High-performance colossal permittivity behaviour persists to ultralow temperature in Co+Ta co-doped SnO2: A spin-defect mediated superstable large electronic moment of defect-dipole

Dong, Wen; Tian, Fan; Ma, Qi; Jiang, Dequan; Seddon, Samuel D.; Xia, Zhengcai; Bakhtiar, Syed ul Hasnain; Liu, Miao; Fu, Qiuyun

doi:10.1016/j.actamat.2021.116965

Cited by 12 publications

(10 citation statements)

References 40 publications

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“…% have been synthesized, where above room temperature ferromagnetic (FM) behavior was observed. − However, antiferromagnetic (AFM) behavior has also been reported in Co-doped t-TiO 2 as well as in Fe-doped cases with doping levels below 25 and 4.6 at. %, respectively. , Ogale et al reported a giant magnetic moment in Co-doped t-SnO 2 , while both Liu et al and our group have reported obvious AFM behavior in Co-doped SnO 2 , with a doping level of ∼5 at. %.…”

Section: Introductionsupporting

confidence: 43%

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Decisive Role of the Defect-Clustering Effect in the Variation of Magnetic Order in Diluted Magnetic Binary Metal Oxides

Bakhtiar,

Ai,

Dong

et al. 2023

J. Phys. Chem. C

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Above room temperature T c, magnetism is becoming viable in diluted magnetic semiconductors, which show different magnetic orders, depending on the dopant type and their fabrication method. However, how the defects can influence the magnetic properties remains unclear at the atomic level. In this article, by taking the Co-doped tetragonal MO2 (t-MO2, M = Ti, Sn, Hf, and Zr) as an example, the density functional theory-based investigations show that the magnetic order is mainly decided by the defect clustering effect, following a “defect-distance-based” defect correlation principle. It is found that the distance between two defects (Co–Co) leads to an alteration of magnetic order, where SnO2 and ZrO2 show antiferromagnetic (AFM) behavior when the nearest Co–Co distance lies within one octahedron, while a larger distance gives rise to the ferromagnetic (FM) state. In contrast, TiO2 exhibits an AFM state at the neighboring Co–Co configuration with the nearest Co–Co distance larger than one octahedra, while HfO2 showed an opposite trend as that of TiO2. Furthermore, the position of oxygen vacancies mainly affects the magnitude of magnetization instead of magnetic order. We believe this work would significantly advances the understanding of defect chemistry and condensed matter physics related to diluted FM-AFM systems.

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Section: Introductionsupporting

confidence: 43%

“…%, respectively. 22,23 Ogale et al reported a giant magnetic moment in Co-doped t-SnO 2 , 24 while both Liu et al 25 and our group 26 have reported obvious AFM behavior in Co-doped SnO 2 , with a doping level of ∼5 at. %.…”

Section: Introductionmentioning

confidence: 57%

Decisive Role of the Defect-Clustering Effect in the Variation of Magnetic Order in Diluted Magnetic Binary Metal Oxides

Bakhtiar,

Ai,

Dong

et al. 2023

J. Phys. Chem. C

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“…The obvious flattened dielectric temperature spectrum of the sample La 0.01 Mn 0.01 proves the relaxation enhancement. Moreover, these defect dipoles in A–B site are suggested to further suppress the long-range order and shrink the domain size, leading to an improved polarization strength . Compared with the overall lower P max of the La or Mn only-doped PBLZST, , the at least two-time improvement of P max in La 0.01 Mn 0.01 confirms the significant polarization contribution of the defect-dipole clusters.…”

Section: Resultsmentioning

confidence: 80%

Enhanced Energy Storage Performance by A–B Site Ambipolar Co-Doping in Antiferroelectrics

Dong

Yang

et al. 2023

ACS Appl. Mater. Interfaces

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Antiferroelectric materials are promising to be used for power capacitive devices. To improve the energy storage performance, solid-solution and defect engineering are widely used to suppress the long-range order by introducing local heterogeneities. However, both methods generally deteriorate either the maximum polarization or breakdown electric field due to damaged intrinsic polarization or increased leakage. Here, we show that forming defect-dipole clusters by A−B site acceptor−donor co-doping in antiferroelectrics can comprehensively enhance the energy storage performance. We took the La−Mn co-doped (Pb 0.9 Ba 0.04 La 0.04 )(Zr 0.65 Sn 0.3 Ti 0.05 )O 3 (PBLZST) as an example. For co-doping with unequal amounts, high dielectric loss, impurity phase, and decreased polarization were observed. By contrast, La and Mn in an equal amount of co-doping can significantly improve the overall energy storage performance. An over 48% increasement in both the maximum polarization (62.7 μC/cm 2 ) and breakdown electric field (242.6 kV/cm) was obtained in 1 mol % La and 1 mol % Mn equally co-doped PBLZST, followed by a nearly two-time enhancement in W rec (6.52 J/cm 3 ) compared with that of the pure matrix. Moreover, a high energy storage efficiency of 86.3% with an enhanced temperature stability over a wide temperature range can be achieved. The defect-dipole clusters associated with charge-compensated co-doping are suggested to contribute to an enhanced dielectric permittivity, linear polarization behavior, and maximum polarization strength compared with that of the unequal co-doping cases. The defect-dipole clusters are suggested to couple with the host, leading to a high energy storage performance. The proposed strategy is believed to be applicable to modify the energy storage behavior of antiferroelectrics.

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“…Therefore, the design and development of material systems with both high dielectric constant and low loss is a research hot spot in the field of dielectric materials. 17–20…”

Section: Introductionmentioning

confidence: 99%

“…Therefore, the design and development of material systems with both high dielectric constant and low loss is a research hot spot in the field of dielectric materials. [17][18][19][20] In 2013, a very promising candidate of donor and acceptor codoped rutile TiO 2 ceramics was found to possess unexpected ultrahigh permittivity and lower dielectric loss (e B 6 Â 10 4 , tan d o 0.05, 10 2 -10 6 Hz). 21 The author claims that the superior CP performance can be attributed to the electron-pinned defect dipole (EPDD) constructed by the diamond shape (Nb 2 5+ Ti 3+ A Ti , A = Ti 3+ /In 3+ /Ti 4+ ) and the triangular In 2 3þ V O Ti 3þ À Á coordination structure, which enable electrons to exist in the highly localized state.…”

Section: Introductionmentioning

confidence: 99%

The origin of dielectric relaxation behavior in TiO₂ based ceramics co-doped with Zn²⁺, W⁶⁺ ions under a N₂/O₂ sintering atmosphere

Zhou

Yang

Yang³

et al. 2023

Phys. Chem. Chem. Phys.

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High-performance colossal permittivity behaviour persists to ultralow temperature in Co+Ta co-doped SnO2: A spin-defect mediated superstable large electronic moment of defect-dipole

Cited by 12 publications

References 40 publications

Decisive Role of the Defect-Clustering Effect in the Variation of Magnetic Order in Diluted Magnetic Binary Metal Oxides

Decisive Role of the Defect-Clustering Effect in the Variation of Magnetic Order in Diluted Magnetic Binary Metal Oxides

Enhanced Energy Storage Performance by A–B Site Ambipolar Co-Doping in Antiferroelectrics

The origin of dielectric relaxation behavior in TiO₂ based ceramics co-doped with Zn²⁺, W⁶⁺ ions under a N₂/O₂ sintering atmosphere

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High-performance colossal permittivity behaviour persists to ultralow temperature in Co+Ta co-doped SnO2: A spin-defect mediated superstable large electronic moment of defect-dipole

Cited by 12 publications

References 40 publications

Decisive Role of the Defect-Clustering Effect in the Variation of Magnetic Order in Diluted Magnetic Binary Metal Oxides

Decisive Role of the Defect-Clustering Effect in the Variation of Magnetic Order in Diluted Magnetic Binary Metal Oxides

Enhanced Energy Storage Performance by A–B Site Ambipolar Co-Doping in Antiferroelectrics

The origin of dielectric relaxation behavior in TiO2 based ceramics co-doped with Zn2+, W6+ ions under a N2/O2 sintering atmosphere

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The origin of dielectric relaxation behavior in TiO₂ based ceramics co-doped with Zn²⁺, W⁶⁺ ions under a N₂/O₂ sintering atmosphere