2019-08-142024-05-17https://scholars.lib.ntu.edu.tw/handle/123456789/672027摘要：本研究規劃為兩年期之跨國性合作計畫，擬透過國立台灣大學 (National Taiwan University, NTU) 與美國阿貢國家實驗室 (Argonne National Laboratory, ANL) 多位研究成員的密切合作，並同時獲得洛斯阿拉莫斯國家實驗室 (Los Alamos National Laboratory, LANL) 研究團隊的支援，期盼能解決目前二維層狀鈣鈦礦(two-dimensional layered perovskites) 的低電荷傳導之瓶頸，藉以大幅提升相關光電元件 (如:光伏元件、發光二極體等) 的工作效能，並透過材料結構設計，保持它們的優異穩定性，進而開發出具有高效率與高穩定性之鈣鈦礦光電元件。具體而言，我們首先將設計和合成新穎的共軛型有機陽離子 (π-conjugate organic cation) 分子，並應用於製備二維層狀鈣鈦礦，其將有助於增加無機層間的電荷轉移。然後，藉由調控分子間的相互作用力和溶劑工程法，使得層狀鈣鈦礦形成垂直取向 (out-of-plane) 的晶體排列，此外，我們將導入有機二銨鹽來降低Ruddlesden-Popper (RP) 相中所產生的凡得瓦 (Van der Waals) 間隙之厚度，提升層間的電荷傳導能力，同時增加二維層狀鈣鈦礦結構的穩定性。另一方面，我們亦將應用本團隊近期開發的脫層蒙托土 (exfoliated montmorillonite, exMMT) 引入新設計的含氟有機陽離子至二維層狀鈣鈦礦系統中，防止有機離子的逃逸及水氣的入侵而產生結構的劣化與崩解。本研究工作之執行，將能更深入了解二維層狀鈣鈦礦系統中，分子結構與組成/晶體型態/光電特徵之間的相關性，並建立各種環境因素所引起的元件功能劣化機制。此等成果將有助於開發新一代高效能的鈣鈦礦光電元件。<br> Abstract: This two-year program aims to resolve the charge transport bottleneck in two-dimensional (2D) layered perovskites to greatly enhance their optoelectronic device performance (i.e. for photovoltaic and light emitting diodes) while maintaining their superior stability through material structural design. We will build a strong collaboration between the experts and scientists from National Taiwan University (Taiwan) and Argonne National Laboratory (U.S.A), and the support from our prestigious collaborators at Los Alamos National Laboratory that ensures the success of the proposed project. Specifically, we will first design and synthesize π-conjugate organic monocations/dications incorporated into the 2D layered perovskite structure that enhances the charge transfer between inorganic cages, and then grow a well-aligned crystalline thin film with out-of- plane orientation via molecular interaction and solvent engineering. The use of organic diammonium may further reduce the thickness of organic spacer sandwiched between inorganic slabs. Moreover, we will utilize our recently developed approach that employs fluorine-containing organic cations in 2D perovskite system to further protect the ion from escaping or degradation by moisture. This work anticipates establishing a comprehensive knowledge on the relationships among molecular structure, morphology and optoelectronic property for 2D layered perovskites and the degradation mechanisms caused by various environmental factors. Such design principles are critical to guide the effort towards high performance device applications.鈣鈦礦載子遷移率二維材料Perovskitecarrier mobility2D materials