本論文使用Ti:sapphire摻鈦藍寶石雷射，對GaSe1-xSx層狀結構進行變溫光致螢光光譜與變溫時間解析螢光光譜量測。GaSe1-xSx 層狀結構光致螢光光譜主要由直接能隙的束縛激子、間接能隙自由激子與間接能隙束縛激子輻射複合造成。不同比例的硫原子摻雜，會使光譜訊號藍移，歸因於硫原子外層電子受到原子核吸引力較大導致導電帶與價電帶的能隙變大，因此螢光光譜才會藍移。隨溫度上升，不同發光機制的非輻射複合活化能分別為: GaSe約14.26meV、11.59 meV 與12.7meV；GaSe0.9S0.1約9.9 meV、15.18meV與4.31meV；GaSe0.8S0.2約17.07 meV、20.62meV與7.67meV；GaSe0.5S0.5約9.56 meV、6.13meV與3.22meV。各樣品的非輻射複合率在溫度上升至100K以上會大幅上升，並主導載子的複合，因此發光強度急遽減弱。

In this thesis, we measured photoluminescence(PL) and time-resolved photoluminescence(TRPL) for GaSe1-xSx layer structure with Mai Tai Ti:sapphire laser at different temperature. Direct bound exciton, indirect free and bound exciton dominate the radiative recombination of GaSe1-xSx layer structure. With different sulfur composition, the peak energy of PL shifts to high energy side. It is attributed to the force of the outside electrons attracted to nucleus of sulfur larger than nucleus of selenium. As temperature increasing, non-radiative recombination active energy for different radiative mechanism are 14.26 meV,11.59 meV and 12.7meV for GaSe；9.9 meV, 15.18 meV and 4.31 meV for GaSe0.9S0.1；17.07 meV, 20.62 meV and 7.67 meV for GaSe0.8S0.2；9.56 meV, 6.13 meV and 3.22 meV for GaSe0.5S0.5. Non-radiative recombination dominates the carrier recombination above 100 K for each sample. As a result, photoluminescence intensity decays rapidly.

論文審定書 i
致謝 ii
摘要 iii
Abstract iv
目錄 v
圖次 vii
表次 x
第一章 導論 1
1.1 文獻回顧 2
第二章 實驗儀器與架設 6
2.1 PicoHarp360 運作原理 6
2.2 單光子計數TCSPC 6
2.3 Avalanche Photo Diode(APD) 8
2.4 Delay box 8
2.5 雷射激發源 9
2.6 TP-2000B Tripler原理 9
2.7 實驗光路架設 10
第三章 載子動力學 12
3.1 載子的複合 13
第四章 分析與討論 16
4.1 樣品介紹 16
4.2 GaSe 層狀結構實驗結果分析 21
4.2.1 GaSe光致螢光光譜 21
4.2.2 GaSe 時間解析螢光光譜 25
4.2.3 GaSe內部量子效應與非輻射複合活化能 29
4.2.4 GaSe輻射與非輻射複合生命週期 31
4.3 GaSe0.9S0.1 層狀結構實驗結果分析 34
4.3.1 GaSe0.9S0.1光致螢光光譜 34
4.3.2 GaSe0.9S0.1時間解析螢光光譜 38
4.3.3 GaSe0.9S0.1內部量子效應與非輻射複合活化能 40
4.3.4 GaSe0.9S0.1輻射與非輻射複合生命週期 40
4.4 GaSe0.8S0.2層狀結構實驗結果分析 40
4.4.1 GaSe0.8S0.2光致螢光光譜 40
4.4.2 GaSe0.8S0.2時間解析螢光光譜 40
4.4.3 GaSe0.8S0.2內部量子效應與非輻射複合活化能 40
4.4.4 GaSe0.8S0.2輻射與非輻射複合生命週期 40
4.5 GaSe0.5S0.5 層狀結構實驗結果分析 40
4.5.1 GaSe0.5S0.5光致螢光光譜 40
4.5.2 GaSe0.5S0.5時間解析螢光光譜 40
4.5.3 GaSe0.5S0.5內部量子效應與非輻射複合活化能 40
4.5.4 GaSe0.5S0.5輻射與非輻射複合生命週期 40
4.6 各樣品實驗結果比較 40
第五章 結論 40
參考資料 40

Geim, A. K. and Novoselov, K. S. “The rise of graphene” Nature Materials. 6. 183 (2007)
Y. Zhang, T. T. Tang, C. Girit, Z. Hao, M. C. Martin, A. Zettl, M. F. Crommie, Y. R. Shen and F. Wang “Direct observation of a widely tunable bandgap in bilayer graphene” Nature. 459. 820 (2009)
K. F. Mak, C. Lee, J. Hone, J. Shan, T. F. Heinz “Atomically thin MoS2: A new direct-gap semiconductor” Phys. Rev. Lett. 105. 136805 (2010)
S. Bertolazzi, D. Krasnozhon, and A. Kis “Nonvolatile Memory Cells Based on MoS2/Graphene Heterostructures” ACS Nano. 7. 3246 (2013)
W. I. Milne and J. C. Anderson “Threshold switching in gallium telluride single crystals” J. Phys. D: Appl. Phys. 6. 2115 (1973)
H. Huang, P. Wang, Y. Gao, X. Wang, T. Lin, J. Wang, L. Liao, J. Sun, X. Meng, Z. Huang, X. Chen and J. Chu, “Highly sensitive phototransistor based on GaSe nanosheets” Appl. Phys. Lett. 107. 143112 (2015)
P. J. Ko, A. Abderrahmane, T. Takamura, N. H. Kim and A. Sandhu “Thickness dependence on the optoelectronic properties of multilayered GaSe based photodetector” Nanotechnology. 27. 325202 (2016)
陳欣宏 “硫化鎵之晶體成長及光學特性研究” 國立臺灣科技大學應用科技研究所碩士論文 (2013)
Ho, C. H., and K. W. Huang. "Visible luminescence and structural property of GaSexS1-x (0≤ x≤ 1) series layered crystals." Sol. State. Commun. 136. 591 (2005)
P. A. Hu, Z. Wen, L. Wang, P. Tan, and K. Xiao “Synthesis of Few-Layer GaSe Nanosheets for High Performance Photodetectors” ACS Nano. 6. No.7 5988 (2012)
O. Del. Pozo-Zamudio, S. Schwarz1, M. Sich, I. A. Akimov, M. Bayer, R. C. Schofield, E. A. Chekhovich, J. Robinson, N. D. Kay, O. V. Kolosov, A. I. Dmitriev, G. V. Lashkarev, D. N. Borisenko, N. N. Kolesnikov and A. I. Tartakovskii "Photoluminescence of two-dimensional GaTe and GaSe films." 2D Mater. 2. 035010. (2015)
C. Wei, X. Chen, D. Li, H. Su, H. He and J. F. Dai “Bound exciton and free exciton states in GaSe thin slab” Sci. Rep. 6. 33890 (2016)
C.C. Wu, C.H. Ho, W.T. Shen, Z.H. Cheng, Y.S. Huang, K.K. Tiong “Optical properties of GaSexS1-x series layered semiconductors grown by vertical Bridgman method” Mater. Chem. Phys. 88. 313 (2004)
C. Pérez León and L. Kador, K. R. Allakhverdiev, T. Baykara, and A. A. Kaya “Comparison of the layered semiconductors GaSe, GaS, and GaSe1-xSxby Raman and photoluminescence spectroscopy” J. Appl. Phys. 98. 103103 (2005)
J. C. J. M. Terhell, V. A. M. Brabers And G. E. Van Egmond “Polytype Phase Transition in the Series GaSe1-xSx” J. Solid. State. Chem. 41. 97 (1982)
V. Capozzi, S. Caneppele, M. Montagna, and F. Levy “Radiative Decay from Free and Bound Excitons in GaSe” Phys. stat. sol. (b). 129. 247 (1985)
V. Capozzi and M. Montagna “Optical spectroscopy of extrinsic recombinations in gallium selenide” Phys. Rev. B. 40. 5 (1989)
R. A. Taylor and J. F. Ryan “Time-resolved exciton photoluminescence in GaSe and GaTe” J. Phys. C: Solid State Phys. 20. 6175 (1987)
王湘富 “氮化銦鎵多重量子井發光二極體之輻射結合與硒化鎂鋅薄膜之螢光光譜研究” 國中山大學物理研究所碩士論文 (2012)
J. Shah, ”Ultrafast Spectroscopy of Semiconductors and Semiconductor Nanostructures”,Second enlarged edition, (Springer) (1999)
曾耀功 ”氮化銦薄膜的載子冷卻研究” 國中山大學物理研究所碩士論文 (2009)
P. Fielding, G. Fischer And E. Mooser “Semiconductors of the type AIIIBVI” J. Phys. Chem. Solids 8. 434 (1959)
D. J. Late, B. Liu, J. Luo, A. Yan, H. S. S. Ramakrishna Matte, M. Grayson, C. N. R. Rao and V. P. Dravid “GaS and GaSe Ultrathin Layer Transistors” Adv. Mater. 24. 3549 (2012)
K. Yanagisawa, N. Kuroda and Y. Nishina “ Electroluminescence in GaSe1-xSx crystals” J. Phys. Soc. Japan. 37. 1180 (1974)
0. L. Belenkii, R. KH. Nani, E. Yu. Salaev and R. A. Suleiman “Edge Luminescence and Light Absorption in GaSxSe1-x Solid Solutions at Low Temperatures” Phys. stat. sol. (a) 31. 707 (1975)
Y. P. Varshni "Temperature dependence of the energy gap in semiconductors." Physica 34. 149 (1967)
L. Liu, L. Wang, D. Li, N. Liu, L. Li, W. Cao, W. Yang, C. Wan, W. Chen, W. Du, X. Hu and Z. C. Feng “Influence of indium composition in the prestrained InGaN interlayer on the strain relaxation of InGaN/GaN multiple quantum wells in laser diode structures” J. Appl. Phys. 109. 073106 (2011)
S. W. Jung, W. I. Park, H. D. Cheong, Gyu-Chul Yi and Hyun M. Jang “Time-resolved and time-integrated photoluminescence in ZnO epilayers grown Al2O3 (0001) on by metalorganic vapor phase epitaxy” Appl. Phys. Lett. 80. 1924 (2002)
A. R. Denton and N. W. Ashcroft “Vegard's law” Phys. Rev. A. 43. 3161 (1991)