Design and Application of a Relativistic Kramers-Kronig Analysis Algorithm

Abstract

Low-loss electron energy loss spectroscopy (EELS) in the scanning transmission electron microscope (STEM) probes the valence electron density and relevant optoelectronic properties such as band gap energies and other band structure transitions. The measured spectra can be formulated in a dielectric theory framework, comparable to optical spectroscopies and ab-initio simulations. Moreover, Kramers-Kronig analysis (KKA), an inverse algorithm based on the homonym relations, can be employed for the retrieval of the complex dielectric function (CDF). However, spurious contributions traditionally not considered in this framework typically impact low-loss EELS modifying the spectral shapes and precluding the correct measurement and retrieval of the dielectric information. A relativistic KKA algorithm is able to account for the bulk and surface radiative-loss contributions to low-loss EELS, revealing the correct dielectric properties. Using a synthetic low-loss EELS model, we propose some modifications on the naive implementation of this algorithm that broadens its range of application. The robustness of the algorithm is improved by regularization, appliying previous knowledge about the shape and smoothness of the correction term. Additionally, our efficient numerical integration methodology allows processing hyperspectral datasets in a reasonable amount of time. Harnessing these abilities, we show how simultaneous relativistic KKA processing of several spectra can share information to produce an improved result.