Controlling attosecond transient absorption with tunable, non-commensurate light fields

We demonstrate a transient absorption scheme that uses a fixed-spectrum attosecond pulse train in conjunction with a tunable probe laser to access a wide range of nonlinear light-atom interactions. We exhibit control over the time-dependent Autler–Townes splitting of the 1s4p absorption line in helium, and study its evolution from a resonant doublet to a light-induced sideband with changing probe wavelength. The non-commensurate probe also allows for the background-free study of two-infrared-photon emission processes in a collinear geometry. Using this capability, we observe two different emission pathways with non-trivial delay dependencies, one prompt and the other delayed. We identify the nonlinear processes underlying these emissions by comparing the experimental results to calculations based on the time-dependent Schrödinger equation

Attosecond Time-Domain Measurement of Core-Level-Exciton Decay in Magnesium Oxide.

Excitation of ionic solids with extreme ultraviolet pulses creates localized core-level excitons, which in some cases couple strongly to the lattice. Here, core-level-exciton states of magnesium oxide are studied in the time domain at the Mg L_{2,3} edge with attosecond transient reflectivity spectroscopy. Attosecond pulses trigger the excitation of these short-lived quasiparticles, whose decay is perturbed by time-delayed near-infrared pulses. Combined with a few-state theoretical model, this reveals that the infrared pulse shifts the energy of bright (dipole-allowed) core-level-exciton states as well as induces features arising from dark core-level excitons. We report coherence lifetimes for the two lowest core-level excitons of 2.3±0.2 and 1.6±0.5  fs and show that these are primarily a consequence of strong exciton-phonon coupling, disclosing the drastic influence of structural effects in this ultrafast relaxation process

Attosecond transient absorption and four-wave mixing with tunable IR pulses

We extend the technique of attosecond transient absorption spectroscopy by incorporating tunable IR pulses from an OPA. This technique is used to control Autler-Townes splitting and drive XUV four-wave mixing processes in Helium

Attosecond transient absorption spectroscopy of molecular nitrogen: Vibrational coherences in the b′ 1Σ+u state

Nuclear and electronic dynamics in a wavepacket comprising bound Rydberg and valence electronic states of nitrogen from 12 to 15 eV are investigated using attosecond transient absorption. Vibrational quantum beats with a fundamental period of 50 femtoseconds persist for a picosecond in the b′ 1Σ+u valence state. Multi-state calculations show that these coherences result primarily from near infrared-induced coupling between the inner and outer regions of the b′ 1Σ+u state potential and the dark a″ 1Σ+g state. The excellent spectral and temporal resolution of this technique allows measurement of the anharmonicity of the b′ 1Σ+u potential directly from the observed quantum beats