Tailoring c-axis orientation in epitaxial Ruddlesden-Popper Pr$_{0.5}$Ca$_{1.5}$MnO$_{4}$ films

TL;DR

This study demonstrates how to control the c-axis orientation in epitaxial Ruddlesden-Popper Pr$_{0.5}$Ca$_{1.5}$MnO$_4$ films using different substrates, buffer layers, and growth techniques, affecting their structural and electronic properties.

Contribution

It introduces methods to tailor c-axis orientation in RP-PCMO films through substrate choice, buffer layers, and various deposition techniques, revealing consistent structural features across methods.

Findings

C-axis orientation depends on substrate and buffer layer choice.

Different deposition techniques yield similar film morphology and structure.

Charge ordering temperature remains close to bulk values.

Abstract

Interest for layered Ruddlesden-Popper strongly correlated manganites of Pr$_{0.5}$Ca$_{1.5}$MnO$_4$ as well as to their thin film polymorphs is motivated by the high temperature of charge orbital ordering above room temperature. We report on the tailoring of the c-axis orientation in epitaxial RP-PCMO films grown on SrTiO$_3$ (STO) substrates with different orientations as well as the use of CaMnO$_3$ (CMO) buffer layers. Films on STO(110) reveal in-plane alignment of the c-axis lying along to the [100] direction. On STO(100), two possible directions of the in-plane c-axis lead to a mosaic like, quasi two-dimensional nanostructure, consisting of RP, rock-salt and perovskite building blocks. With the use of a CMO buffer layer, RP-PCMO epitaxial films with c-axis out-of-plane were realized. Different physical vapor deposition techniques, i.e. ion beam sputtering (IBS), pulsed laser deposition (PLD) as well as metalorganic aerosol deposition (MAD) are applied in order to distinguish between the effect of growth conditions and intrinsic epitaxial properties. For all deposition techniques, despite their very different growth conditions, the surface morphology, crystal structure and orientation of the thin films reveal a high level of similarity as verified by X-ray diffraction, scanning and high resolution transmission electron microscopy. We found that for different epitaxial relations the stress in the films can be relaxed by means of a modified interface chemistry. The charge ordering in the films estimated by resistivity measurements occurs at a temperature close to that expected in bulk material.