultrafast timescales is at the heart of modern technology. Recent progress in ultrafast spectroscopy has allowed us to directly study the dynamical response of an electronic system to interaction with an electromagnetic field. Here, we present energy-dependent photoemission delays from the noble metal surfaces Ag(111) and Au(111). An interferometric technique based on attosecond pulse trains is applied simultaneously in a gas phase and a solid-state target to derive surface-specific photoemission delays. Experimental delays on the order of 100 as are in the same time range as those obtained from simulations. The strong variation of measured delays with excitation energy in Ag(111), which cannot be consistently explained invoking solely electron transport or initial state localization as supposed in previous work, indicates that final state effects play a key role in photoemission from solids.

Time-delay compensated monochromator for the spectral selection of extreme-ultraviolet high-order laser harmonics.

The design and the characterization of a monochromator for the spectral selection of ultrashort high-order laser harmonics in the extreme ultraviolet are presented. The instrument adopts the double-grating configuration to preserve the length of the optical paths of different diffracted rays, without altering the extremely short duration of the pulse. The gratings are used in the off-plane mount to have high efficiency. The performances of the monochromator have been characterized in terms of spectral response, efficiency, photon flux, imaging properties, and temporal response. In particular, the temporal characterization of the harmonic pulses has been obtained using a cross-correlation method: Pulses as short as 8 fs have been measured at the output of the monochromators, confirming the effectiveness of the time-delay compensated configuration.

Attosecond dynamical Franz-Keldysh effect in polycrystalline diamond

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 lights 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 Attosecond spectroscopy probes shifts in the electronic state structure of diamond induced by an intense infrared field. Short, intense laser pulses can be used to access the transition regime between classical and quantum optical responses in dielectrics. In this regime, the relative roles of inter- and intraband light-driven electronic transitions remain uncertain. We applied attosecond transient absorption spectroscopy to investigate the interaction between polycrystalline diamond and a few-femtosecond infrared pulse with intensity below the critical intensity of optical breakdown. Ab initio time-dependent density functional theory calculations, in tandem with a two-band parabolic model, accounted for the experimental results in the framework of the dynamical Franz-Keldysh effect and identified infrared induction of intraband currents as the main physical mechanism responsible for the observations.

Resonance Effects in Photoemission Time Delays

We present measurements of single-photon ionization time delays between the outermost valence electrons of argon and neon using a coincidence detection technique that allows for the simultaneous measurement of both species under identical conditions. The analysis of the measured traces reveals energy-dependent time delays of a few tens of attoseconds with high energy resolution. In contrast to photoelectrons ejected through tunneling, single-photon ionization can be well described in the framework of Wigner time delays. Accordingly, the overall trend of our data is reproduced by recent Wigner time delay calculations. However, besides the general trend we observe resonance features occurring at specific photon energies. These features have been qualitatively reproduced and identified by a calculation using the multiconfigurational Hartree-Fock method, including the influence of doubly excited states and ionization thresholds.

Versatile attosecond beamline in a two-foci configuration for simultaneous time-resolved measurements

We present our attoline which is a versatile attosecond beamline at the Ultrafast Laser Physics Group at ETH Zurich for attosecond spectroscopy in a variety of targets. High-harmonic generation (HHG) in noble gases with an infrared (IR) driving field is employed to generate pulses in the extreme ultraviolet (XUV) spectral regime for XUV-IR cross-correlation measurements. The IR pulse driving the HHG and the pulse involved in the measurements are used in a non-collinear set-up that gives independent access to the different beams. Single attosecond pulses are generated with the polarization gating technique and temporally characterized with attosecond streaking. This attoline contains two target chambers that can be operated simultaneously. A toroidal mirror relay-images the focus from the first chamber into the second one. In the first interaction region a dedicated double-target allows for a simple change between photoelectron/photoion measurements with a time-of-flight spectrometer and transient absorption experiments. Any end station can occupy the second interaction chamber. A surface analysis chamber containing a hemispherical electron analyzer was employed to demonstrate successful operation. Simultaneous RABBITT measurements in two argon jets were recorded for this purpose.

Combining attosecond XUV pulses with coincidence spectroscopy

Here we present a successful combination of an attosecond beamline with a COLTRIMS apparatus, which we refer to as AttoCOLTRIMS. The setup provides either single attosecond pulses or attosecond pulse trains for extreme ultraviolet-infrared pump-probe experiments. We achieve full attosecond stability by using an active interferometer stabilization. The capability of the setup is demonstrated by means of two measurements, which lie at the heart of the COLTRIMS detector: firstly, we resolve the rotating electric field vector of an elliptically polarized few-cycle infrared laser field by attosecond streaking exploiting the access to the 3D momentum space of the charged particles. Secondly, we show streaking measurements on different atomic species obtained simultaneously in a single measurement making use of the advantage of measuring ions and electrons in coincidence. Both of these studies demonstrate the potential of the AttoCOLTRIMS for attosecond science.

Charge migration and charge transfer in molecular systems

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.

Light-Matter Interaction at Surfaces in the Spatiotemporal Limit of Macroscopic Models.

What is the spatiotemporal limit of a macroscopic model that describes the optoelectronic interaction at the interface between different media? This fundamental question has become relevant for time-dependent photoemission from solid surfaces using probes that resolve attosecond electron dynamics on an atomic length scale. We address this fundamental question by investigating how ultrafast electron screening affects the infrared field distribution for a noble metal such as Cu(111) at the solid-vacuum interface. Attosecond photoemission delay measurements performed at different angles of incidence of the light allow us to study the detailed spatiotemporal dependence of the electromagnetic field distribution. Surprisingly, comparison with Monte Carlo semiclassical calculations reveals that the macroscopic Fresnel equations still properly describe the observed phase of the IR field on the Cu(111) surface on an atomic length and an attosecond time scale.

Resolving intra-atomic electron dynamics with attosecond transient absorption spectroscopy

Attosecond transient absorption spectroscopy is a recent addition to the experimental tool set of attosecond science. This all-optical method measures different observables than the previously existing techniques based on electron and ion detection and overcomes several of their limitations. We review the present state-of-the-art of attosecond transient absorption experiments and theory. Applications cover the exploration of ultrafast electron dynamics in atoms as well as in solid-state systems. As an example we discuss the observation of transiently bound electron wavepacket dynamics in helium in more detail. This example illustrates how transient absorption spectroscopy can provide information that is fundamentally inaccessible to the techniques based on ionisation, namely dynamics occurring well below the ionisation threshold. Furthermore, we show that a model based on wavepacket interference and originally developed to explain modulations in the ion yield is not sufficient to explain the observed optical response of the system. The optical response on extremely short timescales and in systems exposed to strong laser fields is still not fully understood. This makes the method also attractive for fundamental studies. Furthermore, it is expected that the technique will also find future applications for studying molecular systems in gas phase, in solution, or as solids and will greatly benefit from the advances of ultrafast lasers with multi-100-W average power improving signal-to-noise ratio by many orders of magnitude in the near future.

Comparison of attosecond streaking and RABBITT

Recent progress in the generation of ultra-short laser pulses has enabled the measurement of photoionization time delays with attosecond precision. For single photoemission time delays the most common techniques are based on attosecond streaking and the reconstruction of attosecond beating by interference of two-photon transitions (RABBITT). These are pump-probe techniques employing an extreme-ultraviolet (XUV) single attosecond pump pulse for streaking or an attosecond pump pulse train for RABBITT, and a phase-locked infrared (IR) probe pulse. These techniques can only extract relative timing information between electrons originating from different initial states within the same atom or different atoms. Here we address the question whether the two techniques give identical timing information. We present a complete study, supported by both experiments and simulations, comparing these two techniques for the measurement of the photoemission time delay difference between valence electrons emitted from the Ne 2p and Ar 3p ground states. We highlight not only the differences and similarities between the two techniques, but also critically investigate the reliability of the methods used to extract the timing information.