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Register a new userOxygen-vacancy-related relaxation and scaling behaviors of Bi0.9La0.1Fe0.98Mg0.02O3 (La,Mg-codoped BiFeO3) ferroelectric thin film
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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.
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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.
We present a comprehensive study of polar and magnetic excitations in BiFeO3 ceramics and a thin film epitaxially grown on an orthorhombic (110) TbScO3 substrate. Infrared reflectivity spectroscopy was performed at temperatures from 5 to 900 K for the ceramics and below room temperature for the thin film. All 13 polar phonons allowed by the factor-group analysis were observed in theceramic samples. The thin-film spectra revealed 12 phonon modes only and an additional weak excitation, probably of spin origin. On heating towards the ferroelectric phase transition near 1100 K, some phonons soften, leading to an increase in the static permittivity. In the ceramics, terahertz transmission spectra show five low-energy magnetic excitations including two which were not previously known to be infrared active; at 5 K, their frequencies are 53 and 56 cm-1. Heating induces softening of all magnetic modes. At a temperature of 5 K, applying an external magnetic field of up to 7 T irreversibly alters the intensities of some of these modes. The frequencies of the observed spin excitations provide support for the recently developed complex model of magnetic interactions in BiFeO3 (R.S. Fishman, Phys. Rev. B 87, 224419 (2013)). The simultaneous infrared and Raman activity of the spin excitations is consistent with their assignment to electromagnons.
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There is growing evidence that domain walls in ferroics can possess emergent properties that are absent in bulk materials. For example, 180 domain walls in the ferroelectric-antiferromagnetic BiFeO3 are particularly interesting because they have been predicted to possess a range of intriguing behaviors; including electronic conduction and enhanced magnetization. To date, however, ordered arrays of such domain structures have not been reported. Here, we report the observation of 180 stripe nanodomains in (110)-oriented BiFeO3 thin films grown on orthorhombic GdScO3 (010)O substrates, and their impact on exchange coupling to metallic ferromagnets. Nanoscale ferroelectric 180 stripe domains with {112 } domain walls were observed in films < 32 nm thick to compensate for large depolarization fields. With increasing film thickness, we observe a domain structure crossover from the depolarization field-driven 180 stripe nanodomains to 71 domains determined by the elastic energy. Interestingly, these 180 domain walls (which are typically cylindrical or meandering in nature due to a lack of strong anisotropy associated with the energy of such walls) are found to be highly-ordered. Additional studies of Co0.9Fe0.1/BiFeO3 heterostructures reveal exchange bias and exchange enhancement in heterostructures based-on BiFeO3 with 180 domain walls and an absence of exchange bias in heterostructures based-on BiFeO3 with 71 domain walls; suggesting that the 180 domain walls could be the possible source for pinned uncompensated spins that give rise to exchange bias. This is further confirmed by X-ray circular magnetic dichroism studies, which demonstrate that films with predominantly 180 domain walls have larger magnetization than those with primarily 71 domain walls. Our results could be useful to extract the structure of domain walls and to explore domain wall functionalities in BiFeO3.
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