Michael Hofstetter

Single-cycle nonlinear optics

Nonlinear optics plays a central role in the advancement of optical science and laser-based technologies. We report on the confinement of the nonlinear interaction of light with matter to a single wave cycle and demonstrate its utility for time-resolved and strong-field science. The electric field of 3.3-femtosecond, 0.72-micron laser pulses with a controlled and measured waveform ionizes atoms near the crests of the central wave cycle, with ionization being virtually switched off outside this interval. Isolated sub-100-attosecond pulses of extreme ultraviolet light (photon energy ∼ 80 electron volts), containing ∼0.5 nanojoule of energy, emerge from the interaction with a conversion efficiency of ∼10–6. These tools enable the study of the precision control of electron motion with light fields and electron-electron interactions with a resolution approaching the atomic unit of time (∼24 attoseconds).

Delay in Photoemission

Defining Time-Zero When a high-energy photon hits an atom and is absorbed, the result can be the excitation and emission of an electron. This photoemission, or photoelectric effect, is generally assumed to occur instantaneously, and represents the definition of “time-zero” in clocking such ultrafast events. Schultze et al. (p. 1658, see the cover; see the Perspective by van der Hart) use ultrafast spectroscopy, with light pulses on the time scale of several tens of attoseconds, to test this assumption directly. They excite neon atoms with 100 eV photons and find that there is a small (20-attosecond) time delay between the emission of electrons from the 2s and 2p orbitals of the atoms. These results should have implications in modeling electron dynamics occurring on ultrafast time scales. Ultrafast metrology reveals a 20-attosecond delay between photoemission from different electronic orbitals in neon atoms. 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.

Controlling dielectrics with the electric field of light

The control of the electric and optical properties of semiconductors with microwave fields forms the basis of modern electronics, information processing and optical communications. The extension of such control to optical frequencies calls for wideband materials such as dielectrics, which require strong electric fields to alter their physical properties. Few-cycle laser pulses permit damage-free exposure of dielectrics to electric fields of several volts per ångström and significant modifications in their electronic system. Fields of such strength and temporal confinement can turn a dielectric from an insulating state to a conducting state within the optical period. However, to extend electric signal control and processing to light frequencies depends on the feasibility of reversing these effects approximately as fast as they can be induced. Here we study the underlying electron processes with sub-femtosecond solid-state spectroscopy, which reveals the feasibility of manipulating the electronic structure and electric polarizability of a dielectric reversibly with the electric field of light. We irradiate a dielectric (fused silica) with a waveform-controlled near-infrared few-cycle light field of several volts per angström and probe changes in extreme-ultraviolet absorptivity and near-infrared reflectivity on a timescale of approximately a hundred attoseconds to a few femtoseconds. The field-induced changes follow, in a highly nonlinear fashion, the turn-on and turn-off behaviour of the driving field, in agreement with the predictions of a quantum mechanical model. The ultrafast reversibility of the effects implies that the physical properties of a dielectric can be controlled with the electric field of light, offering the potential for petahertz-bandwidth signal manipulation.

Powerful 170-attosecond XUV pulses generated with few-cycle laser pulses and broadband multilayer optics

Single 170-as extreme ultraviolet (XUV) pulses delivering more than 10 6 photons/pulse at ∼100 eV at a repetition rate of 3 kHz are produced by ionizing neon with waveform-controlled sub-5 fs near-infrared (NIR) laser pulses and spectrally filtering the emerging near-cutoff high-harmonic continuum with a broadband, chirped multilayer molybdenum-silicon (Mo/Si) mirror.

Attosecond dispersion control by extreme ultraviolet multilayer mirrors

We report the first experimental demonstration of a-periodic multilayer mirrors controlling the frequency sweep (chirp) of isolated attosecond XUV pulses. The concept was proven with about 200-attosecond pulses in the photon energy range of 100-130 eV measured via photoelectron streaking in neon. The demonstrated attosecond dispersion control is engineerable in a wide range of XUV photon energies and bandwidths. The resultant tailor-made attosecond pulses with highly enhanced photon flux are expected to significantly advance attosecond metrology and spectroscopy and broaden their range of applications.

Versatile apparatus for attosecond metrology and spectroscopy

We present the AS-2 Attosecond Beamline at the Joint Laboratory for Attosecond Physics of the Max-Planck-Institut für Quantenoptik and Ludwig-Maximilians-Universität for time resolved pump/probe experiments with attosecond resolution. High harmonic generation and subsequent filtering of the generated extreme ultraviolet (XUV) continuum by means of metal filters and XUV multilayer mirrors serve for the generation of isolated attosecond laser pulses. After high harmonic generation, the remaining fundamental laser pulse is spatially separated from the attosecond XUV pulse, to what is to our knowledge for the first time, by means of a perforated mirror in a Mach-Zehnder interferometer. Active stabilization of this interferometer guarantees the necessary temporal resolution for tracking attosecond dynamics in real time. As a proof-of-principle, photoelectron streaking experiments are performed and experimental techniques for their realization are summarized. Finally we highlight the potential of the presented beamline system for future experiments in comparison with previously demonstrated attosecond beamlines.

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.

Lanthanum–molybdenum multilayer mirrors for attosecond pulses between 80 and 130 eV

A novel multilayer material system consisting of lanthanum and molybdenum nano-layers for both broadband and highly reflecting multilayer mirrors in the energy range between 80 and 130 eV is presented. The simulation and design of these multilayers were based on an improved set of optical constants, which were recorded by extreme ultraviolet (XUV)/soft-x-ray absorption measurements on freestanding lanthanum nano-films between 30 eV and 1.3 keV. Lanthanum–molybdenum (La/Mo) multilayer mirrors were produced by ion-beam sputtering and characterized through both x-ray and XUV reflectivity measurements. We demonstrate the ability to precisely simulate and realize aperiodic stacks. Their stability against ambient air conditions is demonstrated. Finally, the La/Mo mirrors were used in the generation of single attosecond pulses from high-harmonic cut-off spectra above 100 eV. Isolated 200 attosecond-long pulses were measured by XUV-pump/IR-probe streaking experiments and characterized using frequency-resolved optical gating for complete reconstruction of attosecond bursts (FROG/CRAB) analyses.

Ion polished Cr/Sc attosecond multilayer mirrors for high water window reflectivity

Recent advances in the development of attosecond soft X-ray sources ranging into the water window spectral range, between the 1s states of carbon and oxygen (284 eV-543 eV), are also driving the development of suited broadband multilayer optics for steering and shaping attosecond pulses. The relatively low intensity of current High Harmonic Generation (HHG) soft X-ray sources calls for an efficient use of photons, thus the development of low-loss multilayer optics is of uttermost importance. Here, we report about the realization of broadband Cr/Sc attosecond multilayer mirrors with nearly atomically smooth interfaces by an optimized ion beam deposition and assisted interface polishing process. This yields to our knowledge highest multilayer mirror reflectivity at 300 eV near normal incidence. The results are verified by transmission electron microscopy (TEM) and soft/hard X-ray reflectometry.

Generation of circularly polarized high harmonic radiation using a transmission multilayer quarter waveplate

High harmonic radiation is meanwhile nearly extensively used for the spectroscopic investigation of electron dynamics with ultimate time resolution. The majority of high harmonic beamlines provide linearly polarized radiation created in a gas target. However, circular polarization greatly extends the spectroscopic possibilities for high harmonics, especially in the analysis of samples with chirality or prominent spin polarization. We produced a free-standing multilayer foil as a transmission EUV quarter waveplate and applied it for the first time to high harmonic radiation. We measured a broadband (4.6 eV FWHM) ellipticity of 75% at 66 eV photon energy with a transmission efficiency of 5%. The helicity is switchable and the ellipticity can be adjusted to lower values by angle tuning. As a single element it can be easily integrated in any existing harmonic beamline without major changes.