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研究生：	吳俊陞 Wu, Chun-Sheng
論文名稱：	銫鉛溴化物鈣鈦礦高品質微米半球共振腔之單模雷射研究 High-Quality Single-Mode Laser Based on Cesium Lead Bromide Perovskite Hemisphere Microcavity
指導教授：	徐旭政 Hsu, Hsu-Cheng
學位類別：	碩士 Master
系所名稱：	理學院 - 光電科學與工程學系 Department of Photonics
論文出版年：	2019
畢業學年度：	108
語文別：	英文
論文頁數：	78
中文關鍵詞：	銫鉛溴化物、鈣鈦礦、單模雷射、耳語迴廊模態、柏塞爾效應、自發輻射耦合因子
外文關鍵詞：	CsPbBr3, Perovskite, Single-mode laser, Whispering Gallery Mode, Purcell effect, Spontaneous emission coupling factor
相關次數：	點閱：71 下載：6
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具有極高品質因子單模雷射被實現於本文中之銫鉛溴化物鈣鈦礦微米半球，本文為世界上首次於銫鉛溴化物鈣鈦礦系統中展示一系列共振腔相關之詳細雷射特性研究。
在本論文中，我們成功地以化學氣相沉積儀成長大小可變之銫鉛溴化物鈣鈦礦微米半球。半高寬約為0.04 奈米；品質因子約為13673 之單模雷射成功於具備高光束縛因子與高光學增益的銫鉛溴化物鈣鈦礦微米半球微共振腔中達成。
為了更深入探討共振腔對雷射特性的影響，我們展示了雷射閥值對於不同共振腔大小之研究，在實驗中我們發現隨著共振腔半徑縮小，雷射閥值會上升。而其之間的關係可以用Gth ∝ 1/R^2 關係式來做擬合。另外，我們也完成不同大小之共振腔的時間解析螢光光譜，用以進一步驗證上述之共振腔大小與雷射閥值的關係。在此實驗我們發現較大的共振腔具有較長的螢光壽命，利用雷射的載子速率方程式我們可以得出較長螢光壽命者較容易達成雷射，此結論與最初之結論相吻合。除此之外，我們認為在本系統中也應考慮柏塞爾效應的影響，所以我們也進行了在不同共振腔大小中計算柏塞爾因子與自發輻射增強因子的大小。
最後，除了銫鉛溴化物，我們也同時也在銫鉛氯化物與銫鉛碘化物微米球共振腔系統中展示了單模雷射現象。

Ultra high-Q single-mode laser is realized in individual Cesium Lead Bromide (CsPbBr3) perovskite micro-hemispheres. Cavity size-dependence lasing property analysis is first reported under this material system. In this work, we fabricated high quality CsPbBr3 microhemispheres via chemical vapor deposition method with tunable sizes. Due to the good
optical confinement capability of the whispering gallery resonanted cavity and high optical gain of CsPbBr3 Perovskite, single-mode lasing has been achieved with a linewidth (〜 0.04 nm) and ultra high quality factor (about 13673) in CsPbBr3 micro-hemispheres. To indepth study the physical effects between the lasing threshold and the cavity, a series of cavity size-dependence photoluminescence analysis were done. From the size-dependence lasing threshold measurement, we discovered that the lasing threshold increases while the cavity size decreases, and the relation is well fitted by the Gth ∝ 1/R2. The time-resolved PL analysis was also performed to further confirm the size-dependence lasing threshold relation. The larger cavity stands for longer PL lifetime and indicating easier to achieve carrier population inversion. The Purcell effect should also be considered in the microcavity system.
We investigated the Purcell factor and the spontaneous emission coupling factor in different sizes of cavities. At last, we also realized single-mode lasing action in CsPbI3 and CsPbCl3 Perovskite micro-spheres.

摘要i
Abstract ii
誌謝iii
Table of Contents iv
List of Tables vi
List of Figures vii
Chapter 1. Introduction 1
1. Preface . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
2. Historical Review . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.1. WGM Microcavity Laser . . . . . . . . . . . . . . . . . . . . . . . 3
2.2. Perovskite . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
3. Motivation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
Chapter 2. Physical Theories 12
1. Material properties of CsPbX3 Perovskite . . . . . . . . . . . . . . . . . . 12
1.1. Crystal Structure . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
1.2. Point Defect in CsPbBr3 . . . . . . . . . . . . . . . . . . . . . . . 15
2. Optical Properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
2.1. Basic Optical Properties . . . . . . . . . . . . . . . . . . . . . . . 17
2.2. Photo-luminescence . . . . . . . . . . . . . . . . . . . . . . . . . . 19
3. Lasing in CsPbBr3 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21
3.1. Carrier Dynamic in CsPbBr3 . . . . . . . . . . . . . . . . . . . . . 21
4. Microcavity . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
4.1. WGM Resonance . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
4.2. Single-Longitudinal-Mode . . . . . . . . . . . . . . . . . . . . . . 24
4.3. Purcell Effect . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26
4.4. Spontaneous Emission Coupling Factor . . . . . . . . . . . . . . . 26
Chapter 3. Experimental Setups 28
1. Synthesis of Perovskite Mirocrystals . . . . . . . . . . . . . . . . . . . . . 28
1.1. Chemical Vapor Deposition . . . . . . . . . . . . . . . . . . . . . . 28
2. Material Physical Characteristic Measurements . . . . . . . . . . . . . . . 31
2.1. Scanning Electron Microscope (SEM) . . . . . . . . . . . . . . . . 31
2.2. X-ray Diffraction (XRD) . . . . . . . . . . . . . . . . . . . . . . . 33
3. Optical Properties Measurements . . . . . . . . . . . . . . . . . . . . . . . 35
3.1. Micro Photoluminescence Spectroscopy (micro-PL) . . . . . . . . . 35
3.2. Time-Correlated Single Photon Counting System (TCSPC) . . . . . 37
3.3. Optical UV-VIS Absorption . . . . . . . . . . . . . . . . . . . . . 40
Chapter 4. Results and Discussions 41
1. Morphology and Structure . . . . . . . . . . . . . . . . . . . . . . . . . . 41
1.1. Optical Images . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41
1.2. Scanning Electron Microscope (SEM) Images . . . . . . . . . . . . 42
1.3. XRD Anaylsis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 43
2. Basic Optical Properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . 44
2.1. Optical Absorption . . . . . . . . . . . . . . . . . . . . . . . . . . 44
2.2. Steady-State PL . . . . . . . . . . . . . . . . . . . . . . . . . . . . 45
3. Lasing Action Analysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . 47
3.1. Cavity Size-Dependence Free Spectral Range (FSR) . . . . . . . . 47
3.2. Single-Mode Lasing Spectra . . . . . . . . . . . . . . . . . . . . . 49
3.3. Size-Dependence Lasing Threshold Anaylsis . . . . . . . . . . . . 51
3.4. Size-Dependence Time-Resolved PL Anaylsis . . . . . . . . . . . . 56
3.5. Size-Dependence Purcell Factor Anaylsis . . . . . . . . . . . . . . 59
3.6. Size-Dependence Spontaneous Emission Coupling Factor Anaylsis . 61
3.7. Modulation of Single-Mode Lasing Position . . . . . . . . . . . . . 65
4. Comparison Bwtween CsPbX3 (X = Cl -, Br -, I -) . . . . . . . . . . . . . . 66
4.1. Material Anaysis . . . . . . . . . . . . . . . . . . . . . . . . . . . 66
4.2. Optical Property and Performance . . . . . . . . . . . . . . . . . . 67
Chapter 5. Summary 71
1. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 71
References 72

                                    

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