Aging behavior in single-domain Mn-doped ${\mathrm{BaTiO}}_{3}$ crystals: Implication for a unified microscopic explanation of ferroelectric aging

Aging behavior in single-domain Mn-doped ${BaTiO}_{3}$ crystals: Implication for a unified microscopic explanation of ferroelectric aging

Lixue Zhang and Xiaobing Ren

Phys. Rev. B 73, 094121 – Published 24 March 2006

Abstract

The change of ferroelectric, dielectric, and piezoelectric properties with time, the ferroelectric aging phenomena, has been observed in most ferroelectrics. Phenomenologically, aging can be attributed to the gradual stabilization of ferroelectric domains by defects, but the microscopic origin of the domain stabilization has remained controversial. It is unclear whether the domain stabilization is a boundary effect (caused by domain-wall-pinning) or a volume effect (stabilization of the whole domain). In the present paper, we made a single-domain (domain-wall-free) Mn-doped ${BaTiO}_{3}$ single crystal and studied the aging behavior of its hysteresis loop. We found that after aging, the single-domain sample shows a significant increase in the coercive field, clearly indicating a strong stabilization of the single domain. Furthermore, the sample exhibits an abnormal double hysteresis loop, which corresponds to an interesting reversible domain switching process. These are direct evidence for the stabilization of single domain by aging. Our results preclude any explanation by the domain-wall-pinning effect and strongly suggest that the volume effect is the governing mechanism for the aging in hysteresis loop. We further show that the microscopic origin of the volume effect comes naturally from a general symmetry-conforming property of point defects. Such a microscopic mechanism can explain not only the aging in hysteresis loop (large signal aging) but also the aging in dielectric and piezoelectric constants (small signal aging), thus providing a unified microscopic explanation for all kinds of ferroelectric aging.

Received 31 October 2005

DOI:https://doi.org/10.1103/PhysRevB.73.094121

Authors & Affiliations

Lixue Zhang^1,2,3 and Xiaobing Ren^1,2,*

¹Multi-Disciplinary Materials Research Center, Xi’an Jiaotong University, Xi’an 710049, People’s Republic of China
²Materials Physics Group, National Institute for Materials Science, Tsukuba, 305-0047 Ibaraki, Japan
³State Key Laboratory for Mechanical Behavior of Materials, Xi’an Jiaotong University, Xi’an 710049, People’s Republic of China

^*Corresponding author. Electronic mail: ren.xiaobing@nims.go.jp

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Vol. 73, Iss. 9 — 1 March 2006

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Figure 1
A Mn-doped ${BaTiO}_{3}$ single crystal is poled with an applied electric field $E$ along $⟨ 001 ⟩$ (thickness direction) (a). As the result the sample became a single domain (b). Then it was aged for two weeks without $E$ . When $E$ is applied along $⟨ 100 ⟩$ (transverse direction, perpendicular to $P_{S}$ ) to the aged single-domain sample (c), it shows a double hysteresis loop with a large coercive field $E_{C}$ , which is contrasting with the normal hysteresis loop in the unaged state (left-top inset).Reuse & Permissions
Figure 2
Interesting reversible domain switching behavior during electric field cycling in an aged single-domain $Mn − {BaTiO}_{3}$ crystal. The crystal was poled to the single-domain state along [001] (thickness direction, along which microscopy observation was made). The typical micrographs correspond to forward electric field (along [100] direction) of $E = 0$ , 1.5, $3 kV ∕ mm$ and reverse field $E = 1.5$ , $0 kV ∕ mm$ , respectively. For the whole process, see video at our website (Ref. 26).Reuse & Permissions
Figure 3
Schematic explanation for defect-symmetry principle in single-domain $Mn − {BaTiO}_{3}$ crystals (a) and its explanation on aging induced reversible domain switching (a)–(c). As shown in (a), the short-range-order distribution of oxygen vacancies next to a given dopant ${Mn}^{3 +}$ ion shows tetragonal symmetry after aging at the ferroelectric state, conforming to tetragonal crystal symmetry. Defect (crystal) symmetry is represented by a large (small) rectangle, respectively. $P_{S}$ and defect polarization $P_{D}$ are represented by a thick and thin arrow, respectively. When electric field $E$ is applied (a), $P_{S}$ is switched [see the multidomain at intermediate $E$ (b) and single domain at high $E$ (c)], while $P_{D}$ cannot be rotated and thus favored a reverse domain switching. This causes the stabilization of the original single domain (see Fig. 2), and thus generating a double hysteresis loop as shown in Fig. 1.Reuse & Permissions
Figure 4
Domain-wall motion under AC electric field $E$ or mechanical stress $Z$ (for dielectric constant $ε$ or piezoelectric constant $d$ measurement) for unaged (a) and aged (b) samples, respectively. This motion induces a change of polarization $Δ P_{d w}$ , which gives extrinsic contribution to $ε$ and $d$ . (a) Without aging, $Δ P_{d w}$ is larger because defect symmetry is cubic and it does not restrict domain-wall motion; thus a larger $ε$ and $d$ is observed. However, (b) after aging, $Δ P_{d w}$ becomes smaller. This is because the appearance of the $P_{D}$ (following $P_{S}$ according to the defect-symmetry principle), which stabilizes the existing domain configuration. As a result, the domain-wall response to an external field becomes less. This explains the decrease of $ε$ and $d$ after aging.Reuse & Permissions

Physical Review B

covering condensed matter and materials physics

Aging behavior in single-domain Mn-doped ${BaTiO}_{3}$ crystals: Implication for a unified microscopic explanation of ferroelectric aging

Lixue Zhang and Xiaobing Ren

Phys. Rev. B 73, 094121 – Published 24 March 2006

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Physical Review B

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Aging behavior in single-domain Mn-doped BaTiO3 crystals: Implication for a unified microscopic explanation of ferroelectric aging

Lixue Zhang and Xiaobing Ren

Phys. Rev. B 73, 094121 – Published 24 March 2006

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Aging behavior in single-domain Mn-doped ${BaTiO}_{3}$ crystals: Implication for a unified microscopic explanation of ferroelectric aging