应变增强Nb掺杂SrTiO<sub>3</sub>薄膜热电性能

马云鹏; 庄华鹭; 李敬锋; 李千

doi:10.7498/aps.72.20222301

摘要

高性能热电材料的发展有望帮助解决未来能源危机, 且随着可穿戴器件的发展与应用, 热电材料和器件除了要具备更高的热-电转化性能以外, 还必须具有良好的柔性. 将热电材料制成薄膜既可以为微型器件供电, 也有潜力应用于柔性器件. 本文使用脉冲激光沉积方法, 在商用SrTiO₃ (STO)和La_0.3Sr_0.7Al_0.65Ta_0.35O₃ (LSAT)衬底上制备得到了不同厚度的高质量铌掺杂钛酸锶薄膜(Nb:STO), 并对薄膜的表面形貌、结构以及热电性能进行表征与测试. 结果显示, 使用LSAT作为衬底可以对薄膜施加面内压应变, 随着薄膜厚度的增大, 应变逐渐释放并接近于块体Nb:STO. 随着厚度的增大, 薄膜的热电性能逐渐提升, 在STO衬底上生长的208 nm厚样品的室温功率因子相比于52 nm样品提升了187%. 此外, 144 nm厚度的Nb:STO/LSAT薄膜室温塞贝克系数达到了265.95 μV/K, 这是由于衬底应变导致薄膜样品的能带变化. 本工作表明通过应变工程调控铌掺杂钛酸锶薄膜热电性能的可行性, 为后续提高此类薄膜材料的热电性能提供了一种新思路.

关键词:

脉冲激光沉积 /
热电 /
钛酸锶 /
薄膜

Abstract

The development of high-performance thermoelectric materials can help solve the energy crisis in the future. Thin-film thermoelectric materials can meet the requirement for flexibility of wearable devices while supplying electrical power to them. In this study, high-quality Nb-doped SrTiO₃ films (Nb:STO) with different thickness are prepared on SrTiO₃ (STO) and La_0.3Sr_0.7Al_0.65Ta_0.35O₃ (LSAT) substrates by pulsed laser deposition. The surface morphologies, crystal structures, and thermoelectric performances of the films are characterized. The results show that the thermoelectric performance of the strain-free film increase with thickness increasing. The power factor at room temperature increases by 187%. The Seebeck coefficient of the 144 nm-thick Nb:STO/LSAT sample with strain is greatly improved to $265.95\;{\text{μ}}{\rm{V}}/{\rm{K}}$ at room temperature, which is likely to be due to the strain induced changes in the energy band of the thin film. The improvement of the thermoelectric performances of Nb:STO thin films by strain engineering provides a new approach to improving the thermoelectric properties of oxide thin films.

Keywords:

作者及机构信息

清华大学材料学院, 新型陶瓷与精细工艺国家重点实验室, 北京　100084

通信作者: 李千, qianli_mse@tsinghua.edu.cn

基金项目: 国家重点研发计划(批准号: 2020YFA0309100)和国家自然科学基金委原创探索计划(批准号: 52150092)资助的课题.

Authors and contacts

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China

Corresponding author: Li Qian, qianli_mse@tsinghua.edu.cn

Funds: Project supported by the National Key Research and Development Program of China (Grant No. 2020YFA0309100) and the National Natural Science Foundation of China(Grant No. 52150092).

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参考文献

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施引文献

图 1 不同厚度Nb:STO/STO薄膜生长状况表征　(a) XRD谱; (b) AFM形貌图; (c) EDS, 插表为原子摩尔比

Fig. 1. Characterization of Nb doped SrTiO₃ thin films on (001) SrTiO₃ substrates with different thicknesses: (a) XRD spectrum; (b) AFM image; (c) EDS, the inset is the measured element composition.

下载: 全尺寸图片幻灯片

图 2 不同厚度 Nb:STO/STO 薄膜在不同温度下的面内热电性能　(a)电导率; (b)载流子浓度; (c)塞贝克系数; (d)功率因子

Fig. 2. Temperature dependence of in-plane thermoelectric properties of Nb:STO/STO thin films with different thicknesses: (a) Conductivities; (b) carrier concentrations; (c) Seebeck coefficients; (d) power factors.

下载: 全尺寸图片幻灯片

图 3 NSTO/LSAT 薄膜生长状况表征　(a) AFM形貌图; (b) XRD谱; (c) 薄膜 c 轴晶格常数

Fig. 3. Characterization of Nb:STO/LSAT thin films: (a) AFM image; (b) XRD spectrum; (c) lattice parameters of the c axis.

下载: 全尺寸图片幻灯片

图 4 不同厚度Nb:STO/STO和Nb:STO/LSAT 薄膜在不同温度下的面内热电性能　(a) 电导率; (b) 塞贝克系数; (c) 功率因子; (d) 不同衬底、厚度薄膜的电导率对比

Fig. 4. Temperature dependence of in-plane thermoelectric properties of Nb:STO/STO and Nb:STO/LSAT thin films with different thicknesses: (a) Conductivities; (b) Seebeck coefficients; (c) power factors; (d) conductivity of thin films with different thicknesses and substrates.

下载: 全尺寸图片幻灯片

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应变增强Nb掺杂SrTiO₃薄膜热电性能