We introduce and experimentally demonstrate a method, where the two intrinsic time scales of a molecule, the slow nuclear motion and the fast electronic motion, are simultaneously measured in a photo-electron photo-ion coincidence experiment. In our experiment, elliptically polarized, 750 nm, 4.5 fs laser pulses were focused to an intensity of 9×10 14 W/cm 2 onto H2. Using coincidence imaging, we directly observe the nuclear wavepacket evolving on the 1sσg state of H + 2 during its first roundtrip with attosecond temporal and picometer spatial resolution. The demonstrated method should enable insight into the first few femtoseconds of the vibronic dynamics of ionization-induced unimolecular reactions of larger molecules. t −∞ E(t )dt . Thus, measurement of the electron emission angle in the laboratory frame determines the ionization time t i within one cycle. In addition, the magnitude of the emitted electron's momentum vector |p e | is proportional to the instantaneous field strength and thereby provides a measure about the ionization time arXiv:1907.05347v1 [physics.chem-ph]

We report on the unambiguous observation of the subcycle ionization bursts in sequential strong-field double ionization of H 2 and their disentanglement in molecular frame photoelectron angular distributions. This observation was made possible by the use of few-cycle laser pulses with a known carrier-envelope phase, in combination with multiparticle coincidence momentum imaging. The approach demonstrated here will allow sampling of the intramolecular electron dynamics and the investigation of charge-statespecific Coulomb distortions on emitted electrons in polyatomic molecules.

No abstract

We report on an experimental and theoretical study of the ionization-fragmentation dynamics of argon dimers in intense few-cycle laser pulses with a tagged carrier-envelope phase. We find that a field-driven electron transfer process from one argon atom across the system boundary to the other argon atom triggers subcycle electron-electron interaction dynamics in the neighboring atom. This attosecond electron-transfer process between distant entities and its implications manifests itself as a distinct phase-shift between the measured asymmetry of electron emission curves of the Ar þ þ Ar 2þ and Ar 2þ þ Ar 2þ fragmentation channels. This letter discloses a strong-field route to controlling the dynamics in molecular compounds through the excitation of electronic dynamics on a distant molecule by driving intermolecular electrontransfer processes.

We report on the retrieval of the angular dependence of laser-induced electron rescattering in CO2 with a novel method from the measured rotational half revival signals of filed-free aligned molecules using a reaction microscope.