Structure, defects, and microwave dielectric properties of Al-doped and Al/Nd co-doped Ba4Nd9.33Ti18O54 ceramics

Abstract

Abstract Low-loss tungsten-bronze microwave dielectric ceramics are dielectric materials with potential application value for miniaturized dielectric filters and antennas in the fifth-generation (5G) communication technology. In this work, a novel Al/Nd co-doping method of Ba 4 Nd 9.33 Ti 18 O 54 (BNT) ceramics with a chemical formula of Ba 4 Nd 9.33+ z /3 Ti 18− z Al z O 54 (BNT-AN, 0 ⩽ z ⩽ 2) was proposed to improve the dielectric properties through structural and defect modulation. Together with Al-doped ceramics (Ba 4 Nd 9.33 Ti 18− z Al 4 z /3 O 54 , BNT-A, 0 ⩽ z ⩽ 2) for comparison, the ceramics were prepared by a solid state method. It is found that Al/Nd co-doping method has a significant effect on improving the dielectric properties compared with Al doping. As the doping amount z increased, the relative dielectric constant ( ε r ) and the temperature coefficient of resonant frequency ( τ f ) of the ceramics decreased, and the Q×f values of the ceramics obviously increased when z ⩽ 1.5. Excellent microwave dielectric properties of ε r = 72.2, Q×f = 16,480 GHz, and τ f = +14.3 ppm/°C were achieved in BNT-AN ceramics with z = 1.25. Raman spectroscopy and thermally stimulated depolarization current (TSDC) technique were firstly combined to analyze the structures and defects in microwave dielectric ceramics. It is shown that the improvement on Q×f values was originated from the decrease in the strength of the A-site cation vibration and the concentration of oxygen vacancies ( $${\rm{V}}_{\rm{O}}^{ \cdot \cdot }$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:msubsup> <mml:mtext>V</mml:mtext> <mml:mtext>O</mml:mtext> <mml:mrow> <mml:mo>⋅</mml:mo> <mml:mo>⋅</mml:mo> </mml:mrow> </mml:msubsup> </mml:mrow> </mml:math> ), demonstrating the effect and mechanism underlying for structural and defect modulation on the performance improvement of microwave dielectric ceramics.