Thorsten Uphues

Attosecond spectroscopy in condensed matter

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.

Attosecond real-time observation of electron tunnelling in atoms

Atoms exposed to intense light lose one or more electrons and become ions. In strong fields, the process is predicted to occur via tunnelling through the binding potential that is suppressed by the light field near the peaks of its oscillations. Here we report the real-time observation of this most elementary step in strong-field interactions: light-induced electron tunnelling. The process is found to deplete atomic bound states in sharp steps lasting several hundred attoseconds. This suggests a new technique, attosecond tunnelling, for probing short-lived, transient states of atoms or molecules with high temporal resolution. The utility of attosecond tunnelling is demonstrated by capturing multi-electron excitation (shake-up) and relaxation (cascaded Auger decay) processes with subfemtosecond resolution.

Attosecond Electron Spectroscopy Using a Novel Interferometric Pump-Probe Technique

We present an interferometric pump-probe technique for the characterization of attosecond electron wave packets (WPs) that uses a free WP as a reference to measure a bound WP. We demonstrate our method by exciting helium atoms using an attosecond pulse (AP) with a bandwidth centered near the ionization threshold, thus creating both a bound and a free WP simultaneously. After a variable delay, the bound WP is ionized by a few-cycle infrared laser precisely synchronized to the original AP. By measuring the delay-dependent photoelectron spectrum we obtain an interferogram that contains both quantum beats as well as multipath interference. Analysis of the interferogram allows us to determine the bound WP components with a spectral resolution much better than the inverse of the AP duration.

Imaging of carrier-envelope phase effects in above-threshold ionization with intense few-cycle laser fields

Sub-femtosecond control of the electron emission in above-threshold ionization of the rare gases Ar, Xe and Kr in intense few-cycle laser fields is reported with full angular resolution. Experimental data that were obtained with the velocity-map imaging technique are compared to simulations using the strong-field approximation (SFA) and full time-dependent Schrodinger equation (TDSE) calculations. We find a pronounced asymmetry in both the energy and angular distributions of the electron emission that critically depends on the carrier-envelope phase (CEP) of the laser field. The potential use of imaging techniques as a tool for single-shot detection of the CEP is discussed.

Design, fabrication, and analysis of chirped multilayer mirrors for reflection of extreme-ultraviolet attosecond pulses

Chirped Mo/Si multilayer coatings have been designed, fabricated, and characterized for use in extreme-ultraviolet attosecond experiments. By numerically simulating the reflection of the attosecond pulse from a multilayer mirror during the optimization procedure based on a genetic algorithm, we obtain optimized layer designs. We show that normal incidence chirped multilayer mirrors capable of reflecting pulses of approximately 100 attoseconds (as) duration can be designed by enhancing the reflectivity bandwidth and optimizing the phase-shift behavior. The chirped multilayer coatings have been fabricated by electron-beam evaporation in an ultrahigh vacuum in combination with ion-beam polishing of the interfaces and in situ reflectivity measurement for layer thickness control. To analyze the aperiodic layer structure by hard-x-ray reflectometry, we have developed an automatic fitting procedure that allows us to determine the individual layer thicknesses with an error of less than 0.05 nm. The fabricated chirped mirror may be used for production of 150-160 as pulses.

Ion-charge-state chronoscopy of cascaded atomic Auger decay

It has recently been demonstrated that apart from the electron detection realized in the attosecond streak camera, also ion detection can be used for establishing extreme-ultraviolet pump/visible probe experiments, temporally resolving the dynamics of atomic inner-shell relaxation processes. We utilize this method for studying the Auger decay of krypton atoms following the creation of vacancy states in the 3d shell. It is shown that the electronic relaxation occurs through different pathways, each involving cascades of sequential steps which are followed in their native temporal succession.

A flexible apparatus for attosecond photoelectron spectroscopy of solids and surfaces

We describe an apparatus for attosecond photoelectron spectroscopy of solids and surfaces, which combines the generation of isolated attosecond extreme-ultraviolet (XUV) laser pulses by high harmonic generation in gases with time-resolved photoelectron detection and surface science techniques in an ultrahigh vacuum environment. This versatile setup provides isolated attosecond pulses with photon energies of up to 140 eV and few-cycle near infrared pulses for studying ultrafast electron dynamics in a large variety of surfaces and interfaces. The samples can be prepared and characterized on an atomic scale in a dedicated flexible surface science end station. The extensive possibilities offered by this apparatus are demonstrated by applying attosecond XUV pulses with a central photon energy of ∼125 eV in an attosecond streaking experiment of a xenon multilayer grown on a Re(0001) substrate.

Attosecond imaging of XUV-induced atomic photoemission and Auger decay in strong laser fields

Velocity-map imaging has been employed to study the photoemission in Ne and N4,5OO Auger decay in Xe induced by an isolated 85 eV extreme ultraviolet (XUV) pulse in the presence of a strong few-cycle near-infrared (NIR) laser field. Full three-dimensional momentum information about the released electrons was obtained. The NIR and XUV pulse parameters were extracted from the measured Ne streaking traces using a FROG CRAB retrieval algorithm. The attosecond measurements of the Auger decay in Xe show pronounced broadening of the Auger lines corresponding to the formation of sidebands. The temporal evolution of the sideband signals and their asymmetry along the laser polarization axis exhibit oscillations similar to those known from attosecond streaking measurements. The experimental results are in good agreement with model calculations based on an analytical solution of the Schr?dinger equation within the strong field approximation.

Attosecond control of electron localization in one- and two-color dissociative ionization of H 2 and D 2

We present one-color (IR) and two-color (single attosecond XUV pulse + IR) experiments where the sub-cycle evolution of the electric field of light is used to control the dissociative ionization of hydrogen and deuterium molecules.

Attosecond excitation of electron wavepackets

We present experiments, supported by time-dependent Schrodinger simulations, on the dynamics of Helium bound states after an attosecond excitation in the presence of a strong infrared laser field.