In situ photoemission study on atomically-controlled La$_{1-x}$Sr$_x$MnO$_3$ thin films: Composition dependence of the electronic structure

TL;DR

This study uses in situ photoemission and x-ray absorption spectroscopy to explore how the electronic structure of La$_{1-x}$Sr$_x$MnO$_3$ thin films varies with composition, revealing deviations from simple models and evidence of spectral weight transfer.

Contribution

It provides detailed insights into the composition-dependent electronic structure of LSMO thin films, highlighting the limitations of the rigid-band model and identifying spectral weight transfer phenomena.

Findings

Valence band and core levels shift monotonically with doping.

The $e_g$ orbital peak moves toward $E_F$ but decreases in intensity.

Spectral weight transfer indicates a pseudogap and complex electronic behavior.

Abstract

We have investigated change in the electronic structures of atomically-controlled La$_{1-x}$Sr$_x$MnO$_3$ (LSMO) thin films as a function of hole-doping level ($x$) in terms of {\it in situ} photoemission spectroscopy (PES) and x-ray absorption spectroscopy (XAS) measurements. The {\it in situ} PES measurements on a well-ordered surface of high-quality epitaxial LSMO thin films enable us to reveal their intrinsic electronic structures, especially the structure near the Fermi level ($E_F$). We have found that overall features of valence band as well as the core levels monotonically shifted toward lower binding energy as $x$ was increased, indicating the rigid-band like behavior of underlying electronic structure of LSMO thin films. The peak nearest to $E_F$ due to the $e_g$ orbital is also found to move toward $E_F$ in a rigid-band manner, while the peak intensity decreases with increasing $x$. The loss of spectral weight with $x$ in the occupied density of states was compensated by simultaneous increment of the shoulder structure in O 1$s$ XAS spectra, suggesting the existence of a pseudogap, that is depression in spectral weight at $E_F$, for all metallic compositions. These results indicate that the simple rigid-band model does not describe the electronic structure near $E_F$ of LSMO and that the spectral weight transfer from below to above $E_F$ across the gap dominates the spectral changes with $x$ in LSMO thin films.