摘要

本篇論文重點探討過渡金屬和稀土離子摻雜的無機鉛鹵素鈣鈦礦磷光體。目前，磷光體被認為是具有很高研究潛力的材料，在生物醫學應用和固態照明等多個領域表現出色，這要歸功於它們的高發光效率、耐熱性、化學穩定性和長壽命。磷光體材料的特點是它們具有能量轉移機制，使得其發射釋放具有高相對色溫和演色數值的白光輻射。含有磷光體的材料由基材和活化劑組成。可以考慮的基材通常包括氮化物、氧化物、氧氮化物、硒化物、硫化物、硅酸鹽或無機鉛鹵化物。此外，有機無機鉛鹵素鈣鈦礦是一種可調色磷光體，因為它們具有混合鹵化物的能力。然而，使用無機鉛鹵素鈣鈦礦具有很大挑戰，因為它們容易熱降解。為了克服這個問題，摻雜稀土和過渡金屬離子是一種替代方法。
在我們的第一項研究中，我們使用溫度相關光致發光（PL）和時間解析光致發光（TR-PL）來研究Cr摻雜CsPbCl3的載子復合機制。由於Cr摻雜的非均勻性，觀察到激子局部區域化現象。這一特性不僅可以在溫度相關光致發光中觀察到，其中在低於100 K的溫度下發射強度迅速增加，而且也可以在溫度相關的時間解析光致發光中觀察到，其中在20 K至100 K的溫度範圍內，輻射壽命的溫度相關性呈現線性依賴關係。
此外，不同溫度下的時間解析光致發光光譜結果顯示，輻射和非輻射復合的壽命在20 K至300 K之間有所變化。輻射復合壽命的變化與非輻射復合速率一致，而非輻射復合壽命的變化與低室溫下鈣鈦礦的內部量子效率相符。這些發現表明，存在一種簡單的計算內部量子效率的方法，可用於與基於溫度相關光致發光測量的傳統方法相關聯。此外，還研究了20 K下，Cr摻雜CsPbCl3鈣鈦礦之光致發光衰變壽命作為控制放光能量的函數。結果表明，Cr摻雜CsPbCl3鈣鈦礦激子具有很高的局部區域化程度（Eloc）。本文使用的方法有望為研究無機鉛三鹵化物鈣鈦礦放光性能方面的特性開辟具有巨大表徵能力的新途徑。
在第二項研究中，溫度相關光致發光（PL）和時間解析光致發光（TR-PL）也被用來研究Eu摻雜CsPbBr3中束縛和自由激子的復合機制。周圍熱浴中能量的缺失以及溫度的降低導致激子的捕捉增加和束縛激子的形成。當溫度從300 K降至10 K時，束縛激子的放光強度明顯降低。束縛激子的放光強度在T = 100 K時出現，並隨著溫度降至10 K迅速增加。這是由於更豐富的Eu3+離子導致束縛激子和自由激子之間的熱能動態遷移。通過分析不同激發功率下的光致發光光譜，可以證明Eu摻雜CsPbBr3的激子般發射。此外，溫度相關之時間解析光致發光被用來確定束縛激子的輻射和非輻射復合。分別在10 K、60 K和90 K下研究了Eu摻雜CsPbBr3鈣鈦礦磷光體中光致發光壽命與放光能量以及束縛激子PL光譜，以確定束縛激子的局部區域化程度隨溫度降低而提高。另一方面，隨著溫度降低，束縛激子的局部區域深度（Eloc）增加。因此，束縛激子強度的增加是由於局部區域深度隨溫度降低而增加所引起的。

Abstract

This thesis highlights about transition metal and rare earth ion-doped inorganic lead halide perovskite phosphors. Currently, Phosphors are generally considered materials that appear to be very promising in a variety of fields of research, including biomedical applications and solidstate lighting, due to their high efficiency of luminescence, resistance to heat, chemical stability, and long lifetime. A mechanism for transferring energy, which allowing their emission to release white light radiation with a high CCT and CRI is the profile features of phosphor materials. Materials containing phosphors are made up of host materials and activators. The host materials that can be considered are typically nitrides, oxides, oxynitrides, selenides, sulfides, silicates or inorganic lead halides. Furthermore, organic-inorganic lead halide perovskites one of color tunable phosphors due to the mixing capability of halides. However, using inorganic lead halide perovskites is very challenging due to their thermal degradation. To overcome this problem, doping rare earth and transition metal ions is one of the alternative methods.
In our first work temperature-dependent-photoluminescence (PL) and time-resolved-PL (TR-PL) were used to examine the carrier recombination mechanism of Cr-doped CsPbCl3. Exciton localization is observed as a result of non-uniform Cr doping. This property can be seen not only in temperature-dependent-PL, where the intensity of emission increases rapidly at temperatures below 100 K, but also in temperature-dependent-TR-PL, where radiative lifetime temperature dependence at temperatures ranging from 20 K - 100 K shows a linear dependence.
Furthermore, the results of TRPL spectroscopy at various temperatures reveal that both Lifetimes of radiative and non-radiative recombination vary from 20 K to 300 K. The variation in the lifetime of radiative recombination is consistent with the non-radiative recombining rate, whereas the non-radiative recombining lifetime variation is compatible with the internal quantum efficiency of perovskite from low room temperature. These findings imply that there is a simple method for calculating internal quantum efficiency that can be used in related to the traditional method based on temperature-dependent photoluminescence measurement. Besides, the Cr-doped CsPbCl3 perovskite PL decay lifetimes at 20 K are investigated as a function of controlling emission energies. The results show that the Cr-doped CsPbCl3 perovskite excitons have a high degree of localization (Eloc). The methods used in this paper are expected to open up new paths with tremendous characterization capability for studying inorganic lead trihalide perovskites' properties in terms of emission.
In the second work, temperature-dependent-PL and TR-PL were also used to examine the recombination mechanisms of excitons, both bound and free, in Eu-doped CsPbBr3. The lack of energy in the surrounding thermal bath coupled with a decrease in temperature causes a rise in the trapping of excitons and the formation of bound excitons. The emission intensity of bound excitons decreases noticeably as the temperature drops from 300 K - 10 K. The bound exciton emission intensity appears at T = 100 K and rapidly increases as the temperature decreases to 10 K. This is due to the richer Eu3+ ion causing dynamic migration of thermal energy between bound excitons and free excitons. The exciton-like emission of Eu-doped CsPbBr3 can be demonstrated by analyzing the PL spectra under different excitation powers. Besides, the temperature-dependent TR-PL was used to determine the radiative and non-radiative recombination of the bound exciton. The PL lifetime versus emission energy, as well as bound exciton PL spectra in Eu-doped CsbBr3 perovskite phosphor at 10 K, 60 K, and 90 K, respectively were studied to confirm the degree of localization of bound exciton raise as the temperature drops. On the other hand, as the temperature drops, the localization depth (Eloc) of bound excitons increases. As a result, a rise in intensity of bound exciton is caused by the localization depth increasing with decreasing temperature.

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