近年來，鉛鹵化物鈣鈦礦 (Pb-based halide perovskites) 引起人們的注目。由於鉛鹵化物鈣鈦礦擁有不凡的物理特性，例如:優異的發光效率、較高的激子束縛能和可調變的發光波長…等。是故它們被廣泛應用於各式的發光元件，如:發光二極體和雷射元件。然而，鉛離子的毒性卻成為這類鈣鈦礦的致命傷，產生破壞環境生態及對生物有害的隱憂，進而對其發展產生極大的阻礙。為此，無數的科學家以製作出對環境友善及低毒性的鈣鈦礦材料為目標，日以繼夜地研究及改良。在繁多的無鉛鈣鈦礦材料中，錫鹵化物鈣鈦礦 (Sn-based halide perovskites) 嶄露頭角，成為備受期待的新星。相較於鉛鹵化物鈣鈦礦，錫鹵化物鈣鈦礦擁有較低的毒性，被認為能有效降低對環境及生物的有害程度。此外，由於錫和鉛屬於同族元素，因此錫鹵化物鈣鈦礦擁有和鉛鹵化鈣鈦礦相似的晶體結構。同時，錫鹵化物鈣鈦礦也展現出類似鉛鹵化物鈣鈦礦的物理特性。值得一提的是，錫鹵化物鈣鈦礦分解後會形成對環境傷害較低的二氧化錫 (SnO2)，因此這類鈣鈦礦也被視為「綠色材料」。是以錫鹵化物鈣鈦礦成為未來發展高效能無鉛鈣鈦礦發光元件之有力候選人。
在各式錫鹵化鈣鈦礦材料中，碘化錫銫和溴化錫銫展現了不亞於鉛鹵化物鈣鈦礦的物理特性，如:優異的對熱穩定性 (thermal stability) 和更高的載子遷移能力(charge carrier mobility)。目前，對於碘化錫銫和溴化錫銫的研究大都著重在電性，對於它們的光學性質的討論仍舊稀少。因此，本論文針對碘化錫銫 (orthorhombic-phase B-γ-CsSnI3) 鈣鈦礦薄膜及溴化錫銫 (cubic-phase α-CsSnBr3) 鈣鈦礦微米結構(方盤及角錐)之材料性質及在一般環境(ambient condition)中的光致發光 (photoluminescence) 特性進行系統化的研究。研究所用的碘化錫銫鈣鈦礦薄膜及溴化錫銫鈣鈦礦微米結構皆透過化學氣相沉積法 (chemical vapor deposition) 製作而成。在第一部分，我們對碘化錫銫鈣鈦礦薄膜進行系統化的材料及光致發光特性分析。所有的光致發光特性量測皆在無封裝狀態下，於大氣環境中完成。使用化學氣相沉積法製成的碘化錫銫鈣鈦礦薄膜在大氣環境中擁有優異且穩定的光致發光表現。在改變激發雷射光強度之光致發光光譜量測中，我們觀察到來自於碘化錫銫鈣鈦礦薄膜的近紅外光雷射。透過不同觀測角度的雷射光譜量測，確認此一雷射為隨機雷射。利用快速傅立葉分析，我們求得此隨機雷射之有效光學共振腔長度。而在不同觀測角度所量測到的隨機雷射，展現出相異的有效光學共振腔長度，再次證明碘化錫銫鈣鈦礦雷射為隨機雷射。
在第二部分，我們對溴化錫銫鈣鈦礦微米結構(方盤及角錐)的材料特性及一般環境中的光致發光性質進行系統化的研究，並著重在溴化錫銫鈣鈦礦微米結構於高溫環境中的光致發光特性。與第一部分相同，所有的光致發光特性量測皆在無封裝狀態下，於大氣環境中完成。首先，我們針對溴化錫銫鈣鈦礦微米結構在常溫環境之光致發光特性進行分析。此類溴化錫銫鈣鈦礦微米結構於常溫環境展現了非凡且穩定的光致發光特性。無論是利用短波長(532奈米)或是長波長(940奈米)雷射光源進行激發，溴化錫銫鈣鈦礦微米結構皆展現優異的發光表現。同時，我們於溴化錫銫鈣鈦礦微米方盤中觀測到耳語迴廊 (whispering gallery mode) 共振膜態，且在溴化錫銫鈣鈦礦微米角錐中量測到放大自發輻射 (amplified spontaneous emission) 現象。這些結果證明溴化錫銫鈣鈦礦微米結構擁有優異的光學特性。接著，我們對溴化錫銫鈣鈦礦微米結構進行加熱，並觀察其光致發光的表現。由於熱效應的緣故，溴化錫銫鈣鈦礦微米方盤和角錐之光致發光強度皆隨著溫度上升而下降。同時，發光波長則隨著溫度上升，呈現明顯的藍移現象，此一現象源自於emphanisis的特殊現象。隨著溫度遞增，光致發光的線寬 (spectral linewidth) 也逐步變寬，此現象歸因於劇烈的電子與聲子之交互作用 (electron−longitudinal optical (LO) phonon interaction)。利用阿瑞尼士方程式 (Arrhenius equation)，我們估算出一活化能，用以評估由熱效應引發的非輻射複合的現象。溴化錫銫鈣鈦礦微米方盤和角錐之活化能皆超過310毫電子伏特 (meV)，大於在溴化鉛銫所觀測到的數值，證明了溴化錫銫鈣鈦礦在高溫環境中擁有優於鉛鹵化物鈣鈦礦的發光特性。

In recent years, Pb-based halide perovskites with high defect tolerance have shown favorable physical properties, such as high photoluminescence quantum yields (PLQYs), high exciton binding energy, and wavelength-tunable emission in entire visible-light region, etc. With these properties, they have been extensively applied in luminescent devices. Regrettably, the toxicity of Pb2+ results in a great concern that could hinder the developments of Pb-based halide perovskite luminescent devices, such as light-emitting diodes (LEDs) and lasers. As a result, it is important to find eco-friendly and low-toxicity replacements for Pb2+. Over the past few years, Sn2+ has been reported to be substituted for Pb2+. The crystalline structure of Sn-based halide perovskites is similar to that of Pb analogues because Sn and Pb are in the same main group. Moreover, Sn-based halide perovskites present the physical properties similar to that of Pb-based ones. It is worth mentioning that Sn-based halide perovskites have the environmentally friendly degradation, SnO2, which makes them regarded as “green material”. Therefore, Sn2+ is a suitable candidate for the replacement for Pb2+.
Among various Sn-based halide perovskites, CsSnI3 and CsSnBr3 show impressive physical properties comparable to or sometimes even superior to those observed in Pb analogues, such as better thermal stability and higher charge carrier mobilities. So far, most studies in CsSnI3 and CsSnBr3 focus on their electrical properties. Their optical properties have not been fully understood yet. Therefore, the aim of this thesis is to explore the photoluminescence (PL) properties of orthorhombic-phase B-γ-CsSnI3 films and cubic-phase α-CsSnBr3 microsqaures and micropyramids under ambient condition.
Both B-γ-CsSnI3 films and α-CsSnBr3 microstructures reported in this thesis are synthesized on mica substrates through chemical vapor deposition (CVD). In the first part, the systematic PL experiments are performed to investigate the PL characteristics of B-γ-CsSnI3 films. The B-γ-CsSnI3 films exhibit decent PL performances under ambient condition without encapsulation. In the optical absorption and PL measurements, the band-edge absorption of B-γ-CsSnI3 film at 950 nm (~1.3 eV) is compatible with the PL emission, which suggests a band-to-band luminescence. Moreover, the B-γ-CsSnI3 film exhibits the stable PL emission for 70 min. In the fluence-dependent PL measurements, as excitation fluence was above 18 mJ/cm2, the near-infrared lasing behavior from the film is observed under ambient condition. The B-γ-CsSnI3 laser exhibits the quality factor (Q) over 3000. By means of the lasing measurements of B-γ-CsSnI3 film in various detected configurations, the B-γ-CsSnI3 laser is classified as a random laser. The effective optical length for B-γ-CsSnI3 random lasers is estimated through the Fourier-transform analysis. Furthermore, the estimated effective optical cavity lengths observed in various detected configurations are different, which is the typical feature of random lasers.
In the second part, the thermal PL quenching behavior of α-CsSnBr3 microsquares and micropyramids upon temperature increase are investigated systematically besides the typical PL properties. Both microstructures show impressive PL performances under ambient condition without encapsulation. In optical absorption and PL measurements, the PL emission of α-CsSnBr3 microsquare at 688.3 nm is in agreement with the band-edge absorption, which indicates a band-to-band luminescence. Furthermore, both microstructures show the stable PL emission for 480 min. In two-photon excited PL experiments, whispering gallery modes (WGMs) due to constructive interference are formed in the microsquares, and amplified spontaneous emission (ASE) takes place in the micropyramids. The high-temperature-dependent PL measurements help to understand the mechanism of reversible PL losses upon temperature increase for both α-CsSnBr3 microstructures. Monotonic blue shifts observed in PL emission with increasing temperature indicates a band-gap widening correlated with an emphanisis effect which results from the Sn2+ off-centering displacement. The analysis of spectral linewidth at elevated temperature for both samples reveals a linewidth broadening because of the dominant electron−longitudinal optical (LO) phonon interaction. Through the Arrhenius equation, the activation energy of thermally assisted nonradiative recombination for α-CsSnBr3 microsquares and micropyramids are estimated. Both microstructures possess the activation energy over 310 meV which is greater than CsPbBr3 (246 meV) in previous study. These results reveal that the PL properties of α-CsSnBr3 at high temperature are superior to that of Pb-based halide perovskites.

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