Coincident electron-ion detection after photoionization in a "reaction microscope" is a very powerful tool to study atomic and molecular dynamics. However, the implementation of this tool in the field of attosecond science has so far been rather limited, due to the lack of high repetition rate laser sources capable of delivering few-cycle pulses with sufficient energy per pulse. In this article, the development of a Non-collinear Optical Parametric Amplifier (NOPA) capable of delivering Carrier-Envelope Phase (CEP) stable pulses with sub-6 fs duration and pulse energies in the few-µJ range is presented. The potential of combining the high repetition rate source and a reaction microscope operating at this high frequency is demonstrated in a proof-of-principle experiment on strong field ionization of Ar atoms.
Valence band photoionization of CO 2 has been studied by photoelectron spectroscopy using a velocity map imaging spectrometer and synchrotron radiation. The measured data allow retrieving electronic and vibrational branching ratios, vibrationally resolved asymmetry parameters, and the total electron yield which includes multiple strong resonances. Additionally, the spectrum of low kinetic energy electrons has been studied in the resonant region, and the evolution with photon energy of one of the forbidden transitions present in the slow photoelectrons spectrum has been carefully analyzed, indicating that in the presence of auto-ionizing resonances the vibrational populations of the ion are significantly redistributed.
We investigate the interaction of femtosecond laser pulses with an ensemble of ultracold rubidium atoms by applying shaped excitation pulses with two different types of spectral filtering. Although the pulses, which are frequency filtered with a high pass, have no spectral overlap with molecular states, we observe coherent molecular transients. Similar transients obtained with nearly transform-limited pulses, where only the atomic resonance is removed, reveal two differing oscillatory components. The resulting transients are compared among themselves and supported with quantum dynamical simulations which indicate a photoassociation process. The effect is due to the strong field interaction of the pulse with the colliding atom pair.
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