Phase-locking of time-delayed attosecond XUV pulse pairs.

We present a setup for the generation of phase-locked attosecond extreme ultraviolet (XUV) pulse pairs. The attosecond pulse pairs are generated by high harmonic generation (HHG) driven by two phase-locked near-infrared (NIR) pulses that are produced using an actively stabilized Mach-Zehnder interferometer compatible with near-single cycle pulses. The attosecond XUV pulses can be delayed over a range of 400 fs with a sub-10-as delay jitter. We validate the precision and the accuracy of the setup by XUV optical interferometry and by retrieving the energies of Rydberg states of helium in an XUV pump-NIR probe photoelectron spectroscopy experiment.

Experimental Control of Quantum-Mechanical Entanglement in an Attosecond Pump-Probe Experiment.

Entanglement is one of the most intriguing aspects of quantum mechanics and lies at the heart of the ongoing second quantum revolution, where it is a resource that is used in quantum key distribution, quantum computing, and quantum teleportation. We report experiments demonstrating the crucial role that entanglement plays in pump-probe experiments involving ionization, which are a hallmark of the novel research field of attosecond science. We demonstrate that the degree of entanglement in a bipartite ion + photoelectron system, and, as a consequence, the degree of vibrational coherence in the ion, can be controlled by tailoring the spectral properties of the attosecond extreme ultraviolet laser pulses that are used to create them.

Vibrational Relaxation of XUV-Induced Hot Ground State Cations of Naphthalene.

Time-resolved XUV-IR photoion mass spectroscopy of naphthalene conducted with broadband as well as with wavelength-selected narrowband XUV pulses reveals a rising probability of fragmentation characterized by a lifetime of 92 ± 4 fs. This lifetime is independent of the XUV excitation wavelength and is the same for all low appearance energy fragments recorded in the experiment. Analysis of the experimental data in conjunction with a statistical multistate vibronic model suggests that the experimental signals track vibrational energy redistribution on the potential energy surface of the ground-state cation. In particular, populations of the out-of-plane ring twist and the out-of-plane wave bending modes could be responsible for opening new IR absorption channels, leading to enhanced fragmentation.