Real-time observation of electronic, vibrational, and rotational dynamics in nitric oxide with attosecond soft x-ray pulses at 400 eV

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.

High-harmonic generation (HHG) traditionally combines ~100 near-infrared laser photons to generate bright, phase-matched, extreme ultraviolet beams when the emission from many atoms adds constructively. Here, we show that by guiding a mid-infrared femtosecond laser in a high-pressure gas, ultrahigh harmonics can be generated, up to orders greater than 5000, that emerge as a bright supercontinuum that spans the entire electromagnetic spectrum from the ultraviolet to more than 1.6 kilo-electron volts, allowing, in principle, the generation of pulses as short as 2.5 attoseconds. The multiatmosphere gas pressures required for bright, phase-matched emission also support laser beam self-confinement, further enhancing the x-ray yield. Finally, the x-ray beam exhibits high spatial coherence, even though at high gas density the recolliding electrons responsible for HHG encounter other atoms during the emission process.