Ferenc Krausz

Attosecond control of electronic processes by intense light fields.

The amplitude and frequency of laser light can be routinely measured and controlled on a femtosecond (10-15 s) timescale. However, in pulses comprising just a few wave cycles, the amplitude envelope and carrier frequency are not sufficient to characterize and control laser radiation, because evolution of the light field is also influenced by a shift of the carrier wave with respect to the pulse peak. This so-called carrier-envelope phase has been predicted and observed to affect strong-field phenomena, but random shot-to-shot shifts have prevented the reproducible guiding of atomic processes using the electric field of light. Here we report the generation of intense, few-cycle laser pulses with a stable carrier envelope phase that permit the triggering and steering of microscopic motion with an ultimate precision limited only by quantum mechanical uncertainty. Using these reproducible light waveforms, we create light-induced atomic currents in ionized matter; the motion of the electronic wave packets can be controlled on timescales shorter than 250 attoseconds (250 × 10-18 s). This enables us to control the attosecond temporal structure of coherent soft X-ray emission produced by the atomic currents—these X-ray photons provide a sensitive and intuitive tool for determining the carrier-envelope phase.

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).

Time-resolved atomic inner-shell spectroscopy

The characteristic time constants of the relaxation dynamics of core-excited atoms have hitherto been inferred from the linewidths of electronic transitions measured by continuous-wave extreme ultraviolet or X-ray spectroscopy. Here we demonstrate that a laser-based sampling system, consisting of a few-femtosecond visible light pulse and a synchronized sub-femtosecond soft X-ray pulse, allows us to trace these dynamics directly in the time domain with attosecond resolution. We have measured a lifetime of 7.9-0.9+1.0 fs of M-shell vacancies of krypton in such a pump–probe experiment.

Atomic transient recorder

In Bohrs model of the hydrogen atom, the electron takes about 150 attoseconds (1 as = 10-18 s) to orbit around the proton, defining the characteristic timescale for dynamics in the electronic shell of atoms. Recording atomic transients in real time requires excitation and probing on this scale. The recent observation of single sub-femtosecond (1 fs = 10-15 s) extreme ultraviolet (XUV) light pulses has stimulated the extension of techniques of femtochemistry into the attosecond regime. Here we demonstrate the generation and measurement of single 250-attosecond XUV pulses. We use these pulses to excite atoms, which in turn emit electrons. An intense, waveform-controlled, few cycle laser pulse obtains ‘tomographic images’ of the time-momentum distribution of the ejected electrons. Tomographic images of primary (photo)electrons yield accurate information of the duration and frequency sweep of the excitation pulse, whereas the same measurements on secondary (Auger) electrons will provide insight into the relaxation dynamics of the electronic shell following excitation. With the current ∼750-nm laser probe and ∼100-eV excitation, our transient recorder is capable of resolving atomic electron dynamics within the Bohr orbit time.

Compression of high-energy laser pulses below 5 fs.

High-energy 20-fs pulses generated by a Ti:sapphire laser system were spectrally broadened to more than 250 nm by self-phase modulation in a hollow fiber filled with noble gases and subsequently compressed in a broadband high-throughput dispersive system. Pulses as short as 4.5 fs with energy up to 20-microJ were obtained with krypton, while pulses as short as 5 fs with energy up to 70 microJ were obtained with argon. These pulses are, to our knowledge, the shortest generated to date at multigigawatt peak powers.

Chirped multilayer coatings for broadband dispersion control in femtosecond lasers

Optical thin-film structures exhibiting high reflectivity and a nearly constant negative group-delay dispersion over frequency ranges as broad as 80 THz are presented. This attractive combination makes these coatings well suited for intracavity dispersion control in broadband femtosecond solid-state lasers. We address design issues and the principle of operation of these novel devices.

Real-time observation of valence electron motion

The superposition of quantum states drives motion on the atomic and subatomic scales, with the energy spacing of the states dictating the speed of the motion. In the case of electrons residing in the outer (valence) shells of atoms and molecules which are separated by electronvolt energies, this means that valence electron motion occurs on a subfemtosecond to few-femtosecond timescale (1 fs = 10−15 s). In the absence of complete measurements, the motion can be characterized in terms of a complex quantity, the density matrix. Here we report an attosecond pump–probe measurement of the density matrix of valence electrons in atomic krypton ions. We generate the ions with a controlled few-cycle laser field and then probe them through the spectrally resolved absorption of an attosecond extreme-ultraviolet pulse, which allows us to observe in real time the subfemtosecond motion of valence electrons over a multifemtosecond time span. We are able to completely characterize the quantum mechanical electron motion and determine its degree of coherence in the specimen of the ensemble. Although the present study uses a simple, prototypical open system, attosecond transient absorption spectroscopy should be applicable to molecules and solid-state materials to reveal the elementary electron motions that control physical, chemical and biological properties and processes.

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.

A frequency comb in the extreme ultraviolet

Since 1998, the interaction of precision spectroscopy and ultrafast laser science has led to several notable accomplishments. Femtosecond laser optical frequency ‘combs’ (evenly spaced spectral lines) have revolutionized the measurement of optical frequencies and enabled optical atomic clocks. The same comb techniques have been used to control the waveform of ultrafast laser pulses, which permitted the generation of single attosecond pulses, and have been used in a recently demonstrated ‘oscilloscope’ for light waves. Here we demonstrate intra-cavity high harmonic generation in the extreme ultraviolet, which promises to lead to another joint frontier of precision spectroscopy and ultrafast science. We have generated coherent extreme ultraviolet radiation at a repetition frequency of more than 100 MHz, a 1,000-fold improvement over previous experiments. At such a repetition rate, the mode spacing of the frequency comb, which is expected to survive the high harmonic generation process, is large enough for high resolution spectroscopy. Additionally, there may be many other applications of such a quasi-continuous compact and coherent extreme ultraviolet source, including extreme ultraviolet holography, microscopy, nanolithography and X-ray atomic clocks.