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題名 Bi0.5Sb1.5Te3 與 Cu0.02Bi2Te2.7Se0.3熱電微結構陣列之製備與應用
The fabrication and application of Bi0.5Sb1.5Te3 and Cu0.02Bi2Te2.7Se0.3 micro-thermoelectric array
作者 吳宗恆
Wu, Tsung - Heng
貢獻者 陳洋元
Chen, Yang-Yuan
吳宗恆
Wu, Tsung - Heng
關鍵詞 熱電
微型陣列
日期 2017
上傳時間 10-Aug-2017 10:00:01 (UTC+8)
摘要 　本論文為設計微型陣列熱電元件製程與製備，利用金屬遮罩與黃光半導體兩種方式來定義元件中微型陣列的部分，藉此做出熱電元件展現其商業價值。在此研究中利用自製靶材P-type (　Bi0.5Sb1.5Te3　)　與　N-type (Cu0.02Bi2Te2.7Se0.3 )與控制磁控濺鍍系統之功率與壓力的情況，製作最好的熱電薄膜，而　P-type與　N-type的最佳鍍膜條件皆為功率　30 w　與壓力　7mtorr。接著，將濺鍍完成的薄膜進行　200 0C　6小時的退火動作，藉此提升熱電陣列之效率。電極的部分，選用金作為主要組成，整個研究過程中使用厚度為650 μm的方形三氧化二鋁單晶作為基板(35 x 35 mm2)，最後利用半導體黃光製程的方式完成 442 對的熱電陣列，藉此量測電壓電阻。將這些製作完成之元件藉由溫差量測電壓差，將會有幾百個微福特的電壓差產生。
　In our research, we design the micro-thermoelectric array element process and preparation, we use the metal mask and the photoresist to define the micro-thermoelectric array in the element, so as to make the thermoelectric element to be commercial value. In this study, we used for the self-made target P-type (Bi0.5Sb1.5Te3) and N-type (Cu0.02Bi2Te2.7Se0.3 ) , the use controlled RF magnetron sputter system power and pressure conditions, making the best thermoelectric film, the best P-type and N-type are RF power 30 w and pressure 7 mtorr. The best annealing is 200°C for 6 hours. Through the whole process, a square sapphire single crystal with a thickness of 650 μm was used as the substrate (35 x 35 mm2). Finally, a thermoelectric array of 442 pairs was fabricated by Photoresist process to measure the voltage and resistance.
參考文獻 [1]In the 1950s there were hopes that semiconductor thermocouples would
replace mechanical refrigerators, just as semiconductor transistors
supplanted vacuum tubes.
[2]莊沅澄，鈷摻雜對FeSi熱電傳輸性質影響之研究，碩士論文，東華大學，2016
[3]A. Hmood , A. Kadhim , H. Abu Hassan，Lead–ytterbium–telluride thin films prepared using thermal evaporation technique for thermal sensing applications，Superlattices and Microstructures 54 (2013) 204–214
[4]Changcun Li, Fengxing Jiang , Congcong Liu, Wenfang Wang, Xuejing Li, Tongzhou Wang, Jingkun Xu，A simple thermoelectric device based on inorganic/organic composite　thin film for energy harvesting，Chemical Engineering Journal 320 (2017) 201–210
[5]Wei Zhu, Yuan Deng, Lili Cao，Light-concentrated solar generator and sensor based on flexible thin-film thermoelectric device，Nano Energy 34 (2017) 463–471
[6]Ugur Erturun , Kaan Erermis , Karla Mossi，Effect of various leg geometries on thermo-mechanical and power generation performance of thermoelectric devices，Applied Thermal Engineering 73 (2014) 128－141
[7]Ming Tan , Xiuzhen Wang , Yanming Hao , Yuan Deng，Novel Ag nanowire array with high electrical conductivity and fast heat transfer behavior as the electrode for film devices，Journal of Alloys and Compounds 701 (2017) 49－54
[8]L.D. Zhao , B.-P. Zhang , J.-F. Li , M. Zhou , W.S. Liu，Effects of process parameters on electrical properties of n-type Bi2Te3 prepared by mechanical alloying and spark plasma sintering，Physica B 400 (2007) 11–15
[9]Mizue Mizoshiri , Masashi Mikami and Kimihiro Ozaki，The effect of Cr buffer layer thickness on voltage generation of thin-film thermoelectric modules，J. Micromech. Microeng. 23 (2013) 115016
[10]Nanshu Lu, Xi Wang, Zhigang Suo, and Joost Vlassak，Metal films on polymer substrates stretched beyond 50%，APPLIED PHYSICS LETTERS 91, 221909 2007
[11]M.Mizoshiri , M.Mikami , K. Ozaki，Flexible thin-film thermoelectric generator inserting Cr buffer layer，PowerMEMS 2012, Atlanta, GA, USA, December 2-5, 2012
[12]HUEY-JIUAN LIN, KAI-JYUN KANG, JENN-DONG HWANG, HSU-SHEN　CHU,HONG-HSIN HUANG, and MOO-CHIN WANG，Effect of Annealing Temperature on the Thermoelectric Properties of the Bi0.5Sb1.5Te3 Thin Films Prepared by Radio-Frequency Sputtering，METALLURGICAL AND MATERIALS TRANSACTIONS A VOLUME 44A, MAY 2013—2339
[13]Takashi Onishi, Masao Mizuno, Tetsuya Yoshikawa , Jun Munemasa, Masataka Mizuno, Teruo Kihara , Hideki Araki, and Yasuharu Shirai，Highly-enhanced reflow characteristics of sputter deposited Cu alloy thin films for large scale integrated interconnections，JOURNAL OF APPLIED PHYSICS 110, 034304 (2011)
[14]C. C. Wei, P. C. Liu, Chih Chen, Jeffrey C.B. Lee, and I Ping Wang，Relieving Sn whisker growth driven by oxidation on Cu leadframe by annealing and　reflowing treatments，JOURNAL OF APPLIED PHYSICS 102, 043521 2007
[15]Xu Chen , Feng Xue , Jian Zhou , Yao Yao，Effect of In on microstructure, thermodynamic characteristic and mechanical properties of Sn–Bi based lead-free solder，Journal of Alloys and Compounds 633 (2015) 377–383
[16]Omid Mokhtari , Hiroshi Nishikawa，Correlation between microstructure and mechanical properties of Sn–Bi–X solders，Materials Science & Engineering A651 (2016) 831–839
[17]Alberto Torres, Luis Hernández, Octavio Domínguez，Effect of Antimony Additions on Corrosion and Mechanical Properties of Sn-Bi Eutectic Lead-Free Solder Alloy，Materials Sciences and Applications, 2012, 3, 355-362
[18]Th. Heckmann , Th. Souvignet , S. Lepeer , D. Naccache ，Low-temperature low-cost 58 Bismuth e 42 Tin alloy forensic chip re-balling and re-soldering，Digital Investigation 19 (2016) 60－68
[19]Wen P. Lin • Daniel E. Wesolowski ，Barrier/bonding layers on bismuth telluride (Bi2Te3) for high temperature thermoelectric modules，J Mater Sci: Mater Electron (2011) 22:1313–1320
[20]Yusuke Sasaki, Masayuki Takashiri，Effects of Cr interlayer thickness on adhesive, structural, and thermoelectric properties of antimony telluride thin films deposited by radio-frequency magnetron sputtering，Thin Solid Films 619 (2016) 195–201
[21]Complex thermoelectric materials，REVIEW ARTICLE
[22]Abu Raihan Mohammad Siddique, Shohel Mahmud⁎, Bill Van Heyst，A review of the state of the science on wearable thermoelectric power generators (TEGs) and their existing challenges，Renewable and Sustainable Energy Reviews 73 (2017) 730–744
[23]YI MA, WARUNA WIJESEKARA and ANDERS E. C. PALMQVIST，YI MA,1,2 WARUNA WIJESEKARA,1 and ANDERS E. C. PALMQVIST1,3，Journal of ELECTRONIC MATERIALS, Vol. 41, No. 6, 2012
[24]Koksal Yildiz, Unal Akgul , Hartmut S. Leipner , Yusuf Atici ，Electron microscopy study of thermoelectric n-type Bi2(Te0.9Se0.1)3 film deposited by dc sputtering，Superlattices and Microstructures 58 (2013) 60–71
[25]Haiyu Fang, Bhooshan C. Popere, Elayne M. Thomas, Cheng-Kang Mai, William B. Chang,Guillermo C. Bazan, Michael L. Chabinyc, Rachel A. Segalman，Large-scale integration of flexible materials into rolled and corrugated thermoelectric modules，J. APPL. POLYM. SCI. 2017, DOI: 10.1002/APP.44208
[26]G. JEFFREY SNYDER, JAMES R. LIM, CHEN-KUO HUANG AND JEAN-PIERRE FLEURIAL，Thermoelectric microdevice fabricated by a MEMS-like electrochemical process，nature materials(AUGUST 2003) 528-531
描述 碩士
國立政治大學
應用物理研究所
104755015
資料來源 http://thesis.lib.nccu.edu.tw/record/#G0104755015
資料類型 thesis
dc.contributor.advisor 陳洋元zh_TW
dc.contributor.advisor Chen, Yang-Yuanen_US
dc.contributor.author (Authors) 吳宗恆zh_TW
dc.contributor.author (Authors) Wu, Tsung - Hengen_US
dc.creator (作者) 吳宗恆zh_TW
dc.creator (作者) Wu, Tsung - Hengen_US
dc.date (日期) 2017en_US
dc.date.accessioned 10-Aug-2017 10:00:01 (UTC+8)-
dc.date.available 10-Aug-2017 10:00:01 (UTC+8)-
dc.date.issued (上傳時間) 10-Aug-2017 10:00:01 (UTC+8)-
dc.identifier (Other Identifiers) G0104755015en_US
dc.identifier.uri (URI) http://nccur.lib.nccu.edu.tw/handle/140.119/111791-
dc.description (描述) 碩士zh_TW
dc.description (描述) 國立政治大學zh_TW
dc.description (描述) 應用物理研究所zh_TW
dc.description (描述) 104755015zh_TW
dc.description.abstract (摘要) 　本論文為設計微型陣列熱電元件製程與製備，利用金屬遮罩與黃光半導體兩種方式來定義元件中微型陣列的部分，藉此做出熱電元件展現其商業價值。在此研究中利用自製靶材P-type (　Bi0.5Sb1.5Te3　)　與　N-type (Cu0.02Bi2Te2.7Se0.3 )與控制磁控濺鍍系統之功率與壓力的情況，製作最好的熱電薄膜，而　P-type與　N-type的最佳鍍膜條件皆為功率　30 w　與壓力　7mtorr。接著，將濺鍍完成的薄膜進行　200 0C　6小時的退火動作，藉此提升熱電陣列之效率。電極的部分，選用金作為主要組成，整個研究過程中使用厚度為650 μm的方形三氧化二鋁單晶作為基板(35 x 35 mm2)，最後利用半導體黃光製程的方式完成 442 對的熱電陣列，藉此量測電壓電阻。將這些製作完成之元件藉由溫差量測電壓差，將會有幾百個微福特的電壓差產生。zh_TW
dc.description.abstract (摘要) 　In our research, we design the micro-thermoelectric array element process and preparation, we use the metal mask and the photoresist to define the micro-thermoelectric array in the element, so as to make the thermoelectric element to be commercial value. In this study, we used for the self-made target P-type (Bi0.5Sb1.5Te3) and N-type (Cu0.02Bi2Te2.7Se0.3 ) , the use controlled RF magnetron sputter system power and pressure conditions, making the best thermoelectric film, the best P-type and N-type are RF power 30 w and pressure 7 mtorr. The best annealing is 200°C for 6 hours. Through the whole process, a square sapphire single crystal with a thickness of 650 μm was used as the substrate (35 x 35 mm2). Finally, a thermoelectric array of 442 pairs was fabricated by Photoresist process to measure the voltage and resistance.en_US
dc.description.tableofcontents 第一章　　緒論　　　　　　　　　　　　　　　　　　　　　　　　　　　1
1.1　研究背景與動機 1
1.2　熱電元件基本概述 2
第二章　　熱電基本性質與元件介紹　　　　　　　　　　　　　　　　　　3
2.1 熱電效應 3
2.1.1 席貝克效應(Seebeck效應) 3
2.1.2 撇爾特效應(peltier效應) 4
2.1.3 湯普森效應(Thomson效應) 4
2.1.4 電導率 5
2.1.5 熱傳導率 6
2.1.5.1　　熱傳導率之電子影響 6
2.1.5.1　　熱傳導率之聲子影響 7
2.1.6 熱電優值係數 8
2.2 熱電元件構造 8
2.3 熱電元件工作原理 10
第三章　　製程總覽與實驗步驟　　　　　　　　　　　　　　　　　　　　11
3.1 陣列製程介紹 11
3.2 相關儀器介紹 15
3.2.1　　基板清洗 15
3.2.2　　金屬遮罩與光罩設計 16
3.2.3　　電子束熱蒸鍍系統沉積電極 20
3.2.4　　N-type (Cu0.02Bi2Te2.7Sb0.3)靶材製備 22
3.2.5　　磁控濺鍍系統沉積熱電材料 23
3.2.6　　熱壓系統退火 25
3.2.7　　熱蒸鍍系統沉積焊料 27
3.2.8　　反應離子蝕刻系統(RIE&ICP) 28
3.2.9　　焊料選擇 30
3.2.10　　光阻選擇 31
3.2.11　　對準系統 34
3.3 相關量測系統 36
3.3.1 　　膜厚量測儀 36
3.3.2 X光射線繞射儀 37
3.3.3 Seebeck系數和電阻測試系統(ZEM-3) 39
3.3.4 掃描式電子顯微鏡(SEM) 39
3.3.5　　雷射閃光法測定裝置(Laser flash analysis，LFA) 40
第四章　　實驗結果與討論　　　　　　　　　　　　　　　　　　　　　　42
4.1　　熱電薄膜性質 42
4.1.1　　退火參數對熱電性能之影響 42
4.1.2　　熱電材料之量測 43
4.1.2.1　　P-type(Bi0.5Sb1.5Te3)之Seebeck系數與電阻率量測 43
4.1.2.2　　N-type(Cu0.02Bi2Te2.7Sb0.3)之Seebeck系數與電阻率量測 43
4.1.3　　影像數據 48
4.1.4　　XRD 特性與晶粒大小 50
4.2　　陣列之製程 52
4.2.1　　光阻厚度檢測 52
4.2.2　　焊料選擇之結果 54
4.2.3　　上下電極對貼結果 56
4.2.4　　針對單一對數之電壓與電阻量測 57
4.2.5　　加入鉻再鍍上材料結果 61
4.2.6　　黃光製程沉積上電極結果 62
4.2.7　　圖形暈開之解決辦法 65
第五章　　結論　　66

 		zh_TW
dc.format.extent 5176609 bytes-
dc.format.mimetype application/pdf-
dc.source.uri (資料來源) http://thesis.lib.nccu.edu.tw/record/#G0104755015en_US
dc.subject (關鍵詞) 熱電zh_TW
dc.subject (關鍵詞) 微型陣列zh_TW
dc.title (題名) Bi0.5Sb1.5Te3 與 Cu0.02Bi2Te2.7Se0.3熱電微結構陣列之製備與應用zh_TW
dc.title (題名) The fabrication and application of Bi0.5Sb1.5Te3 and Cu0.02Bi2Te2.7Se0.3 micro-thermoelectric arrayen_US
dc.type (資料類型) thesisen_US
dc.relation.reference (參考文獻) [1]In the 1950s there were hopes that semiconductor thermocouples would
replace mechanical refrigerators, just as semiconductor transistors
supplanted vacuum tubes.
[2]莊沅澄，鈷摻雜對FeSi熱電傳輸性質影響之研究，碩士論文，東華大學，2016
[3]A. Hmood , A. Kadhim , H. Abu Hassan，Lead–ytterbium–telluride thin films prepared using thermal evaporation technique for thermal sensing applications，Superlattices and Microstructures 54 (2013) 204–214
[4]Changcun Li, Fengxing Jiang , Congcong Liu, Wenfang Wang, Xuejing Li, Tongzhou Wang, Jingkun Xu，A simple thermoelectric device based on inorganic/organic composite　thin film for energy harvesting，Chemical Engineering Journal 320 (2017) 201–210
[5]Wei Zhu, Yuan Deng, Lili Cao，Light-concentrated solar generator and sensor based on flexible thin-film thermoelectric device，Nano Energy 34 (2017) 463–471
[6]Ugur Erturun , Kaan Erermis , Karla Mossi，Effect of various leg geometries on thermo-mechanical and power generation performance of thermoelectric devices，Applied Thermal Engineering 73 (2014) 128－141
[7]Ming Tan , Xiuzhen Wang , Yanming Hao , Yuan Deng，Novel Ag nanowire array with high electrical conductivity and fast heat transfer behavior as the electrode for film devices，Journal of Alloys and Compounds 701 (2017) 49－54
[8]L.D. Zhao , B.-P. Zhang , J.-F. Li , M. Zhou , W.S. Liu，Effects of process parameters on electrical properties of n-type Bi2Te3 prepared by mechanical alloying and spark plasma sintering，Physica B 400 (2007) 11–15
[9]Mizue Mizoshiri , Masashi Mikami and Kimihiro Ozaki，The effect of Cr buffer layer thickness on voltage generation of thin-film thermoelectric modules，J. Micromech. Microeng. 23 (2013) 115016
[10]Nanshu Lu, Xi Wang, Zhigang Suo, and Joost Vlassak，Metal films on polymer substrates stretched beyond 50%，APPLIED PHYSICS LETTERS 91, 221909 2007
[11]M.Mizoshiri , M.Mikami , K. Ozaki，Flexible thin-film thermoelectric generator inserting Cr buffer layer，PowerMEMS 2012, Atlanta, GA, USA, December 2-5, 2012
[12]HUEY-JIUAN LIN, KAI-JYUN KANG, JENN-DONG HWANG, HSU-SHEN　CHU,HONG-HSIN HUANG, and MOO-CHIN WANG，Effect of Annealing Temperature on the Thermoelectric Properties of the Bi0.5Sb1.5Te3 Thin Films Prepared by Radio-Frequency Sputtering，METALLURGICAL AND MATERIALS TRANSACTIONS A VOLUME 44A, MAY 2013—2339
[13]Takashi Onishi, Masao Mizuno, Tetsuya Yoshikawa , Jun Munemasa, Masataka Mizuno, Teruo Kihara , Hideki Araki, and Yasuharu Shirai，Highly-enhanced reflow characteristics of sputter deposited Cu alloy thin films for large scale integrated interconnections，JOURNAL OF APPLIED PHYSICS 110, 034304 (2011)
[14]C. C. Wei, P. C. Liu, Chih Chen, Jeffrey C.B. Lee, and I Ping Wang，Relieving Sn whisker growth driven by oxidation on Cu leadframe by annealing and　reflowing treatments，JOURNAL OF APPLIED PHYSICS 102, 043521 2007
[15]Xu Chen , Feng Xue , Jian Zhou , Yao Yao，Effect of In on microstructure, thermodynamic characteristic and mechanical properties of Sn–Bi based lead-free solder，Journal of Alloys and Compounds 633 (2015) 377–383
[16]Omid Mokhtari , Hiroshi Nishikawa，Correlation between microstructure and mechanical properties of Sn–Bi–X solders，Materials Science & Engineering A651 (2016) 831–839
[17]Alberto Torres, Luis Hernández, Octavio Domínguez，Effect of Antimony Additions on Corrosion and Mechanical Properties of Sn-Bi Eutectic Lead-Free Solder Alloy，Materials Sciences and Applications, 2012, 3, 355-362
[18]Th. Heckmann , Th. Souvignet , S. Lepeer , D. Naccache ，Low-temperature low-cost 58 Bismuth e 42 Tin alloy forensic chip re-balling and re-soldering，Digital Investigation 19 (2016) 60－68
[19]Wen P. Lin • Daniel E. Wesolowski ，Barrier/bonding layers on bismuth telluride (Bi2Te3) for high temperature thermoelectric modules，J Mater Sci: Mater Electron (2011) 22:1313–1320
[20]Yusuke Sasaki, Masayuki Takashiri，Effects of Cr interlayer thickness on adhesive, structural, and thermoelectric properties of antimony telluride thin films deposited by radio-frequency magnetron sputtering，Thin Solid Films 619 (2016) 195–201
[21]Complex thermoelectric materials，REVIEW ARTICLE
[22]Abu Raihan Mohammad Siddique, Shohel Mahmud⁎, Bill Van Heyst，A review of the state of the science on wearable thermoelectric power generators (TEGs) and their existing challenges，Renewable and Sustainable Energy Reviews 73 (2017) 730–744
[23]YI MA, WARUNA WIJESEKARA and ANDERS E. C. PALMQVIST，YI MA,1,2 WARUNA WIJESEKARA,1 and ANDERS E. C. PALMQVIST1,3，Journal of ELECTRONIC MATERIALS, Vol. 41, No. 6, 2012
[24]Koksal Yildiz, Unal Akgul , Hartmut S. Leipner , Yusuf Atici ，Electron microscopy study of thermoelectric n-type Bi2(Te0.9Se0.1)3 film deposited by dc sputtering，Superlattices and Microstructures 58 (2013) 60–71
[25]Haiyu Fang, Bhooshan C. Popere, Elayne M. Thomas, Cheng-Kang Mai, William B. Chang,Guillermo C. Bazan, Michael L. Chabinyc, Rachel A. Segalman，Large-scale integration of flexible materials into rolled and corrugated thermoelectric modules，J. APPL. POLYM. SCI. 2017, DOI: 10.1002/APP.44208
[26]G. JEFFREY SNYDER, JAMES R. LIM, CHEN-KUO HUANG AND JEAN-PIERRE FLEURIAL，Thermoelectric microdevice fabricated by a MEMS-like electrochemical process，nature materials(AUGUST 2003) 528-531		zh_TW