P. Peng, C. Marceau, M. Hervé, P. B. Corkum, A. Yu Naumov, and D. M. Villeneuve

Transient absorption spectroscopy is utilized extensively for measurements of bound- and quasibound-state dynamics of atoms and molecules. The extension of this technique into the extreme ultraviolet (XUV) region with attosecond pulses has the potential to attain unprecedented time resolution. Here we apply this technique to aligned-in-space molecules. The XUV pulses are much shorter than the time during which the molecules remain aligned, typically < < 100 fs. However, transient absorption is not an instantaneous probe, because long-lived coherences re-emit for picoseconds to nanoseconds. Due to dephasing of the rotational wavepacket, it is not clear if these coherences will be evident in the absorption spectrum, and whether the properties of the initial excitations will be preserved. We studied Rydberg states of N2 2 and O2 2 from 12 to 23 eV. We were able to determine the polarization direction of the electronic transitions, and hence identify the symmetry of the final states.

Xiaoyan Ding, R. Forbes, M. Kübel, Kevin, F. Lee, M. Spanner, A. Yu. Naumov, D. M. Villeneuve, A. Stolow, P. B. Corkum, and A. Staudte

We study the near-threshold photodissociation dynamics of NO2 by a kinematically complete femtosecond pump-probe scheme using a cold target recoil ion momentum spectrometer. We excite NO2 to the optically bright Ã2B2 state with a 400 nm pulse and probe the ensuing dynamics via strong field single and double ionization with a 25 fs, 800 nm pulse. The pump spectrum spans the NO(X2Π) + O(3P) dissociation channel threshold, and therefore, following internal conversion, excited NO2 is energetically prepared both “above threshold” (dissociating) and “below threshold” (nondissociating). Experimentally, we can clearly discriminate a weak two-photon pump channel from the dominant single-photon data. In the single ionization channel, we observe NO+ fragments with nonzero momentum at 200 fs delay and an increasing yield of NO+ fragments with near-zero momentum at 3.0 ps delay. For double ionization events, we observe a time-varying Coulombic kinetic energy release between the NO+ and O+ fragments impulsively created from the evolving “hot” neutral ground state. Supported by classical trajectory calculations, we assign the decreasing Coulombic kinetic energy release at longer time delays to the increasing average NO–O distances in the ground electronic state during its large amplitude phase space evolution toward free products. The time-resolved kinetic energy release in the double ionization channel probes the large amplitude ground state evolution from a strongly coupled “inner region” to a loosely coupled “outer region” where one O atom is on average much further away from the NO. Both the time evolution of the kinetic energy release and the NO+ angular distributions support our assignments.

F. Hufnagel, A. Sit, F. Grenapin, F. Bouchard, K. Heshami, D. England, Y. Zhang, B. J. Sussman, R. W. Boyd, G. Leuchs, and E. Karimi

We examine the propagation of optical beams possessing different polarization states and spatial modes through the Ottawa River in Canada. A Shack-Hartmann wavefront sensor is used to record the distorted beam’s wavefront. The turbulence in the underwater channel is analysed, and associated Zernike coefficients are obtained in real-time. Finally, we explore the feasibility of transmitting polarization states as well as spatial modes through the underwater channel for applications in quantum cryptography.