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Register a new userOrigin of the Enhanced Polarization in La and Mg Co-substituted BiFeO3 Thin Film during the Fatigue Process
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We have studied the polarization fatigue of La and Mg co-substituted BiFeO3 thin film, where a polarization peak is observed during the fatigue process. The origin of such anomalous behavior is analyzed on the basis of the defect evolution using temperature-dependent impedance spectroscopy. It shows that the motion of oxygen vacancies (VO..) is associated with a lower energy barrier, accompanied by the injection of electrons into the film during the fatigue process. A qualitative model is proposed to explain the fatigue behavior, which involves the modification of the Schottky barrier upon the accumulation of VO.. at the metal-dielectric interface.
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The conductive characteristics of Bi0.9La0.1Fe0.96Mg0.04O3(BLFM) thin film are investigated at various temperatures and a negative differential resistance (NDR) is observed in the thin film, where a leakage current peak occurs upon application of a downward electric field above 80 oC. The origin of the NDR behavior is shown to be related to the ionic defect of oxygen vacancies (VO..) present in the film. On the basis of analyzing the leakage mechanism and surface potential behavior, the NDR behavior can be understood by considering the competition between the polarized distribution and neutralization of VO...
As a room-temperature multiferroic, BiFeO3 has been intensively investigated for both magnetoelectric devices and non-volatile ferroelectric memory applications. Both magnetoelectric and ferroelectric memory devices have the same control knob: polarization switching by an applied electric field. Due to the rhombohedral symmetry of BiFeO3, there are four ferroelastic variances and three different polarization switching events: (1) 71{deg} switching from r1- to r3+, (2) 109{deg} switching from r1- to r2+ (or r4+), and (3) 180o switching from r1- to r1+ (the superscript + and - stand for up and down polarization, respectively). Each switching path is coupled to a different reorientation of the BiFeO3 unit cell, and hence different coupling to the magnetic order as well as different magnitudes of switchable polarization. A degradation of the ferroelectric properties of BiFeO3 will result in losing controllability of magnetic order switching in magnetoelectric devices and capacity for information storage in ferroelectric memory devices. Especially, polarization fatigue will directly restrict the reliability of the actual devices. Hence it is important to understand the intrinsic fatigue behavior of each polarization switching path in BiFeO3 thin films. In this communication, we report polarization fatigue in BiFeO3 depending on switching path, and propose a fatigue model which will broaden our understanding of the fatigue phenomenon in low-symmetry materials.
The influence of La and Nd co-substitution on the structural and magnetic properties of BiFeO3 (BFO) thin films was examined. Epitaxial thin films of pure and, La and Nd co-doped BFO on the SrRuO3 buffered single crystal SrTiO3 (001) substrate were deposited using pulsed laser deposition. The structural change in co doped La and Nd BFO thin films which was caused by the changes of force constant in the crystal lattice induced by ionic radii mismatch was investigated. Raman spectroscopy studies manifest the structural change in doped BFO films from rhombohedral to monoclinic distorted phase which is induced by the co substitution of La and Nd. Room temperature magnetic hysteresis curves indicated that saturation magnetization is enhanced in the doped film with saturation magnetization of ~20 emu/cm3. The dielectric and magnetic properties are effectively improved in BLNFO films compared to pure BFO thin films.
Oxygen-vacancies-related dielectric relaxation and scaling behaviors of Bi0.9La0.1Fe0.98Mg0.02O3 (BLFM) thin film have been investigated by temperature-dependent impedance spectroscopy from 40 oC up to 200 oC. We found that hopping electrons and single-charged oxygen vacancies (VO.) coexist in the BLFM thin film and make contribution to dielectric response of grain and grain boundary respectively. The activation energy for VO. is shown to be 0.94 eV in the whole temperature range investigated, whereas the distinct activation energies for electrons are 0.136 eV below 110oC and 0.239 eV above 110oC in association with hopping along the Fe2+- VO.-Fe3+ chain and hopping between Fe2+-Fe3+, respectively, indicating different hopping processes for electrons. Moreover, it has been found that hopping electrons is in form of long rang movement, while localized and long range movement of oxygen vacancies coexist in BLFM film. The Cole-Cole plots in modulus formalism show a poly-dispersive nature of relaxation for oxygen vacancies and a unique relaxation time for hopping electrons. The scaling behavior of modulus spectra further suggests that the distribution of relaxation times for oxygen vacancies is temperature independent.
Fatigue failure in ferroelectrics has been intensively investigated in the past few decades. Most of the mechanisms discussed for ferroelectric fatigue have been built on the hypothesis of variation in charged defects, which however are rarely evidenced by experimental observation. Here, using a combination of complex impedance spectra techniques, piezoresponse force microscopy and first-principles theory, we examine the microscopic evolution and redistribution of charged defects during the electrical cycling in BiFeO3 thin films. The dynamic formation and melting behaviors of oxygen vacancy (VO) order are identified during the fatigue process. It reveals that the isolated VO tend to self-order along grain boundaries to form a planar-aligned structure, which blocks the domain reversals. Upon further electrical cycling, migration of VO within vacancy clusters is accommodated with a lower energy barrier (~0.2 eV) and facilitates the formation of nearby-electrode layer incorporated with highly concentrated VO. The interplay between the macroscopic fatigue and microscopic evolution of charged defects clearly demonstrates the role of ordered VO cluster in the fatigue failure of BiFeO3 thin films.
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