Nonlinear polarization holography of nanoscale iridium films

Abstract

Attosecond nonlinear polarization spectroscopy designates the subcycle-precise retrieval of the electric field of a femtosecond laser pulse together with the nonlinear polarization response that the laser pulse triggers in a sample. Here, we introduce a method that is all-optical and applicable to metal films. The method is called nonlinear polarization holography because it is based on the comparison of two time-domain holograms with and without a metal film on a substrate. The working principle can be understood as the time-domain analog of holographic interferometry, in which the comparison of two spatial holograms reveals changes in an object’s size and position with interferometric precision (i.e. to fractions of the wavelength). Analogously, nonlinear polarization holography provides subcycle precision (i.e. to fractions of the optical period). Nonlinear polarization holography is used here to retrieve the time-domain nonlinear response of a nanoscale iridium film. Using density matrix calculations it is shown that the knowledge of the nonlinear response with subcycle precision allows distinguishing excitation and relaxation mechanisms of low-energetic electrons.

Keywords

• ultrafast spectroscopy
• atomic layer deposition
• nonlinear polarization spectroscopy