Applicability and breakdown of transient magnetic linear dichroism

Abstract

In highly out-of-equilibrium states of matter, such as those induced by a pump laser, the applicability of well-established spectroscopic probes of magnetic order are called into question. Here we address the validity of x-ray absorption techniques in pump laser conditions, focusing on magnetic linear dichroism (MLD), a crucial probe of antiferromagnetic (AFM) order. We directly compute the dynamics of the square of the spin moment and compare the results to those obtained via the MLD response. For AFM FePd the agreement between these distinct routes to the magnetic moment severely degrades at pulse fluences greater than ∼1mJ/cm2, indicating a breakdown of the MLD response as an accurate probe of the transient moment. This contrasts with the MLD for ferromagnetic FePt, which reliably tracks the moment for fluences (and absorbed energies) up to an order of magnitude greater than the breakdown threshold for AFM FePd. We find the underlying microscopic reason for this to be increased laser induced excitations out of the d band in AFM FePd, where this increase is made possible by the AFM pseudogap.