LGT晶体高温电阻率与全矩阵材料系数表征

doi:10.15541/jim20230101

无机材料学报 ›› 2023, Vol. 38 ›› Issue (11): 1364-1370.DOI: 10.15541/jim20230101

LGT晶体高温电阻率与全矩阵材料系数表征

苏茂心¹^,²(), 李昕宸¹, 熊开南², 王升², 陈云琳¹(), 涂小牛²(), 施尔畏²

1.北京交通大学理学院, 应用微纳米材料研究所, 北京 100049
2.中国科学院上海硅酸盐研究所, 上海200050

收稿日期:2023-02-28 修回日期:2023-03-06 出版日期:2023-07-28 网络出版日期:2023-07-28
通讯作者: 陈云琳, 教授. E-mail: ylchen@bjtu.edu.cn;
涂小牛, 高级工程师. E-mail: xiaoniu_tu@mail.sic.ac.cn
作者简介:苏茂心(1994-), 男, 硕士研究生. E-mail: 1069016053@qq.com
基金资助:
国家重点研发计划(2022YFB3204000);国家自然科学基金重点项目(51832009)

Characterization of High Temperature Resistivity and Full Matrix Material Coefficient of LGT Crystals

SU Maoxin¹^,²(), LI Xinchen¹, XIONG Kainan², WANG Sheng², CHEN Yunlin¹(), TU Xiaoniu²(), SHI Erwei²

1. Institute of Applied Micro-Nano Materials, School of Science, Beijing Jiaotong University, Beijing 100049, China
2. Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China

Received:2023-02-28 Revised:2023-03-06 Published:2023-07-28 Online:2023-07-28
Contact: CHEN Yunlin, professor. E-mail: ylchen@bjtu.edu.cn;
TU Xiaoniu, senior engineer. E-mail: xiaoniu_tu@mail.sic.ac.cn
About author:SU Maoxin (1994-), male, Master candidate. E-mail: 1069016053@qq.com
Supported by:
National Key R&D Program of China(2022YFB3204000);National Natural Science Foundation of China(51832009)

摘要/Abstract

摘要：

基于声表面波(Surface acoustic wave, SAW)技术的无线无源器件是在极端条件下工作的首选传感器, 其中压电衬底在高温环境下的稳定性是影响SAW器件性能的关键因素。钽酸镓镧(LGT)晶体因电阻率高和稳定性好, 是SAW器件理想的高温压电衬底。为了全面评估LGT晶体的高温电阻率和材料系数稳定性, 本工作分别测试了纯LGT和掺铝钽酸镓镧(LGAT)晶体在氧气、氮气和氩气气氛中的高温电阻率, 并采用超声谐振谱(Resonant ultrasound spectroscopy, RUS)技术定征了纯LGT晶体高温全矩阵材料系数。电阻率测试结果显示, 在不同气氛下LGT晶体的高温导电行为明显不同, 纯LGT晶体在400~525 ℃范围内, 氮气中的电阻率最高; 在525~700 ℃范围内, 氩气中的电阻率最高, 700 ℃电阻率高达2.05×10⁶ Ω·cm; 而对于LGAT晶体, 在整个测试温度区间氮气中的电阻率均最高, 700 ℃电阻率达1.12×10⁶ Ω·cm, 略低于纯LGT晶体。高温全矩阵材料系数测试结果显示, 室温~400 ℃范围内, LGT晶体的电弹性能稳定, 随着温度升高, 弹性系数略有降低, 而压电系数d₁₁几乎保持不变。以上结果表明, LGT晶体在高温下具有非常高的电阻率和材料稳定性, 适合作为压电衬底用于制备高温压电器件。本工作的研究结果为LGT基高温压电器件的设计与制备奠定了基础。

关键词: 钽酸镓镧, 高温电阻率, 封装气氛, 高温材料系数

Abstract:

Wireless passive devices based on surface acoustic wave (SAW) technology are the firstly selected sensors in extreme conditions, and high temperature stability of piezoelectric substrates is the key factor limiting the performance of SAW devices. Langatate (LGT) crystal is an ideal high temperature piezoelectric substrate for SAW devices due to high resistivity and stability. The high temperature resistivity of pure LGT and aluminum- doped langatate (LGAT) crystals in oxygen, nitrogen and argon atmosphere were characterized, and the high temperature full matrix material coefficient of pure LGT crystal was characterized by ultrasonic resonance spectroscopy (RUS) technology. The results show that conductive behavior of LGT crystal under high temperature were significantly varied when tested in different atmospheres. The pure LGT crystal in nitrogen has the highest resistivity in the temperature range of 400-525 ℃, and in argon has highest resistivity between 525 ℃ and 700 ℃, with resistivity up to 2.05×10⁶ Ω·cm at 700 ℃. However, LGAT crystal in nitrogen has the highest resistivity in the whole test temperature range, with a resistivity of 1.12×10⁶ Ω·cm at 700 ℃, compared to pure LGT crystal. The elastic and piezoelectric properties of LGT crystal are very stable from room temperature to 400 ℃ according to RUS analysis results. As the temperature rises, the elastic coefficient decreases slightly, while the piezoelectric coefficient d₁₁ is remained almost unchanged. In conclusion, LGT crystal has very high resistivity and stability at high temperature so that it is suitable to be used as piezoelectric substrate for fabricating high temperature piezoelectric devices, shedding light on the design and fabrication of LGT-based high temperature piezoelectric devices.

Key words: langatate, high temperature resistivity, encapsulation atmosphere, high temperature material coefficient

中图分类号:

TQ174

苏茂心, 李昕宸, 熊开南, 王升, 陈云琳, 涂小牛, 施尔畏. LGT晶体高温电阻率与全矩阵材料系数表征[J]. 无机材料学报, 2023, 38(11): 1364-1370.

SU Maoxin, LI Xinchen, XIONG Kainan, WANG Sheng, CHEN Yunlin, TU Xiaoniu, SHI Erwei. Characterization of High Temperature Resistivity and Full Matrix Material Coefficient of LGT Crystals[J]. Journal of Inorganic Materials, 2023, 38(11): 1364-1370.

图/表 9

参考文献 19

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Atmosphere	T /℃	E_a(LGT)/eV	E_a(LGAT)/eV
Oxygen	400-500	1.14	0.99
Oxygen	525-650	1.05	0.99
Nitrogen	400-550	1.0	0.95
Nitrogen	550-700	1.36	1.26
Argon	400-700	0.84	0.91

Atmosphere	T /℃	E_a(LGT)/eV	E_a(LGAT)/eV
Oxygen	400-500	1.14	0.99
Oxygen	525-650	1.05	0.99
Nitrogen	400-550	1.0	0.95
Nitrogen	550-700	1.36	1.26
Argon	400-700	0.84	0.91

T/℃	$\varepsilon _{11}^{\text{S}}/{{\varepsilon }_{0}}$	$\varepsilon _{33}^{\text{S}}/{{\varepsilon }_{0}}$
20	18.6	75.9
400	19.8	59.7

T/℃	$\varepsilon _{11}^{\text{S}}/{{\varepsilon }_{0}}$	$\varepsilon _{33}^{\text{S}}/{{\varepsilon }_{0}}$
20	18.6	75.9
400	19.8	59.7

T/℃	Elastic coefficient/(×10¹⁰, N·m^-2)						Piezoelectric coefficient/(C·m^-2)
T/℃	$c_{11}^{\text{E}}$	$c_{12}^{\text{E}}$	$\text{ }\!\!~\!\!\text{ }c_{13}^{\text{E}}$	$c_{14}^{\text{E}}$	$c_{33}^{\text{E}}$	$c_{44}^{\text{E}}$	${{e}_{11}}$	${{e}_{14}}$
20	18.586	10.524	9.785	1.353	26.003	5.093	-0.439	0.123
400	18.346	10.314	9.694	1.256	25.340	5.056	-0.429	0.209

LGT晶体高温电阻率与全矩阵材料系数表征

Characterization of High Temperature Resistivity and Full Matrix Material Coefficient of LGT Crystals

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$c_{ij}^{\text{E}}$/(×10¹⁰, N·m^–2)								$c_{ij}^{\text{D}}$/(×10¹⁰, N·m^–2)
$c_{11}^{\text{E}}$	$c_{12}^{\text{E}}$		$c_{13}^{\text{E}}$	$c_{14}^{\text{E}}$	$c_{33}^{\text{E}}$		$c_{44}^{\text{E}}$	$c_{11}^{\text{D}}$	$c_{12}^{\text{D}}$		$c_{\text{13}}^{\text{D}}$	$c_{\text{14}}^{\text{D}}$	$c_{\text{33}}^{\text{D}}$			$c_{\text{44}}^{\text{D}}$
18.586	10.524		9.785	1.353	26.003		5.093	18.703	10.406		9.785	1.320	26.003			5.102
$s_{ij}^{\text{E}}$/(×10^–12, m²·N^–1)								$s_{ij}^{\text{D}}$/(×10^–12, m²·N^–1)
$s_{\text{11}}^{\text{E}}$	$s_{\text{12}}^{\text{E}}$		$s_{\text{13}}^{\text{E}}$	$s_{\text{14}}^{\text{E}}$	$s_{\text{33}}^{\text{E}}$		$s_{\text{44}}^{\text{E}}$	$s_{\text{11}}^{\text{D}}$	$s_{\text{12}}^{\text{D}}$		$s_{\text{13}}^{\text{D}}$	$s_{\text{14}}^{\text{D}}$		$s_{\text{33}}^{\text{D}}$		$s_{\text{44}}^{\text{D}}$
9.108	-4.509		-1.731	-3.617	5.148		21.56	8.866	-4.268		-1.731	-3.397		5.148		21.36
${{e}_{ij}}$/(C·m^–2)								${{d}_{ij}}$/(×10^–12, C·N^–1)
${{e}_{11}}$				${{e}_{14}}$				${{d}_{11}}$				${{d}_{14}}$
-0.439				0.123				-6.43				5.83
${{g}_{ij}}$/(×10^–2, ${{\text{V}}_{m}}$·N^–1)								${{h}_{ij}}$/(×10⁸, V·m^–1)
${{g}_{11}}$				${{g}_{14}}$				${{h}_{11}}$				${{h}_{14}}$
-3.903				3.543				-26.67				7.482
$\varepsilon _{ij}^{\text{T}}$ (ε₀)				$\varepsilon _{ij}^{\text{S}}$ (ε₀)				$\beta _{ij}^{\text{T}}$ (×10^–4 /ε₀)				$\beta _{ij}^{\text{S}}$(×10^–4/ε₀)
$\varepsilon _{\text{11}}^{\text{T}}$		$\varepsilon _{\text{33}}^{\text{T}}$		$\varepsilon _{\text{11}}^{\text{S}}$		$\varepsilon _{\text{33}}^{\text{S}}$		$\beta \ _{\text{11}}^{\text{T}}$		$\beta _{\text{33}}^{\text{T}}$		$\beta \ _{\text{11}}^{\text{S}}$			$\beta _{\text{33}}^{\text{S}}$
19.3		75.9		18.6		75.9		518		132		538			132

$c_{ij}^{\text{E}}$/(×10¹⁰, N·m^–2)								$c_{ij}^{\text{D}}$/(×10¹⁰, N·m^–2)
$c_{\text{11}}^{\text{E}}$	$c_{\text{12}}^{\text{E}}$		$c_{\text{13}}^{\text{E}}$	$c_{\text{14}}^{\text{E}}$	$c_{\text{33}}^{\text{E}}$		$c_{\text{44}}^{\text{E}}$	$c_{\text{11}}^{\text{D}}$	$c_{\text{12}}^{\text{D}}$		$c_{\text{13}}^{\text{D}}$	$c_{\text{14}}^{\text{D}}$	$c_{\text{33}}^{\text{D}}$		$c_{\text{44}}^{\text{D}}$
18.346	10.314		9.694	1.256	25.340		5.056	18.451	10.209		9.694	1.205	25.340		5.081
$s_{ij}^{\text{E}}$/(×10^-12, m²·N^–1)								$s_{ij}^{\text{D}}$/(×10^-12, m²·N^–1)
$s_{\text{11}}^{\text{E}}$	$s_{\text{12}}^{\text{E}}$		$s_{\text{13}}^{\text{E}}$	$s_{\text{14}}^{\text{E}}$	$s_{\text{33}}^{\text{E}}$		$s_{\text{44}}^{\text{E}}$	$s_{\text{11}}^{\text{D}}$	$s_{\text{12}}^{\text{D}}$		$s_{\text{13}}^{\text{D}}$	$s_{\text{14}}^{\text{D}}$	$s_{\text{33}}^{\text{D}}$		$s_{\text{44}}^{\text{D}}$
9.103	-4.396		-1.801	-3.353	5.324		21.44	8.873	-4.165		-1.801	-3.092	5.324		21.15
${{e}_{ij}}$/(C·m^–2)								${{d}_{ij}}$/(×10^–12, C·N^–1)
e₁₁				e₁₄				d₁₁				d₁₄
-0.429				0.209				-6.48				7.34
${{g}_{ij}}$/(×10^–2, ${{\text{V}}_{m}}$·N^–1)								${{h}_{ij}}$/(×10⁸, V·m^–1)
g₁₁				g₁₄				h₁₁				h₁₄
-3.699				4.190				-24.45				11.89
$\varepsilon _{ij}^{\text{T}}$ (ε₀)				$\varepsilon _{ij}^{\text{S}}$ (ε₀)				$\beta _{ij}^{\text{T}}$ (×10^–4/ε₀)				$\beta _{ij}^{\text{S}}$ (×10^–4/ε₀)
$\varepsilon _{11}^{\text{T}}$		$\varepsilon _{33}^{\text{T}}$		$\varepsilon _{11}^{\text{S}}$		$\varepsilon _{33}^{\text{S}}$		$\beta _{11}^{\text{T}}$		$\beta _{33}^{\text{T}}$		$\beta \ _{11}^{\text{S}}$		$\beta _{33}^{\text{S}}$
20.6		59.7		19.8		59.7		485		168		505		168