Research progress of Cu<sub>2</sub>Se thin film thermoelectric properties

Yang Liang-Liang; Qin Yuan-Hao; Wei Jiang-Tao; Song Pei-Shuai; Zhang Ming-Liang; Yang Fu-Hua; Wang Xiao-Dong

doi:10.7498/aps.70.20201677

Abstract

Thermoelectric (TE) materials can directly realize the mutual conversion between heat and electricity, and it is an environmentally friendly functional material. At present, the thermoelectric conversion efficiencies of thermoelectric materials are low, which seriously restricts the large-scale application of thermoelectric devices. Therefore, finding new materials with better thermoelectric properties or improving the thermoelectric properties of traditional thermoelectric materials has become the subject of thermoelectric research. Thin film materials, compared with bulk materials, possess both the two-dimensional macroscopic properties and one-dimensional nanostructure characteristics, which makes it much easier to study the relationships between physical mechanisms and properties. Besides, thin film are also suitable for the preparation of wearable electronic devices. This article summarizes five different preparation methods of Cu₂Se thin films, i.e. electrochemical deposition, thermal evaporation, spin coating, sputtering, and pulsed laser deposition. In addition, combing with typical examples, the characterization methods of the film are summarized, and the influence mechanism of each parameter on the thermoelectric performance from electrical conductivity, Seebeck coefficient and thermal conductivity is discussed. Finally, the hot application direction of Cu₂Se thin film thermoelectrics is also introduced.

Keywords:

Authors and contacts

1.
Engineering Research Center for Semiconductor Integrated Technology, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083, China
2.
College of Microelectronics and Research Center of Materials and Optoelectronics, University of Chinese Academy of Sciences, Beijing 100049, China
3.
Beijing Institute of Quantum Information Science, Beijing 100193, China
4.
Beijing Semiconductor Micro/Nano Integrated Engineering Technology Research Center, Beijing 100083, China

Corresponding author: Wang Xiao-Dong, xdwang@semi.ac.cn

Funds: Project supported by the National Key Research and Development Program of China (Grant Nos. 2019YFB1503602, 2018YFB1107502), the Pilot B Program of the Chinese Academy of Sciences, China (Grant No. XDB43020500) and Development Program of Scientific Research Instruments and Equipment of the Chinese Academy of Sciences, China (Grant No. GJJSTD20200006)

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References

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Cited By

图 1 Cu₂Se高温β相晶体结构^[34]　(a)在8c和32f间隙位置显示有铜原子的晶胞; (b)沿着立方[$1\bar{1} 0$]方向的晶体结构的投影平面表示

Figure 1. Cu₂Se high temperature β- phase crystal structure^[34] (a) Unit cell where the 8c and 32f interstitial positions are shown with Cu atoms; (b) projected plane representation of the crystal structure along the cubic [$1\bar{1} 0$] direction.

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图 2 (a)电镀沉积生长机制示意图; (b) Cu₂Se薄膜的XRD图案; (c) Cu₂Se薄膜的场发射扫描电子显微镜(FESEM)图像; (d) ITO基板上Cu₂Se薄膜的AFM 3D图像^[41]

Figure 2. (a) Schematic diagram of Galvanic Deposition mechanism; (b) XRD pattern of Cu₂Se thin film; (c) FESEM image of Cu₂Se thin film; (d) AFM 3D image of Cu₂Se film on ITO substrate^[41].

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图 3 (a)溶解在硫醇胺中的Cu_2–xSe溶液; (b) 旋涂和退火后, 玻璃上的Cu₂Se薄膜; (c) (d) Cu_2–xSe薄膜样品浸泡前的SEM图像; (d) Cu_2–xSe薄膜样品浸泡后的SEM图像; (e) 旋涂制备的Cu_2–xSe样品的XRD图谱^[54]

Figure 3. (a) Cu_2–x Se solution dissolved in thiolamine; (b) after spin coating and annealing, the Cu₂Se film on the glass; (c) SEM image of Cu_2–xSe thin film sample before soaking; (d) SEM image of Cu_2–xSe thin film sample after soaking; (e) XRD pattern of Cu_2–xSe sample prepared by spin coating^[54].

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图 4 (a) Al₂O₃基板上沉积的Cu₂Se薄膜的照片; (b) 在573 K下退火的薄膜能量色散X射线光谱(EDS); (c) Al₂O₃基材上薄膜的横截面SEM分析; (d) 薄膜中纳米晶体的TEM分析, 其中虚线突出了晶界, 插图是TEM图像的相应FFT^[40]

Figure 4. (a) Photograph of Cu₂Se thin film deposited on Al₂O₃ substrate; (b) energy dispersive X-ray spectroscopy (EDS) of thin film annealed at 573 K; (c) cross-sectional SEM analysis of thin film on Al₂O₃ substrate; (d) TEM analysis of nanocrystals in the thin film, the dotted line highlights the grain boundaries, the inset is the corresponding FFT of the TEM image.^[40]

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图 5 (a) 脉冲混合反应磁控溅射(PHRMS)沉积系统; (b) 从标称成分分别为Cu/Se = 1, 2, 2.4, 3.6, 5和9的薄膜上获得的掠入射同步辐射X射线衍射图^[60]

Figure 5. (a) Pulse hybrid reactive magnetron sputtering (PHRMS) deposition system; (b) grazing incident synchrotron radiation X Ray diffraction pattern obtained from a film with a nominal composition of Cu/Se = 1, 2, 2.4, 3.6, 5 and 9^[60].

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图 6 具有不同铜/硒比的薄膜的SEM图像^[60]　(a) Cu/Se = 1; (b) Cu/Se = 2; (c) Cu/Se = 2.4; (d) Cu/Se = 3.6; (e) Cu/Se = 5; (f) Cu/Se = 9

Figure 6. SEM images of films with different copper/selenium ratios^[60] (a) Cu/Se = 1; (b) Cu/Se = 2; (c) Cu/Se = 2.4; (d) Cu/Se = 3.6; (e) Cu/Se = 5; (f) Cu/Se = 9.

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图 7 (a)由各种Cu_2+xSe靶沉积的Cu_2–ySe膜中的XRD图案; (b) 根据布拉格定律计算的(001)面的晶面晶体间距(c); (c) Cu₂Se膜的截面HRTEM图像; (d) (e)不同Cu_2–xSe靶沉积的Cu_2–ySe膜的FESEM图像, (d) x = 0.1, (d) x = 0.3 ^[10]

Figure 7. (a) XRD patterns in Cu_2–y Se films deposited from various Cu_2+x Se targets; (b) (001) plane crystal spacing (c) calculated according to Bragg's law; (c) HRTEM image of the cross-section of Cu₂Se film; (d)(e) FESEM images of Cu_2–ySe films deposited on different Cu_2–x Se targets, (d) x = 0.1, (e) x = 0.3 ^[10]

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图 8 (a)在不同温度下退火的Cu₂Se薄膜中的室温载流子浓度; (b)电导率对薄膜中载流子浓度的依赖性; (c)塞贝克系数对薄膜中载流子浓度的依赖性; (d) (e) 柔性塑料基板上Cu₂Se薄膜的热电性能; (f)沉积在聚酰亚胺基板上的薄膜的电导率σ, (g)塞贝克系数S, (h) 功率因数PF = σS² ^[40]

Figure 8. (a) Room temperature carrier concentration in Cu₂Se thin films annealed at different temperatures; (b) dependence of conductivity on carrier concentration in thin films; (c) dependence of Seebeck coefficient on carrier concentration in film; (d)(e) thermoelectric properties of Cu₂Se film on flexible plastic substrate, (f) conductivity σ of the film deposited on polyimide substrate, (g) Seebeck coefficient S, (h) power factor PF = σS² ^[40].

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图 9 (a) Cu₂Se/PEDOT: PSS复合膜的输出电压与温度梯度的关系; (b) 在不同温差下的输出电压和功率与电流的关系; (c) 设备的数码照片; (d) 由于手臂和周围环境之间的温差而产生的4.5 mV电压的照片; (e) 将茶水倒入500 mL烧杯中直至液位到达设备下边缘时产生的15.4 mV电压的照片, d部分和e部分的插图是红外热像图^[77]

Figure 9. (a) Cu₂Se/PEDOT: Relationship between the output voltage of the PSS composite film and the temperature gradient; (b) relationship between output voltage and power and current under different temperature differences; (c) digital photos of the device; (d) photo of the 4.5 mV voltage generated due to the temperature difference between the arm and the surrounding environment; (e) pour the tea water into a 500 mL beaker until the liquid level reaches the bottom edge of the device at 15.4 mV voltage, where Illustrations in the (d) and (e) parts are infrared thermal images^[77]

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表 1 近年来Cu₂Se薄膜热电性能研究进展

Table 1. Research progress of Cu₂Se thin film thermoelectric properties in recent years.

Methods	Film	Cu/Se	Crystallite size/mm	S/μV·K^–1	σ/ ×10³ S/m	κ/ W·(m·K)^–1	PF/ mW·(m·K²) ^–1	ZT	Ref.
Chemical deposition	600	1.8	38		18				[68]
	330	2.125			1				[69]
	403	1.96	37.039		17.8				[70]
	1700	1.81			8.13 × 10³				[71]
Pulsed laser deposition	40	1.7	< 10		450				[72]
	234			57	130		619		[10]
				60	10		350		[61]
Electrochemial deposition	90—100	1.92—1.89			0.14—0.22				[42]
		1.78	40—50	80	27	0.77	173	0.07	[41]
		2.191	34	56			130		[73]
Sputtering deposition		1—3	1000	10—100	100				[74]
		3—10	100	> 100	1
	48—131	1.777		37.3	1.4—4.9				[5]
	600—850	1—9	25—84	100	100	0.8 ± 0.1	110	0.4	[60]
Spin coating process			300—500		44.603				[75]
	62.6	1.9—1.995		200—250	25	0.62	653	0.34	[54]
	50—100			80	100	0.4—1.4		0.14	[76]
	55	1.79 ± 0.06	10			1.3—1.5	620		[40]
Simple mechanical pressing	10000—50000	1.743		14.3	557.82	0.79	111.84	0.04	[9]
Wet-chemical process	8000	1.98		50.8	104.7	0.25—0.3	270.3	0.3	[77]

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Research progress of Cu₂Se thin film thermoelectric properties

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