article published yes P M Kraus author Denitsa Rangelova Baykusheva author 71b4d059-2a03-11ee-914d-dfa3beed6530 H J Wörner author 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. IOP Publishing2014 eng Condensed Matter PhysicsAtomic and Molecular Physicsand Optics 0953-4075 1361-6455 1311.392310.1088/0953-4075/47/12/124030 4712 yes Kraus, P. M., Baykusheva, D. R., &#38; Wörner, H. J. (2014). Two-pulse orientation dynamics and high-harmonic spectroscopy of strongly-oriented molecules. <i>Journal of Physics B: Atomic, Molecular and Optical Physics</i>. IOP Publishing. <a href="https://doi.org/10.1088/0953-4075/47/12/124030">https://doi.org/10.1088/0953-4075/47/12/124030</a> P. M. Kraus, D. R. Baykusheva, and H. J. Wörner, “Two-pulse orientation dynamics and high-harmonic spectroscopy of strongly-oriented molecules,” <i>Journal of Physics B: Atomic, Molecular and Optical Physics</i>, vol. 47, no. 12. IOP Publishing, 2014. Kraus PM, Baykusheva DR, Wörner HJ. 2014. Two-pulse orientation dynamics and high-harmonic spectroscopy of strongly-oriented molecules. Journal of Physics B: Atomic, Molecular and Optical Physics. 47(12), 124030. Kraus, P. M., et al. “Two-Pulse Orientation Dynamics and High-Harmonic Spectroscopy of Strongly-Oriented Molecules.” <i>Journal of Physics B: Atomic, Molecular and Optical Physics</i>, vol. 47, no. 12, 124030, IOP Publishing, 2014, doi:<a href="https://doi.org/10.1088/0953-4075/47/12/124030">10.1088/0953-4075/47/12/124030</a>. Kraus, P M, Denitsa Rangelova Baykusheva, and H J Wörner. “Two-Pulse Orientation Dynamics and High-Harmonic Spectroscopy of Strongly-Oriented Molecules.” <i>Journal of Physics B: Atomic, Molecular and Optical Physics</i>. IOP Publishing, 2014. <a href="https://doi.org/10.1088/0953-4075/47/12/124030">https://doi.org/10.1088/0953-4075/47/12/124030</a>. Kraus PM, Baykusheva DR, Wörner HJ. Two-pulse orientation dynamics and high-harmonic spectroscopy of strongly-oriented molecules. <i>Journal of Physics B: Atomic, Molecular and Optical Physics</i>. 2014;47(12). doi:<a href="https://doi.org/10.1088/0953-4075/47/12/124030">10.1088/0953-4075/47/12/124030</a> P.M. Kraus, D.R. Baykusheva, H.J. Wörner, Journal of Physics B: Atomic, Molecular and Optical Physics 47 (2014). 140212023-08-10T06:38:48Z2023-08-22T09:04:30Z