Reconstruction of correlation-driven electron-hole dynamics by high-harmonic-generation spectroscopy

We present detailed analysis of the recently proposed technique of high-order-harmonic generation spectroscopy of correlation-driven electron hole dynamics in atoms and molecules. This novel technique resolves Auger-type processes with attosecond-scale resolution by clocking the decay process with high-harmonic generation. The harmonic generation is driven by an attosecond, XUV pump pulse and a long-duration, infrared pulse. We present the strong-field-approximation-based theory of such an XUV-initiated high-order-harmonic generation process. We detail different ways of recovering the hole survival probability by altering experimental parameters to change the time-energy mapping of the harmonics. The various reconstruction methods are then simulated for M_4,5NN Auger decay in krypton and molecular-orbital breakdown dynamics in trans-butadiene and propanal.