拓樸超導性質已經在銅摻雜拓樸絕緣體中被發現，例如: CuxBi2Se3，然而尚未有過文獻探討銅摻雜Sb2Se3-xTex系列晶體(x從0到3)，因此本論文研究使用熔融法(Melting growth method)生長Cu0.3:Sb2Se3-xTex單晶樣品，隨後將所生長的高品質單晶樣品進行各項性質量測。
本實驗利用X光繞射儀(X-ray diffractometer，XRD)和穿透式電子顯微鏡(Transmission electron microscopy，TEM)分析樣品的結構和結晶方向，並計算其C軸長度；利用電子微探儀(Electron probe microanalyzer，EPMA)來做定量分析；利用拉曼光譜儀(Raman spectroscopy)分析晶體內部原子的振動模式；利用X射線光電子能譜儀(X-ray photoelectron spectroscopy，XPS)分析銅在晶體內是否帶價數；利用超導量子干涉儀(Superconducting quantum interference device，SQUID)來量測樣品是否具有超導現象。
目前所得到的實驗結果顯示：EPMA分析發現在四元晶體中有雜相存在；XRD和TEM分析確認了晶體結構，另外發現摻銅後C軸晶格常數變大，推論銅可能嵌入在凡德瓦爾層中；Raman分析顯示隨著Se摻雜量變多，有藍移現象發生；XPS分析得到銅為0價，可能以嵌入凡德瓦爾層中的形式存在在主相中；SQUID分析顯示所生長的晶體皆無超導特性。

Superconductivity has been discovered in Cu doped-topological insulators(TIs), for example, CuxBi2Se3. However, none of papers studied Cu doped Sb2Se3-xTex(x from 0 to 3) whether has superconductivity; therefore, this thesis presented the study of Cu0.3:Sb2Se3-xTex(x from 0 to 3) grown by melting growth method. The crystal structure and the c-axis lattice constant of the samples were confirmed by X-ray Diffraction(XRD) and Transmission Electron Microscopy(TEM) analysis. Qualitative and quantitative analysis were studied by EPMA. The vibration mode of phonons was studied by Raman spectroscopy. X-ray photoelectron spectroscopy(XPS) showed the valence of Cu. Superconducting quantum interference device(SQUID) was used to verify the samples whether have superconductivity or not.
The EPMA result showed that crystal has second phase. Moreover, according to XRD and TEM analyzation Cu might intercalated into the Van der Waals layer and caused the c-axis lattice constant increased. However superconductivity doesn’t exist in the crystal.

目錄
論文審定書……………………………………………………………………………………….i
致謝………………………………………………………………………………………………ii
摘要 iii
Abstract………………………………………………………………………………………….iv
圖目錄 vii
表目錄 xi
第一章 序論 1
1.1 前言 1
1.2 研究動機 2
第二章 文獻回顧與理論基礎 4
2.1 拓樸絕緣體(Topological insulator) …………………………………………………...4
2.2 拓樸超導體(Topological superconductor) …………………………………………….8
2.3 Sb2Se3-xTex的結構與性質 …………………………………………………………...10
2.4 熔融生長法 …………………………………………………………………………..13
第三章 實驗內容 14
3.1 實驗步驟 14
3.2 量測設備簡介 18
3.2.1 X光繞射分析儀(X-ray diffractometer，XRD)….…...………………………..18
3.2.2 電子微探儀(Electron probe microanalyzer，EPMA)………....... ….………….19
3.2.3 穿透式電子顯微鏡(Transmission electron microscopy，TEM)….……………20
3.2.4 拉曼光譜儀(Raman spectroscopy) ………………............................................ 21
3.2.5 X射線光電子能譜儀(X-ray photoelectron spectroscopy，XPS)……………..22
3.2.6 超導量子干涉儀(Superconducting quantum interference device，SQUID)... 23
第四章 實驗結果與討論 25
4.1 樣品形貌 25
4.2 電子微探儀(EPMA)分析………………….…........................................................... 26
4.3 粉末繞射(X-ray powder diffraction，XRD)分析 .…………………………………..35
4.4 高解析XRD(High resolution X-ray diffraction，HRXRD)分析………………...... 40
4.5 JCPDS card …………………………………………………………………………...55
4.6 穿透式電子顯微鏡(TEM)分析….…………………………………………………...57
4.7 拉曼(Raman)光譜分析……………………………………………………………… 64
4.8 X射線光電子能譜(XPS)分析……………………………………………………….66
4.9 超導量子干涉儀(SQUID)分析……………………………………………………... 70
第五章 結論 74
第六章 參考文獻 76

第六章 參考文獻
[1] Y. Xia, D. Qian, D. Hsieh, L. Wray, A. Pal, H. Lin, A. Bansil, D. Grauer, Y. S. Hor, R. J. Cava and M. Z. Hasan, Nature Physics, 5, 398. (2009)
[2] Y. L. Chen, J. G. Analytis, J. H. Chu, Z. K. Liu, S. -K. Mo, X. L. Qi, H. J. Zhang, D. H. Lu, X. Dai, Z. Fang, S. C. Zhang, I. R. Fisher, Z. Hussain and Z. -X. Shen, Science, 325, 178. (2009)
[3] D. Hsieh, Y. Xia, D. Qian, L. Wray, F. Meier, J. H. Dil, J. Osterwalder, L. Patthey, A. V. Fedorov, H. Lin, A. Bansil, D. Grauer, Y. S. Hor, R. J. Cava and M. Z. Hasan, Phys. Rev. Lett. 103, 146401. (2009)
[4] Andreas P. Schnyder, Shinsei Ryu, Akira Furusaki and Andreas W. W. Ludwig, Phys. Rev. B 78, 195125. (2008)
[5] Y. S. Hor, A. J. Williams, J. G. Checkelsky, P. Roushan, J. Seo, Q. Xu, H. W. Zandbergen, A. Yazdani, N. P. Ong, and R. J. Cava, Phys. Rev. Lett. 104, 057001. (2010)
[6] M. Kriener, Kouji Segawa, Zhi Ren, Satoshi Sasaki, and Yoichi Ando, Phys. Rev. Lett. 106, 127004. (2011)
[7] J. L. Zhang, S. J. Zhang, H. M. Weng, W. Zhang, L. X. Yang, Q. Q. Liu, S. M. Feng, X. C. Wang, R. C. Yu, L. Z. Cao, Lin Wang, W. G. Yang, H. Z. Liu, W. Y. Zhao, S. C. Zhang, X. Dai, Z. Fang and C. Q. Jin, PNAS, 108, 24. (2011)
[8] K. E. Arpino, D. C. Wallace, Y. F. Nie, T. Birol, P. D. C. King, S. Chatterjee, M. Uchida, S. M. Koohpayeh, J.-J. Wen, K. Page, C. J. Fennie, K. M. Shen, and T. M. McQueen, Phys. Rev. Lett. 112, 017002. (2014)

[9] L. Andrew Wray, Suyang Xu, Yuqi Xia, Dong Qian, Alexei V. Fedorov, Hsin Lin, Arun Bansil, Yew San Hor, Robert J. Cava and M. Zahid Hasan, Nature Physics, 6, 855-859. (2010)
[10] J. Zhu, J. L. Zhang, P. P. Kong, S. J. Zhang, X. H. Yu, J. L. Zhu, Q. Q. Liu, X. Li, R. C. Yu, R. Ahuja, W. G. Yang, G. Y. Shen, H. K. Mao, H. M. Weng, X. Dai, Z. Fang, Y. S. Zhao, and C. Q. Jin, Sci. Rep., 3, 2016. (2013)
[11] C. L. Kane and E. J. Mele, Phys. Rev. Lett., 95, 146802. (2005)
[12] B. Andrei Bernevig, Taylor L. Hughes and Shou-Cheng Zhang, Science, 314, 1757. (2006)
[13] M. König, S. Wiedmann, C. Brüne, A. Roth, H. Buhmann, L. W. Molenkamp, X. L. Qi, and S. C. Zhang, Science 318, 766. (2007)
[14] Liang Fu and C. L. Kane, Phys. Rev. B, 76, 045302. (2007)
[15] Shuichi Murakami, New J. Phys., 9, 356. (2007)
[16] D. Hsieh, D. Qian, L. Wray, Y. Xia, Y. S. Hor, R. J. Cava and M. Z. Hasan, Nature, 452, 970. (2008)
[17] M. Z. Hasan and C. L. Kane, Rev. Mod. Phys., 82, 3045. (2010)
[18] Joel Moore, Nature Physics, 5, 378. (2009)
[19] Haijun Zhang, Chao-Xing Liu, Xiao-Liang Qi, Xi Dai, Zhong Fang and Shou-Cheng Zhang, Nature Physics, 5, 438. (2009)
[20] Yoichi Ando, J. Phys. Soc. Jpn., 82, 102001. (2013)
[21] Tong Zhang, Peng Cheng, Xi Chen, Jin-Feng Jia, Xucun Ma, Ke He, Lili Wang, Haijun Zhang, Xi Dai, Zhong Fang, Xincheng Xie and Qi-Kun Xue, Phys. Rev. Lett., 103, 266803. (2009)
[22] Liang Fu and C. L. Kane, Phys. Rev. Lett., 100, 096407. (2008)
[23] Frank Wilczek, Nature Physics, 5, 614. (2009)
[24] Liang Fu and C. L. Kane, Phys. Rev. Lett., 102, 216403. (2009)
[25] R. Akhmerov, Johan Nilsson and C. W. J. Beenakker, Phys. Rev. Lett., 102, 216404. (2009)
[26] Jay D. Sau, Roman M. Lutchyn, Sumanta Tewari, S. Das Sarma, Phys. Rev. Lett., 104, 040502. (2010)
[27] K. T. Law, Patrick A. Lee, T. K. Ng, Phys. Rev. Lett., 103, 237001. (2009)
[28] Ryusuke Kondo, Taiki Yoshinaka, Yoshinori Imai and Atsutaka Maeda, J. Phys. Soc. Jpn., 82, 063702. (2013)
[29] Satoshi Sasaki, M. Kriener, Kouji Segawa, Keiji Yada, Yukio Tanaka, Masatoshi Sato and Yoichi Ando, Phys. Rev. Lett., 107, 217001. (2011)
[30] Pradip Das, Yusuke Suzuki, Masashi Tachiki and Kazuo Kadowaki,
Phys. Rev. B, 83, 220513. (2011)
[31] Jin-Peng Xu, Canhua Liu, Mei-Xiao Wang, Jianfeng Ge, Zhi-Long Liu, Xiaojun Yang, Yan Chen, Ying Liu, Zhu-An Xu, Chun-Lei Gao, Dong Qian, Fu-Chun Zhang and Jin-Feng Jia, Phys. Rev. Lett., 112, 217001. (2014)
[32] J. A. Schneeloch, R. D. Zhong, Z. J. Xu, G. D. Gu and J. M. Tranquada, Phys. Rev. B, 91, 144506. (2015)
[33] Meng Wang, Yanru Song, Lixing You, Zhuojun Li, Bo Gao, Xiaoming Xie and Mianheng Jiang, Scientific Reports, 6, 22713. (2016)
[34] Zhongheng Liu, Xiong Yao, Jifeng Shao, Ming Zuo, Li Pi, Shun Tan, Changjin Zhang and Yuheng Zhang, J. Am. Chem. Soc., 137, 10512. (2015)
[35] Y. S. Hor, J. G. Checkelsky, D. Qu, N. P. Ong and R. J. Cava, J. Phys. Chem. Solids, 72, 572. (2011)
[36] Satoshi Sasaki, Zhi Ren, A. A. Taskin, Kouji Segawa, Liang Fu and Yoichi Ando, Phys. Rev. Lett., 109, 217004. (2012)
[37] Zhiwei Wang, A. A. Taskin, Tobias Frölich, Markus Braden and Yoichi Ando, Chem. Mater., 28, 779. (2016)
[38] K. Matsubayashi, T. Terai, J. S. Zhou and Y. Uwatoko, Phys. Rev. B, 90, 125126. (2014)
[39] 嚴友志，“Sb2Te3-xSex晶體性質探討”，國立中山大學材料與光電科學學系碩士論文 (2017)
[40] G. H. Cao, H. J. Liu, J. H. Liang, L. Cheng, D. D. Fan, Z. Y. Zhang, arXiv, 1607. 05911. (2016)
[41] Rajasekaraumar Vadapoo, Sridevi Krishnan, Hulusi Yilmaz and Carlos Marin, Phys.Status Solidi B, 248, No.3, 7700-705. (2011)
[42] Li Xuelai, Sun Zhimei, Song Zhitang, Rao Feng, Wu Liangcai, Liu Weili, Solid State Sciences, 13, 131-134. (2011)
[43] Guolin Hao, Xiang Qi, Guang Wang, Xiangyang Peng, Shengli Chang, Xiaolin Weia and Jianxin Zhong, RSC Advances, 2, 10694–10699. (2012)
[44] H. Zhang and S. C. Zhang, Phys. Status Solidi-R, 7, 72-81. (2013)
[45] Ilias Efthimiopoulos, Jiaming Zhang, Melvin Kucway, Changyong Park, Rodney C. Ewing and Yuejian Wang, Sci. Rep., 3, 2665. (2013)
[46] Lee, C.-K. et al. Robustness of a Topologically Protected Surface State in a Sb2Te2Se Single Crystal. Sci. Rep. 6, 36538; doi: 10.1038/srep36538 (2016)
[47] Long Ren, Xiang Qi, Yundan Liu. et al. J. Mater. Chen. 22, 4921-4926. (2012)
[48] Jian Yuan, Meng Zhao, Wengzhi Yu, Yao Lu, Caiyun Chen, Meng Xu, Shaojuan Li, Kian Ping Loh and Bao Qiaoliang, Materials, 8(8), 5007-5017. (2015)
[49] Xuchu Ma, Zude Zhang, Xiong Wang, Shutao Wang, Fen Xu and Yitai Qian, Journal of Crystal Growth, 263,491-497. (2003)