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<p>Potassium sodium niobate (K<sub>0.5</sub>Na<sub>0.5</sub>NbO<sub>3</sub>, KNN) single crystals fabricated via the seed-free solid-state crystal growth (SFSSCG) method were previously shown to exhibit excellent comprehensive properties, warranting further systematic investigation. In this study, Cu, Bi, and Ga-co-doped KNN lead-free piezoelectric single crystals were successfully grown using the SFSSCG technique. The role of CuO doping concentration in modulating the crystal structure and electromechanical properties of (1-<i>x</i>)(0.996KNN–0.004BiGaO<sub>3</sub>)-<i>x</i>CuO single crystals were systematically investigated. The results demonstrated that the incorporation of an appropriate amount of CuO into 0.996KNN–0.004BiGaO<sub>3</sub> single crystals effectively enhanced the overall electrical performance of KNN-based materials. Moderate CuO doping (0 ≤ <i>x</i> ≤ 0.009) was found to improve crystal growth conditions by facilitating liquid-phase-assisted sintering, enabling the growth of high-quality single crystals with a maximum size of 21 × 22 × 2 mm<sup>3</sup>. Among all compositions, the crystal with <i>x</i> = 0.003 exhibited the optimal comprehensive electrical performance, delivering a piezoelectric coefficient (<i>d</i><sub><i>33</i></sub>) of 580 pC/N, maximum effective piezoelectric response (<InlineEquation ID="IEq1"> <EquationSource Format="TEX">\({d}_{33}^{*}\)</EquationSource> <EquationSource Format="MATHML"><math> <mmultiscripts> <mi>d</mi> <mrow> <mn>33</mn> </mrow> <mrow> <mrow /> <mo>∗</mo> </mrow> </mmultiscripts> </math></EquationSource> </InlineEquation>) of 1208&#xa0;pm/V, a remanent polarization (<i>P</i><sub><i>r</i></sub>) of 42.5 μC/cm<sup>2</sup>, a mechanical quality factor (<i>Q</i><sub><i>m</i></sub>) of 58, and an electromechanical coupling factor (<i>k</i><sub><i>t</i></sub>) of 0.40. In addition, a high Curie temperature (<i>T</i><sub><i>C</i></sub>) of 405&#xa0;°C, a relative permittivity (<i>Ɛ</i><sub><i>r</i></sub>) of 361, and a low dielectric loss (<i>tanδ</i>) of 0.021 were achieved. These findings confirmed that CuO-assisted multi-element doping is an effective strategy for optimizing the electrical properties of KNN-based piezoelectric single crystals.</p>

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Effects of CuO doping on the crystal growth, structural characteristics, and electrical properties of lead-free K0.5Na0.5NbO3–BiGaO3 single crystals

  • 期刊论文

  • 发表日期：

    2026年4月8日

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  • Zerong Chen,
  • Minhong Jiang,
  • Wenqi Wei,
  • Yiming Di,
  • Shousong Yan,
  • Tong Li,
  • Guanghui Rao

摘要

Potassium sodium niobate (K0.5Na0.5NbO3, KNN) single crystals fabricated via the seed-free solid-state crystal growth (SFSSCG) method were previously shown to exhibit excellent comprehensive properties, warranting further systematic investigation. In this study, Cu, Bi, and Ga-co-doped KNN lead-free piezoelectric single crystals were successfully grown using the SFSSCG technique. The role of CuO doping concentration in modulating the crystal structure and electromechanical properties of (1-x)(0.996KNN–0.004BiGaO3)-xCuO single crystals were systematically investigated. The results demonstrated that the incorporation of an appropriate amount of CuO into 0.996KNN–0.004BiGaO3 single crystals effectively enhanced the overall electrical performance of KNN-based materials. Moderate CuO doping (0 ≤ x ≤ 0.009) was found to improve crystal growth conditions by facilitating liquid-phase-assisted sintering, enabling the growth of high-quality single crystals with a maximum size of 21 × 22 × 2 mm3. Among all compositions, the crystal with x = 0.003 exhibited the optimal comprehensive electrical performance, delivering a piezoelectric coefficient (d33) of 580 pC/N, maximum effective piezoelectric response ( \({d}_{33}^{*}\) d 33 ∗ ) of 1208 pm/V, a remanent polarization (Pr) of 42.5 μC/cm2, a mechanical quality factor (Qm) of 58, and an electromechanical coupling factor (kt) of 0.40. In addition, a high Curie temperature (TC) of 405 °C, a relative permittivity (Ɛr) of 361, and a low dielectric loss (tanδ) of 0.021 were achieved. These findings confirmed that CuO-assisted multi-element doping is an effective strategy for optimizing the electrical properties of KNN-based piezoelectric single crystals.