Bi_2A_2Co_2O_y（A＝Ca、Sr、Ba）体系热电薄膜的LITV效应及其电输运性质的研究
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摘要
本文首次在倾斜生长的Bi_2Ca_2Co_2O_y.Bi_2Ba_2Co_2O_y热电薄膜中观察到激光感生热电电压(LITV)效应。并根据LITV信号的拟合数据研究了薄膜的热扩散系数和各向异性塞贝克系数。分析了薄膜的层间失配度对其热电性能和LITV信号的影响。
采用固相反应法制备了Bi_2Ca_2Co_2O_y、Bi_2Sr_2Co_2O_y、Bi_2Ba_2Co_2O_y多晶陶瓷作为沉积薄膜的靶材。用X射线衍射(XRD)分析了它们的结构,表明所制备的靶材基本上为单相的具有c轴择优取向的多晶陶瓷。用四引线法测量了电阻-温度曲线,得出在所测温度范围内Bi_2Ca_2Co_2O_y表现为半导体导电特性,Bi_2Sr_2Co_2O_y存在一个由半导体导电向金属导电转变的温度,Bi_2Ba_2Co_2O_y表现为金属导电特性。对靶材的半导体导电行为根据公式计算了电阻率-温度曲线,并应用半导体导电的热激活模型的理论计算了热激活能。分析表明导电性是随着多晶的层间失配度的降低而变好的。
采用脉冲激光沉积技术(PLD)在A1203单晶衬底上制备了Bi_2Ca_2Co_2O_y. Bi_2Ca_2Co_2O_y外延薄膜,讨论了温度、氧压等参数对其生长质量的影响。用X射线衍射(XRD)分析表明它们都具有高度的c轴择优取向。用四探针法测量了电阻-温度曲线,表明Bi_2Ca_2Co_2O_y和Bi_2Sr_2Co_2O_y都存在一个由半导体导电向金属导电转变的温度,Bi_2Ba_2Co_2O_y表现为金属导电特性。分析了薄膜的导电性随晶格失配度的变化关系,并和多晶的电输运性能做了简单的对比和分析。
在倾斜角度为10。的A1203单晶衬底上制备了以上三个系列的热电薄膜,并在其中观察到了LITV信号。研究了厚度对LITV信号的影响,表明对应LITV信号的最大值存在一个最佳的薄膜厚度。研究了层间失配度对LITV信号的影响,表明层间失配度越大LITV信号也越大。
通过拟合LITV信号下降沿时间参数得到了薄膜的热扩散系数D与薄膜厚度的关系,根据一维热传导模型推导了薄膜上下表面的温差,结合文献中报道的激光感生热电电压公式,推导出了一个崭新的计算各向异性塞贝克系数(Sab-Sc)的公式；根据上述结论和测量的薄膜的LITV信号,计算出了薄膜的热扩散系数D和Sab-Sc。分析了D和Sab-Sc随层间失配度的变化关系,D是随着层间失配度的增大而先减小后增大,Sab-Sc。是随着层间失配度的增大而减小的,另一方面也说明了塞贝克系数大的材料其各向异性塞贝克系数也大,反之亦然。
根据以上结论,提出了快速评估该体系材料热电性能的新方法。即：通过测量LITV信号可以根据其峰值的高低来判断其各向异性塞贝克系数(Sab-Sc)的大小,而(Sab-Sc)大的材料其塞贝克系数也大；通过拟合LITV信号的下降沿时间可以估算其热扩散系数,从而也可以比较其热导率的大小：通过四探针法测量R-T关系可以推断其电输运性质的优劣。这样影响热电材料的优值的三个重要的参数我们都可以进行判断,进而可以分析比较其热电性能的好坏了。
Laser induced thermoelectric voltage (LITV) effect was observed on these Bi2Ca2Co2Oy, Bi2Ba2Co2Oy thermoelectric thin films grown on vicinal-cut single crystalline substrates for the first time. Film thermal diffusivity and anisotropy of the Seebeck coefficient of the signal were studied by fitting the data LITV and mismatch performances of their thermoelectric properties with LITV signals were analyzed.
The Bi2Ca2Co2Oy, Bi2Sr2Co2Oy, and Bi2Ba2Co2Oy polycrystalline ceramics were prepared by solid state reaction as thin film deposition targets. Their structures were analysised by X-ray diffraction (XRD), the results showed that these prepared targets were single phase with c-axis preferred orientation of polycrystalline ceramics, we employed resistance & temperature behaviors techniques to investigate electric properties of these targets.The data showed that Bi2Ca2Co2Oy showed semiconducting properties in the measured temperature range.For Bi2Sr2Co2Oy, there is a phenomenon of semiconducting to metal conductivity transition at a certain temperature and Bi2Ba2Co2Oy was metallic electrical properties. The semiconductor behavior of the targets was investigated under the formula to the resistivity-temperature curve, and the semiconductor conductive thermal activation model was employed of to calculate the thermal activation energy. Analysis showed that the conductivity of polycrystalline layers becomed better with the lower of the mismatch.
The Bi2Ca2Co2Oy, Bi2Sr2Co2Oy, Bi2Ba2Co2Oy films were prepared by pulsed laser deposition (PLD) on the Al2O3 single crystal substrates. We discussed the influence of different growth conditions on structure, properties of these thin films, such as temperature, oxygen pressure and other parameters. X-ray diffraction (XRD) analysis showed that they all have a high degree of c-axis orientation. Resistance & temperature behaviors techniques were measured by four probe method. The results indicated that there were a semiconducting to metal conductivity transition temperature for Bi2Ca2Co2Oy and Bi2Sr2Co2Oy, but Bi2Ba2Co2Oy shows metallic electrical properties. Conductivity of films were analyzed with the change of lattice mismatch, And a simple comparison and analysis were done in the electrical transport properties between films and polycrystalline.
The three series of thermoelectric thin films were grown on the 10°vicinal-cut Al2O3 single crystal substrates, and the LITV signals were observed on all these films. The thickness was studied to investigate the influence on the LITV signals. The results show that there is an optimum film thickness to the maximum LITV signal. Mismatch between layers impacting on the LITV signal was also studied, and shows that when the mismatch between layers was the greater, the LITV signal was greater too.
The relationship between film thermal diffusivity D and film thickness was obtained by fitting the parameters LITV signal fall time, according to one-dimensional heat conduction model we derived the temperature between upper and lower surface of the film, A new formula with anisotropic Seebeck coefficient (Sab-Sc) was pushed through reported in the literature combined with laser induced thermoelectric voltage formula. These were calculated according to the findings and measurement of the film LITV signal to that the thermal diffusivity of films D and Sab-Sc. It was analysised that D and Sab-Sc with the mismatch between layers changes in relations. D is from increase to decrease with the the increase of mismatch between layers, and Sab-Sc is always decrease with that, On the other hand it also shows that the material which have a larger Seebeck coefficient also have a larger anisotropy of Seebeck coefficient, and vice versa.
According to the above conclusions, a new method for rapid assessment of the thermoelectric properties of materials has been proposed. Namely:determining anisotropy Seebeck coefficient (Sab-Sc) can rely on measuring the peak level of its LITV signal, whereas (Sab-Sc) of its large Seebeck coefficient of the material must be greater; The thermal diffusion coefficient can be estimated by fitting the falling edge of the signal time LITV, and thus to compare the size of the thermal conductivity; It may be inferred that the merits of their electrical transport properties by four-probe measurement of R-T relationships. There for,we can determine the three important parameters which affect the value of thermoelectric materials, in turn, can compare the thermoelectric properties of a good or bad.
采用固相反应法制备了Bi_2Ca_2Co_2O_y、Bi_2Sr_2Co_2O_y、Bi_2Ba_2Co_2O_y多晶陶瓷作为沉积薄膜的靶材。用X射线衍射(XRD)分析了它们的结构,表明所制备的靶材基本上为单相的具有c轴择优取向的多晶陶瓷。用四引线法测量了电阻-温度曲线,得出在所测温度范围内Bi_2Ca_2Co_2O_y表现为半导体导电特性,Bi_2Sr_2Co_2O_y存在一个由半导体导电向金属导电转变的温度,Bi_2Ba_2Co_2O_y表现为金属导电特性。对靶材的半导体导电行为根据公式计算了电阻率-温度曲线,并应用半导体导电的热激活模型的理论计算了热激活能。分析表明导电性是随着多晶的层间失配度的降低而变好的。
采用脉冲激光沉积技术(PLD)在A1203单晶衬底上制备了Bi_2Ca_2Co_2O_y. Bi_2Ca_2Co_2O_y外延薄膜,讨论了温度、氧压等参数对其生长质量的影响。用X射线衍射(XRD)分析表明它们都具有高度的c轴择优取向。用四探针法测量了电阻-温度曲线,表明Bi_2Ca_2Co_2O_y和Bi_2Sr_2Co_2O_y都存在一个由半导体导电向金属导电转变的温度,Bi_2Ba_2Co_2O_y表现为金属导电特性。分析了薄膜的导电性随晶格失配度的变化关系,并和多晶的电输运性能做了简单的对比和分析。
在倾斜角度为10。的A1203单晶衬底上制备了以上三个系列的热电薄膜,并在其中观察到了LITV信号。研究了厚度对LITV信号的影响,表明对应LITV信号的最大值存在一个最佳的薄膜厚度。研究了层间失配度对LITV信号的影响,表明层间失配度越大LITV信号也越大。
通过拟合LITV信号下降沿时间参数得到了薄膜的热扩散系数D与薄膜厚度的关系,根据一维热传导模型推导了薄膜上下表面的温差,结合文献中报道的激光感生热电电压公式,推导出了一个崭新的计算各向异性塞贝克系数(Sab-Sc)的公式；根据上述结论和测量的薄膜的LITV信号,计算出了薄膜的热扩散系数D和Sab-Sc。分析了D和Sab-Sc随层间失配度的变化关系,D是随着层间失配度的增大而先减小后增大,Sab-Sc。是随着层间失配度的增大而减小的,另一方面也说明了塞贝克系数大的材料其各向异性塞贝克系数也大,反之亦然。
根据以上结论,提出了快速评估该体系材料热电性能的新方法。即：通过测量LITV信号可以根据其峰值的高低来判断其各向异性塞贝克系数(Sab-Sc)的大小,而(Sab-Sc)大的材料其塞贝克系数也大；通过拟合LITV信号的下降沿时间可以估算其热扩散系数,从而也可以比较其热导率的大小：通过四探针法测量R-T关系可以推断其电输运性质的优劣。这样影响热电材料的优值的三个重要的参数我们都可以进行判断,进而可以分析比较其热电性能的好坏了。
Laser induced thermoelectric voltage (LITV) effect was observed on these Bi2Ca2Co2Oy, Bi2Ba2Co2Oy thermoelectric thin films grown on vicinal-cut single crystalline substrates for the first time. Film thermal diffusivity and anisotropy of the Seebeck coefficient of the signal were studied by fitting the data LITV and mismatch performances of their thermoelectric properties with LITV signals were analyzed.
The Bi2Ca2Co2Oy, Bi2Sr2Co2Oy, and Bi2Ba2Co2Oy polycrystalline ceramics were prepared by solid state reaction as thin film deposition targets. Their structures were analysised by X-ray diffraction (XRD), the results showed that these prepared targets were single phase with c-axis preferred orientation of polycrystalline ceramics, we employed resistance & temperature behaviors techniques to investigate electric properties of these targets.The data showed that Bi2Ca2Co2Oy showed semiconducting properties in the measured temperature range.For Bi2Sr2Co2Oy, there is a phenomenon of semiconducting to metal conductivity transition at a certain temperature and Bi2Ba2Co2Oy was metallic electrical properties. The semiconductor behavior of the targets was investigated under the formula to the resistivity-temperature curve, and the semiconductor conductive thermal activation model was employed of to calculate the thermal activation energy. Analysis showed that the conductivity of polycrystalline layers becomed better with the lower of the mismatch.
The Bi2Ca2Co2Oy, Bi2Sr2Co2Oy, Bi2Ba2Co2Oy films were prepared by pulsed laser deposition (PLD) on the Al2O3 single crystal substrates. We discussed the influence of different growth conditions on structure, properties of these thin films, such as temperature, oxygen pressure and other parameters. X-ray diffraction (XRD) analysis showed that they all have a high degree of c-axis orientation. Resistance & temperature behaviors techniques were measured by four probe method. The results indicated that there were a semiconducting to metal conductivity transition temperature for Bi2Ca2Co2Oy and Bi2Sr2Co2Oy, but Bi2Ba2Co2Oy shows metallic electrical properties. Conductivity of films were analyzed with the change of lattice mismatch, And a simple comparison and analysis were done in the electrical transport properties between films and polycrystalline.
The three series of thermoelectric thin films were grown on the 10°vicinal-cut Al2O3 single crystal substrates, and the LITV signals were observed on all these films. The thickness was studied to investigate the influence on the LITV signals. The results show that there is an optimum film thickness to the maximum LITV signal. Mismatch between layers impacting on the LITV signal was also studied, and shows that when the mismatch between layers was the greater, the LITV signal was greater too.
The relationship between film thermal diffusivity D and film thickness was obtained by fitting the parameters LITV signal fall time, according to one-dimensional heat conduction model we derived the temperature between upper and lower surface of the film, A new formula with anisotropic Seebeck coefficient (Sab-Sc) was pushed through reported in the literature combined with laser induced thermoelectric voltage formula. These were calculated according to the findings and measurement of the film LITV signal to that the thermal diffusivity of films D and Sab-Sc. It was analysised that D and Sab-Sc with the mismatch between layers changes in relations. D is from increase to decrease with the the increase of mismatch between layers, and Sab-Sc is always decrease with that, On the other hand it also shows that the material which have a larger Seebeck coefficient also have a larger anisotropy of Seebeck coefficient, and vice versa.
According to the above conclusions, a new method for rapid assessment of the thermoelectric properties of materials has been proposed. Namely:determining anisotropy Seebeck coefficient (Sab-Sc) can rely on measuring the peak level of its LITV signal, whereas (Sab-Sc) of its large Seebeck coefficient of the material must be greater; The thermal diffusion coefficient can be estimated by fitting the falling edge of the signal time LITV, and thus to compare the size of the thermal conductivity; It may be inferred that the merits of their electrical transport properties by four-probe measurement of R-T relationships. There for,we can determine the three important parameters which affect the value of thermoelectric materials, in turn, can compare the thermoelectric properties of a good or bad.
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