We report on structural, microstructural, spectroscopic, dielectric, electrical, ferroelectric, ferromagnetic, and magnetodielectric coupling studies of BiFeO3–GdMnO3[(BFO)1–
- NSF-PAR ID:
- 10226853
- Date Published:
- Journal Name:
- RSC Advances
- Volume:
- 10
- Issue:
- 66
- ISSN:
- 2046-2069
- Page Range / eLocation ID:
- 40229 to 40233
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract x –(GMO)x ], wherex is the concentration of GdMnO3(x = 0.0, 0.025, 0.05, 0.075, 0.1, 0.15, and 0.2), nanocrystalline ceramic solid solutions by auto-combustion method. The analysis of structural property by Rietveld refinement shows the existence of morphotropic phase boundary (MPB) atx = 0.10, which is in agreement with the Raman spectroscopy and high resolution transmission electron microscopy (HRTEM) studies. The average crystallite size obtained from the transmission electron microscopy (TEM) and x-ray line profile analysis was found to be 20–30 nm. The scanning electron micrographs show the uniform distribution of grains throughout the surface of the sample. The dielectric dispersion behavior fits very well with the Maxwell-Wagner model. The frequency dependent phase angle (θ ) study shows the resistive nature of solid solutions at low frequency, whereas it shows capacitive behavior at higher frequencies. The temperature variation of dielectric permittivity shows dielectric anomaly at the magnetic phase transition temperature and shifting of the phase transition towards the lower temperature with increasing GMO concentration. The Nyquist plot showed the conduction mechanism is mostly dominated by grains and grain boundary resistances. The ac conductivity of all the samples follows the modified Jonscher model. The impedance and modulus spectroscopy show a non-Debye type relaxation mechanism which can be modeled using a constant phase element (CPE) in the equivalent circuit. The solid-solutions of BFO-GMO show enhanced ferromagnetic-like behavior at room temperature. The ferroelectric polarization measurement shows lossy ferroelectric behavior. The frequency dependent magnetocapacitance and magnetoimpedance clearly show the existence of intrinsic magnetodielectric coupling. The (BFO)1–x –(GMO)x solid solutions withx = 0.025–0.075 show significantly higher magnetocapacitance and magnetoimpedance compared to the pure BFO. -
null (Ed.)Controlling the growth of complex relaxor ferroelectric thin films and understanding the relationship between biaxial strain–structural domain characteristics are desirable for designing materials with a high electromechanical response. For this purpose, epitaxial thin films free of extended defects and secondary phases are urgently needed. Here, we used optimized growth parameters and target compositions to obtain epitaxial (40–45 nm) 0.67Pb(Mg 1/3 Nb 2/3 )O 3 –0.33PbTiO 3 /(20 nm) SrRuO 3 (PMN–33PT/SRO) heterostructures using pulsed-laser deposition (PLD) on singly terminated SrTiO 3 (STO) and ReScO 3 (RSO) substrates with Re = Dy, Tb, Gd, Sm, and Nd. In situ reflection high-energy electron diffraction (RHEED) and high-resolution X-ray diffraction (HR-XRD) analysis confirmed high-quality and single-phase thin films with smooth 2D surfaces. High-resolution scanning transmission electron microscopy (HR-STEM) revealed sharp interfaces and homogeneous strain further confirming the epitaxial cube-on-cube growth mode of the PMN–33PT/SRO heterostructures. The combined XRD reciprocal space maps (RSMs) and piezoresponse force microscopy (PFM) analysis revealed that the domain structure of the PMN–33PT heterostructures is sensitive to the applied compressive strain. From the RSM patterns, an evolution from a butterfly-shaped diffraction pattern for mildly strained PMN–33PT layers, which is evidence of stabilization of relaxor domains, to disc-shaped diffraction patterns for high compressive strains with a highly distorted tetragonal structure, is observed. The PFM amplitude and phase of the PMN–33PT thin films confirmed the relaxor-like for a strain state below ∼1.13%, while for higher compressive strain (∼1.9%) the irregularly shaped and poled ferroelectric domains were observed. Interestingly, the PFM phase hysteresis loops of the PMN–33PT heterostructures grown on the SSO substrates (strain state of ∼0.8%) exhibited an enhanced coercive field which is about two times larger than that of the thin films grown on GSO and NSO substrates. The obtained results show that epitaxial strain engineering could serve as an effective approach for tailoring and enhancing the functional properties in relaxor ferroelectrics.more » « less
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Abstract The present paper reports the multifunctional properties of lead‐free BiFeO3–La (BFO–La) thin films. The structural, microstructural, and optical properties have been investigated as a function of the lanthanum doping concentration. The structural properties at room temperature showed the formation of the perovskite structure, thus suggesting the high quality of the obtained thin film compositions. Raman spectroscopy analysis revealed a slight variation in both the peak position and absolute intensity for the Raman active modes, as lanthanum content increases in BiFeO3–La. Crystallized thin films with well‐defined grains as well as crack‐free surfaces have been obtained, for all the studied compositions, as inferred from atomic force microscopy images. The optical properties have been measured, and the values for the direct bandgap was significantly lower than those reported for other BFO‐based systems, being the lowest ∼1.87 eV for the Bi0.90La0.10FeO3composition. Results revealed a noteworthy effect of the defect concentrations induced by the lanthanum doping on the long‐range crystallinity and directly affecting the polarizability of the A–O bond as well as the Fe–O and Fe–O–Fe bond lengths in the perovskite structure. The enhanced optical absorption properties registered for the Bi1–
x Lax FeO3(x = 0–20) compositions make these perovskite multiferroic thin films as a potential candidate material for the high‐performance photovoltaic device applications. -
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Abstract Ferroelectric domain walls, topological entities separating domains of uniform polarization, are promising candidates as active elements for nanoscale memories. In such applications, controlled nucleation and stabilization of domain walls are critical. Here, using in situ transmission electron microscopy and phase‐field simulations, a controlled nucleation of vertically oriented 109° domain walls in (110)‐oriented BiFeO3(BFO) thin films is reported. In the switching experiment, reversed domains that are nucleated preferentially at the nanoscale edges of the “crest and sag” pattern‐like electrode under external bias subsequently grow into a stable stripe configuration. In addition, when triangular pockets (with an in‐plane polarization component) are present, these domain walls are pinned to form stable flux‐closure domains. Phase field simulations show that i) field enhancement at the edges of the electrode causes site‐specific domain nucleation, and ii) the local electrostatics at the domain walls drives the formation of flux closure domains, thus stabilizing the striped pattern, irrespective of the initial configuration. The results demonstrate how flux closure pinning can be exploited in conjunction with electrode patterning and substrate orientation to achieve a desired topological defect configuration. These insights constitute critical advancements in exploiting domain walls in next generation ferroelectronic devices.
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null (Ed.)A systematic study of (1− x )Pb(Fe 0.5 Nb 0.5 )O 3 – x BiFeO 3 ( x = 0–0.5) was performed by combining dielectric and electromechanical measurements with structural and microstructural characterization in order to investigate the strengthening of the relaxor properties when adding BiFeO 3 into Pb(Fe 0.5 Nb 0.5 )O 3 and forming a solid solution. Pb(Fe 0.5 Nb 0.5 )O 3 crystalizes in monoclinic symmetry exhibiting ferroelectric-like polarization versus electric field ( P–E ) hysteresis loop and sub-micron-sized ferroelectric domains. Adding BiFeO 3 to Pb(Fe 0.5 Nb 0.5 )O 3 favors a pseudocubic phase and a gradual strengthening of the relaxor behavior of the prepared ceramics. This is indicated by a broadening of the peak in temperature-dependent permittivity, narrowing of P–E hysteresis loops and decreasing size of ferroelectric domains resulting in polar nanodomains for x = 0.20 composition. The relaxor behavior was additionally confirmed by Vogel–Fulcher analysis. For the x ≥ 0.30 compositions, broad high-temperature anomalies are observed in dielectric permittivity versus temperature measurements in addition to the frequency-dispersive peak located close to room temperature. These samples also exhibit pinched P–E hysteresis loops. The observed pinching is most probably related to the reorganization of polar nanoregions under the electric field as shown by synchrotron X-ray diffraction measurements as well as by piezo-response force microscopy analysis, while in part affected by the presence of charged point defects and anti-ferroelectric order, as indicated from rapid cooling experiments and high-resolution transmission electron microscopy, respectively.more » « less
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/d0ra06775j
