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A theory of ultra-fast pump-probe experiments proposed by us earlier [F.H.M.Faisal et al., Phys. Rev. Lett. 98, 143001 (2007) and F.H.M. Faisal and A.Abdurrouf, Phys. Rev. Lett. 100, 123005 (2008)] is developed here fully andapplied to investigate the phenomena of dynamic alignment and high harmonicgeneration (HHG) from coherently rotating linear molecules. The theory providesessentially analytical results for the signals that allow us to investigate thesimultaneous dependence of the HHG signals on the two externally availablecontrol parameters, namely, the relative angle between the polarizations, andthe delay-time between the two pulses. It is applied to investigate thecharacteristics of high harmonic emission from nitrogen and oxygen moleculesthat have been observed experimentally in a number of laboratories. The resultsobtained both in the time-domain and in the frequency-domain are compared withthe observed characteristics as well as directly with the data and are found toagree remarkably well. In addition we have predicted the existence of a "magic"polarization angle at which all modulations of the harmonic emission fromnitrogen molecule changes to a steady emission at the harmonic frequency. Amongother things we have also shown a correlation between the existence of the"magic" or critical polarization angles and the symmetry of the activemolecular orbitals, that is deemed to be useful in connection with the "inverseproblem" of molecular imaging from the HHG data.

physical review. a, atomic, molecular, and optical physics/physical review, a, atomic, molecular, and optical physics

A theory of intense-field dynamic alignment and high harmonic generation  from coherently rotating molecules and interpretation of intense-field  ultrafast pump-probe experiments