近幾年關於金屬鹵化物鈣鈦礦材料的研究蓬勃發展，不過在眾多研究中，此材料的形貌多數呈現正方體或四角板。有鑑於此，本篇研究發展了新的方法，合成出不同型貌的CsPbCl3晶體，由於形貌的改變，其顯露的晶面也隨之改變。不同以往，此方法不需使用常用的吸附劑，例如接有長碳鏈的胺類以及羧酸，而是使用離子型的介面活性劑十二烷基硫酸鈉，且在室溫下即可進行反應。當前驅物CsCl與PbCl2的莫耳比例為1:1時，可合成出立方體形狀的CsPbCl3晶體，顯露的晶面為四個{100}以及兩個{001}晶面，當CsCl與PbCl2的比例上升至1:1.6時，則形成截邊長方體，暴露出四個{100}、兩個{001}、四個{110}以及八個{011}晶面。這種改變前驅物比例進而影響暴露之晶面的現象，可用熱力學的過飽和參數Δμ來解釋之。透過XRD的分析，兩種形狀的CsPbCl3晶體，皆為四方晶系，立方體的尺寸為50到155奈米之間，而截邊長方體則在130至400奈米之間。尺寸較小的立方體其光致發光量子產率幾乎為尺寸較大之截邊長方體的2.4倍，且當形狀從立方體轉變為截邊長方體時，其載子生命週期從1.36奈秒降至0.65奈秒，顯示了光學上的晶面效應。

Highly popular luminescent metal halide perovskites have been extensively studied recently. However, the shapes of crystals are mostly confined to six-faceted cubes and platelets. Here novel CsPbCl3 crystals with tunable morphologies and exposed facets have been synthesized in DMSO at room temperature without adding typical capping agents such as long carbon chain amines and carboxylic acids. Instead, ionic surfactant SDS was used in the reaction. CsPbCl3 cubes exposing four {100} and two {001} facets can be obtained at a CsCl to PbCl2 molar ratio of 1:1, while edge-truncated cuboids exposing four {100}, two {001}, four {110}, and eight {011} facets were produced at a CsCl:PbCl2 molar ratio of 1:1.6. The supersaturation parameter Δμ can be used to explain the appearance of higher surface energy facets with changing mole ratios. XRD analysis shows both the cubes and edge-truncated cuboids have a tetragonal crystal structure. The smaller cubes with sizes in the range 50 to 155 nm show almost 2.4 times higher photoluminescence quantum yield than the larger edge-truncated cuboids with sizes from 130 to 400 nm, and the average emission lifetime decreases from 1.36 to 0.65 ns as particle shape changes from cubes to edge-truncated cuboids. The result shows facet-dependent optical properties.

論文摘要..........................................I
ABSTRACT ........................................II
ACKNOWLEDGEMENT ................................ III
TABLE OF CONTENTS .............................. IV
LIST OF FIGURES ................................ VI
LIST OF SCHEMES ................................ XII
LIST OF TABLES ................................. XIII
Chapter 1 Introduction ......................... 1
1.1 Facet- and size-dependent optical properties of Cu2O nanocrystals .............. 1
1.2 Metal halide perovskites ..................... 4
1.2.1 Hot injection (HI) method .................. 5
1.2.2 Ligand-assisted reprecipitation (LARP) approach .............................11
1.2.3 Advantages and disadvantages of the hot injection (HI) method and the ligand-assisted reprecipitation (LARP) approach ............................. 15
1.3 Cesium lead chloride ............................................... 15
Chapter 2 Synthesis of CsPbCl3 cubes and edge-truncated cuboids at room temperature .............................. 22
2.1 Experimental section ............................................... 24
2.1.1 Chemicals ............................... 24
2.1.2 Instrumentation ............................................... 24
2.1.3 Synthesis of CsPbCl3 nanocrystals with tunable shapes .................... 25
2.2 Results and discussion ............................................... 27
2.2.1 Exposed facets in a tetrahedral crystal ............................................... 27
2.2.2 Scanning electron microscopy (SEM) ............................................... 29
V
2.2.3 Powder X-ray diffraction (PXRD) patterns ............................................... 32
2.2.4 Transmission electron microscopy (TEM) ........................................ 34
2.2.5 Energy-dispersive X-ray spectroscopy (EDS) ................................... 36
2.2.6 X-ray photoelectron spectroscopy (XPS) .......................................... 38
2.2.7 Thermodynamic theory support ........................................... 43
2.2.8 Facet and size effects in optical properties ........................................ 51
2.3 Conclusion ......................... 60
REFERENCES ............................. 61

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