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We experimentally investigated a delayed fragmentation of hydrocarbon molecules on nanosecond to microsecond timescale after double ionization by femtosecond laser pulses. Quantum chemical simulations suggest that it originates from meta-stable high-lying vibrational states of dications.

Single and double electron recapture processes into Rydberg states driven by few-cycle laser pulses are studied for argon dimers. The electron emission and recapture dynamics show a strong dependence on the pulses’ carrier-envelope phase.

We demonstrated coincidence detection of high-lying Rydberg states populated in strong field interaction. Simulations reveals the measured ionization signal of Rydberg states originates from DC field induced tunneling ionization and photoionization by blackbody radiation.

Using a double-pulse scheme we visualize and control molecular dynamics taking place on intermediately populated states during different sequential double ionization pathways of CO2. Exchanging the pulse-sequence can almost completely switch the pathway.

The dynamics of sequential two-electron emission from helium is extracted from measured momentum distributions. Emission in between the field-maxima and on sub-laser-cycle times is identified. The corresponding structures are roughly reproduced by a semi-classical model.

Using coincidence momentum spectroscopy we show that the external laser field’s properties driving the internal molecular dynamics have negligible influence on the decision to follow a given fragmentation pathway in three-body fragmentation of polyatomic molecules.