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<p>Dielectrics with high permittivity, low dielectric loss, and good temperature stability are crucial for electronic components to meet the ever-increasing application demands. However, challenges remain in further optimizing dielectric properties due to the correlation between these parameters. Here, we propose a chemical bonding engineering strategy in high-entropy CaTiO<sub>3</sub> ceramics and realize colossal permittivity with low loss and excellent stability. Our results reveal that the high-concentration oxygen vacancy (<InlineEquation ID="IEq1"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="41467_2025_59226_Article_IEq1.gif" Format="GIF" Height="18" Rendition="HTML" Resolution="72" Type="Linedraw" Width="23" /> </InlineMediaObject> <EquationSource Format="TEX">\({{{\rm{V}}}}_{{{\rm{O}}}}^{\cdot \cdot }\)</EquationSource> <EquationSource Format="MATHML"><math> <msubsup> <mrow> <mi mathvariant="normal">V</mi> </mrow> <mrow> <mi mathvariant="normal">O</mi> </mrow> <mrow> <mo>⋅</mo> <mo>⋅</mo> </mrow> </msubsup> </math></EquationSource> </InlineEquation>)-related defects and the decreased activation energy of grain/grain boundary led to a colossal permittivity dielectric behavior, which should be ascribed to the weakened chemical bonding and the reduced formation energy of defects confirmed by our first-principles calculation. Consequently, in the high-entropy CaTiO<sub>3</sub> ceramic, a permittivity of 2.37 × 10<sup>5</sup>, low loss of 0.005, and good temperature stability (&lt;± 15%) in -50–250 °C are simultaneously achieved. This finding implies that chemical bonding engineering may be a promising strategy for designing colossal permittivity materials and provides a broad opportunity for the development of other defect-dependent functional materials.</p>

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Colossal permittivity in high-entropy CaTiO3 ceramics by chemical bonding engineering

  • 期刊论文

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  • 发表日期：

    2025年4月29日

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  • Jinghan Cai,
  • Shun Lan,
  • Bin Wei,
  • Junlei Qi,
  • Ce-Wen Nan,
  • Yuan-Hua Lin

摘要

Dielectrics with high permittivity, low dielectric loss, and good temperature stability are crucial for electronic components to meet the ever-increasing application demands. However, challenges remain in further optimizing dielectric properties due to the correlation between these parameters. Here, we propose a chemical bonding engineering strategy in high-entropy CaTiO3 ceramics and realize colossal permittivity with low loss and excellent stability. Our results reveal that the high-concentration oxygen vacancy ( \({{{\rm{V}}}}_{{{\rm{O}}}}^{\cdot \cdot }\) V O ⋅ ⋅ )-related defects and the decreased activation energy of grain/grain boundary led to a colossal permittivity dielectric behavior, which should be ascribed to the weakened chemical bonding and the reduced formation energy of defects confirmed by our first-principles calculation. Consequently, in the high-entropy CaTiO3 ceramic, a permittivity of 2.37 × 105, low loss of 0.005, and good temperature stability (<± 15%) in -50–250 °C are simultaneously achieved. This finding implies that chemical bonding engineering may be a promising strategy for designing colossal permittivity materials and provides a broad opportunity for the development of other defect-dependent functional materials.