Abstract

Sub-10 nm ferroelectric and multiferroic materials are attracting increased scientific and technological interest, owing to their exciting physical phenomena and prospects in miniaturized electronic devices, neuromorphic computing, and ultra-compact data storage. The Bi6Ti2.9Fe1.5Mn0.6O18 (B6TFMO) Aurivillius system is a rare example of a multiferroic that operates at room temperature. Since the formation of magnetic impurity phases can complicate attempts to measure ferromagnetic signal intrinsic to the B6TFMO multiferroic phase and thus limits its use, herein we minimize this by utilizing relatively large (49%) bismuth excess to counteract its volatility during sub-10 nm growth. X-ray diffraction, electron microscopy, and atomic force microscopy show sample crystallinity and purity are substantially improved on increasing bismuth excess from 5 to 49%, with the volume fraction of surface impurities decreasing from 2.95–3.97 vol% down to 0.02–0.31 vol%. Piezoresponse force microscopy reveals 8 nm B6TFMO films are ferroelectric, with an isotropic random distribution of stable in-plane domains and weaker out-of-plane piezoresponse. By reducing the volume fraction of magnetic impurities, this work demonstrates the recent progress in the optimization of ultra-thin B6TFMO for future multiferroic technologies. We show how the orientation of the ferroelectric polarization can be switched in 8 nm B6TFMO and arrays can be “written” and “read” to express states permitting anti-parallel information storage.

Highlights

  • The demonstration of robust room temperature ferroelectric and multiferroic properties that persist at sub-10 nm dimensions is crucial to their implementation in technologically competitive data storage applications (Spaldin & Ramesh, 2019)

  • This work demonstrates the recent progress in the optimization of B6TFMO materials toward achieving the ultimate goal of room temperature single-phase multiferroic behavior at sub-10 nm length scales

  • By utilizing an excess (49%) of bismuth precursor within the established (Deepak et al, 2013, 2015a, 2015b) growth window for a scalable direct liquid injection chemical vapor deposition (DLI-CVD) bismuth self-limiting process, B6TFMO films were achieved that enabled as much as a 200-fold reduction in (Mn, Fe)3O4 spinel ferrimagnetic impurity phases, compared with films synthesized with only 5% bismuth precursor excess

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Summary

Introduction

The demonstration of robust room temperature ferroelectric and multiferroic properties that persist at sub-10 nm dimensions is crucial to their implementation in technologically competitive data storage applications (Spaldin & Ramesh, 2019). In purely electronic memristors where ultra-thin (

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