Attophysics

Abstract: 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.

Abstract: We generated single-cycle isolated attosecond pulses around ∼36 electron volts using phase-stabilized 5-femtosecond driving pulses with a modulated polarization state. Using a complete temporal characterization technique, we demonstrated the compression of the generated pulses for as low as 130 attoseconds, corresponding to less than 1.2 optical cycles. Numerical simulations of the generation process show that the carrier-envelope phase of the attosecond pulses is stable. The availability of single-cycle isolated attosecond pulses opens the way to a new regime in ultrafast physics, in which the strong-field electron dynamics in atoms and molecules is driven by the electric field of the attosecond pulses rather than by their intensity profile.

Abstract: 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.

Abstract: Chemical reactions are triggered by the dynamics of valence electrons in molecular orbitals. These motions typically unfold on a subfemtosecond scale and have eluded real-time access until now. Attosecond spectroscopy (an attosecond is 10−18 seconds), first applied to tracking electronic transitions from one quantum state to another, has now been extended to follow the hyperfast (subfemtosecond) motion of electron wavepackets in the valence shell — the bond-forming electrons — of krypton ions. This first proof-of-principle demonstration uses a simple system, but the expectation is that attosecond transient absorption spectroscopy of this type will ultimately reveal the elementary electron motions in molecules and solid-state materials that determine physical, chemical and biological properties. Attosecond technology (1 as = 10−18 S) promises the tools needed to directly probe electron motion in real time. These authors report attosecond pump–probe measurements that track the movement of valence electrons in krypton ions. This first proof-of-principle demonstration uses a simple system, but the expectation is that attosecond transient absorption spectroscopy will ultimately also reveal the elementary electron motions that underlie the properties of molecules and solid-state materials. 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 ions1. We generate the ions with a controlled few-cycle laser field2 and then probe them through the spectrally resolved absorption of an attosecond extreme-ultraviolet pulse3, 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.