@article{14021,
  abstract     = {We present the detailed analysis of a new two-pulse orientation scheme that achieves macroscopic field-free orientation at the high particle densities required for attosecond and high-harmonic spectroscopies (Kraus et al 2013 arXiv:1311.3923). Carbon monoxide molecules are oriented by combining one-colour and delayed two-colour non-resonant femtosecond laser pulses. High-harmonic generation is used to probe the oriented wave-packet dynamics and reveals that a very high degree of orientation (Nup/Ntotal = 0.73–0.82) is achieved. We further extend this approach to orienting carbonyl sulphide molecules. We show that the present two-pulse scheme selectively enhances orientation created by the hyperpolarizability interaction whereas the ionization-depletion mechanism plays no role. We further control and optimize orientation through the delay between the one- and two-colour pump pulses. Finally, we demonstrate a complementary encoding of electronic-structure features, such as shape resonances, in the even- and odd-harmonic spectrum. The achieved progress makes two-pulse field-free orientation an attractive tool for a broad class of time-resolved measurements.},
  author       = {Kraus, P M and Baykusheva, Denitsa Rangelova and Wörner, H J},
  issn         = {1361-6455},
  journal      = {Journal of Physics B: Atomic, Molecular and Optical Physics},
  keywords     = {Condensed Matter Physics, Atomic and Molecular Physics, and Optics},
  number       = {12},
  publisher    = {IOP Publishing},
  title        = {{Two-pulse orientation dynamics and high-harmonic spectroscopy of strongly-oriented molecules}},
  doi          = {10.1088/0953-4075/47/12/124030},
  volume       = {47},
  year         = {2014},
}