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Zusammenfassung:
Encoded in the transient x-ray absorption (XAS) and magnetic circular (MCD) response functions resides a wealth of information of the microscopic processes of ultrafast demagnetization. Employing state-of-the-art first-principles dynamical simulations we show that the experimentally observed energy shift of the L3 XAS peak in Ni, and the absence of a corresponding shift in the dichroic MCD response, can be explained in terms of laser-induced changes in band occupation. Strikingly, we predict that for the same ultrashort pump pulse applied to Co the opposite effect will occur: a substantial shift upward in energy of the MCD peaks will be accompanied by very small change in the position of XAS peaks, a fact we relate to the reduced d-band filling of Co that allows a greater energetic range above the Fermi energy into which charge can be excited. We also carefully elucidate the dependence of this effect on pump pulse parameters. These findings (i) establish an electronic origin for early-time peak shifts in transient XAS and MCD spectroscopy and (ii) illustrate the rich information that may be extracted from transient response functions of the underlying dynamical system.
