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Register a new userMicrostructural Evolution of Charged Defects in the Fatigue Process of Polycrystalline BiFeO3 Thin Films
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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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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.
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.
We present the temperature- and thickness-dependent structural and morphological evolution of strain induced transformations in highly-strained epitaxial BiFeO3 films deposited on LaAlO3 (001) substrates. Using high-resolution X-ray diffraction and temperature-dependent scanning-probe-based studies we observe a complex temperature- and thickness-dependent evolution of phases in this system. A thickness-dependent transformation from a single monoclinically distorted tetragonal-like phase to a complex mixed-phase structure in films with thicknesses up to ~200 nm is the consequence of a strain-induced spinodal instability in the BiFeO3/LaAlO3 system. Additionally, a breakdown of this strain-stabilized metastable mixed-phase structure to non-epitaxial microcrystals of the parent rhombohedral structure of BiFeO3 is observed to occur at a critical thickness of ~300 nm. We further propose a mechanism for this abrupt breakdown that provides insight into the competing nature of the phases in this system.
In this work we report on the controlled fabrication of a self-assembled line network in highly epitaxial BiFeO3 thin films on top of LaAlO3 in the kinetically limited grown region by RF sputtering. As previously shown in the case of manganite thin films, the remarkable degree of ordering is achieved using vicinal substrates with well-defined step-terrace morphology. Nanostructured BiFeO3 thin films show mixed-phase morphology. Besides typical formation following (100) and (010) axes, some mixed phase nanodomains are detected also in-between the regular line network. These particular microstructures open a playground for future applications in multiferroic nanomaterials.
By using piezoelectric force microscopy and scanning Kelvin probe microscopy, we have investigated the domain evolution and space charge distribution in planar BiFeO3 capacitors with different electrodes. It is observed that charge injection at the film/electrode interface leads to domain pinning and polarization fatigue in BiFeO3. Furthermore, the Schottky barrier at the interface is crucial for the charge injection process. Lowering the Schottky barrier by using low work function metals as the electrodes can also improve the fatigue property of the device, similar to what oxide electrodes can achieve.
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