Summary form only given. Fundamental processes in atoms, molecules, as well as condensed matter are triggered or mediated by the motion of electrons inside or between atoms. Electronic dynamics on atomic length scales tends to unfold within tens to thousands of attoseconds (1 attosecond [as] = 10-18 s). Recent breakthroughs in laser science are now opening the door to watching and controlling these hitherto inaccessible microscopic dynamics. The key to accessing the attosecond time domain is the control of the electric field of (visible) light, which varies its strength and direction within less than a femtosecond (1 femtosecond = 1000 attoseconds). Atoms exposed to a few oscillations cycles of intense laser light are able to emit a single extreme ultraviolet (XUV) burst lasting less than one femtosecond. Full control of the evolution of the electromagnetic field in laser pulses comprising a few wave cycles have recently allowed the reproducible generation and measurement of isolated sub-femtosecond XUV pulses, demonstrating the control of microscopic processes (electron motion and photon emission) on an attosecond time scale. These tools have enabled us to visualize the oscillating electric field of visible light with an attosecond "oscilloscope", to control single-electron and probe multi-electron dynamics in atoms, molecules and solids. Recent experiments hold promise for the development of an attosecond X-ray source, which may pave the way towards 4D electron imaging with sub-atomic resolution in space and time.

Attosecond Physics

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 x 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.

Attosecond control of electronic processes by intense light fields

High-order harmonic generation is a nonlinear optical process that enables the creation of light pulses at frequencies much higher than that from a seed laser. The host medium for this interaction is typically a gas. Now, the process has been observed in a bulk crystalline solid with important implications for attosecond science.

/pdf/observation-of-high-order-harmonic-generation-in-a-bulk-2ujjcse9va.pdf

Observation of high-order harmonic generation in a bulk crystal

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.

Time-resolved atomic inner-shell spectroscopy

In Bohr's 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 approximately 750-nm laser probe and approximately 100-eV excitation, our transient recorder is capable of resolving atomic electron dynamics within the Bohr orbit time.

Atomic transient recorder

In principle, the temporal beating of superposed high harmonics obtained by focusing a femtosecond laser pulse in a gas jet can produce a train of very short intensity spikes, depending on the relative phases of the harmonics. We present a method to measure such phases through two-photon, two-color photoionization. We found that the harmonics are locked in phase and form a train of 250-attosecond pulses in the time domain. Harmonic generation may be a promising source for attosecond time-resolved measurements.

https://science.sciencemag.org/content/sci/292/5522/1689.full.pdf

Observation of a Train of Attosecond Pulses from High Harmonic Generation

We present an alternative method for measuring ultrashort extreme-ultraviolet pulses that can be synchronized with an intense infrared pulse. The method, based on photoionization of a target atom by the extreme-ultraviolet pulse in the presence of the infrared pulse, has a potential accuracy of close to 1 fs and is susceptible to single-shot operation. It is demonstrated on harmonic 15 of a titanium:sapphire laser. The minimum pulse duration that can be measured is limited only by the frequency of the radiation used for the ponderomotive shift of the ionization potential (3 fs in the case of the titanium:sapphire fundamental).

https://www.physics.ohio-state.edu/~dimauro/Publications/Agostini/2000.Ponderomotive.Toma.pdf

Ponderomotive streaking of the ionization potential as a method for measuring pulse durations in the XUV domain with fs resolution

The high harmonics produced by focusing an intense femtosecond laser in a gas are theoretically shown to be locked in phase. The physics of this locking is discussed and a new method based on quantum interference in two-photon, two-color ionization allowing to retrieve the relative phase of harmonic pairs is described. The main result is that the 5 harmonics of orders 11-19 produced in argon generate a train of subfemtosecond pulses with a period of 1.35 fs and a duration of 250 attoseconds.

/pdf/towards-attosecond-pulses-with-high-harmonics-5azrak8uoa.pdf

E. S. Toma

Papers

Observation of a Train of Attosecond Pulses from High Harmonic Generation

Ponderomotive streaking of the ionization potential as a method for measuring pulse durations in the XUV domain with fs resolution

Towards attosecond pulses with high harmonics