Abstract

Bi3.15Nd0.85Ti2.99Mn0.01O12 (BNTM) thin films with (200)-orientations, (117)-orientations, and mixed-orientations were prepared by sol-gel methods. The influence of orientations on polarization fatigue behaviors of BNTM thin films were systematically investigated at both low and elevated temperatures. It was found that the changed trends of the polarization fatigue of (200)-oriented and (117)-oriented BNTM thin films at elevated temperatures were opposite. The fatigue properties become exacerbated for the (200)-oriented ones and become improved for the (117)-oriented ones, while the reduction of remanent polarization first decreases and then increases for the mixed-oriented ones. It can be assumed that the different roles played by domain walls and interface layer with increasing T in these thin films have caused such differences, which was certified by the lower activation energies (0.12–0.13 eV) of (200)-oriented BNTM thin films compared to those of BNTM thin films (0.17–0.31 eV) with other orientations through the temperature-dependent impedance spectra analysis. With the aid of piezoresponse force microscopy (PFM), the non-neutral tail-to-tail or head-to-head polarization configurations with greater probabilities for (117)-oriented and mixed-oriented thin films were found, while a majority of the neutral head-to-tail polarization configurations can be observed for (200)-oriented ones.

Highlights

  • Bi4Ti3O12 (BIT)-based layered ferroelectric thin films have always been one of the most potential ferroelectric materials to replace the commercial (Pb, Zr)TiO3 (PZT)-based ferroelectric random access memory (FRAM) for its high curie temperature, large remanent polarization, and good anti-fatigue properties [1,2,3]

  • Zhong et al reported that Bi3.15Nd0.85Ti2.99Mn0.01O12 (BNTM) thin film with an annealing temperature of 750 oC showed higher tunability and dielectric constant than Nd-substituted BIT (BNT) thin film annealing under a temperature of 700 °C [7]

  • Layer-by-layer crystallization was adopted in the preparation of BNTM thin films

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Summary

Introduction

Bi4Ti3O12 (BIT)-based layered ferroelectric thin films have always been one of the most potential ferroelectric materials to replace the commercial (Pb, Zr)TiO3 (PZT)-based ferroelectric random access memory (FRAM) for its high curie temperature, large remanent polarization, and good anti-fatigue properties [1,2,3]. There are numerous factors such as layer thickness, precursor solution, and annealing condition that affect the orientation of Nd-substituted BIT (Bi3.15Nd0.85Ti3O12, BNT) films [5,6,7]. Yu et al proposed that 0.10 M precursor solution for BNT showed the best ferroelectric and dielectric properties [6]. Zhong et al reported that Bi3.15Nd0.85Ti2.99Mn0.01O12 (BNTM) thin film with an annealing temperature of 750 oC showed higher tunability and dielectric constant than BNT thin film annealing under a temperature of 700 °C [7]. It has reported that BNT thin films with different orientations exhibit varying polarization

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