  The detection of electron motion and electronic wavepacket dynamics is one of
the core goals of attosecond science. Recently, choosing the nitric oxide (NO)
molecule as an example, we have introduced and demonstrated a new experimental
approach to measure coupled valence electronic and rotational wavepackets using
high-harmonic generation (HHG) spectroscopy [Kraus et al., Phys. Rev. Lett.
111, 243005 (2013)]. A short outline of the theory to describe the combination
of the pump and HHG probe process was published together with an extensive
discussion of experimental results [Baykusheva et al., Faraday Discuss 171, 113
(2014)]. The comparison of theory and experiment showed good agreement on a
quantitative level. Here, we present the generalized theory in detail, which is
based on a generalized density matrix approach that describes the pump process
and the subsequent probing of the wavepackets by a semiclassical quantitative
rescattering approach. An in-depth analysis of the different Raman scattering
contributions to the creation of the coupled rotational and electronic
spin-orbit wavepackets is made. We present results for parallel and
perpendicular linear polarizations of the pump and probe laser pulses.
Furthermore, an analysis of the combined rotational-electronic density matrix
in terms of irreducible components is presented, that facilitates
interpretation of the results.
