本論文分別針對有機鹵化鉛鈣鈦礦太陽能對電池吸光層鈣鈦礦材料的製備與電極界面層於元件效能的影響作探討。在第一項工作中，我們利用電噴塗法沉積固態的前驅物晶體於基板上並探討其轉變成斜方晶甲基碘化鉛鈣鈦礦薄膜的形成機制，以電噴塗法所製備的固態晶體改善了塗佈法成膜時候的去濕潤現象。經調變電噴塗過程中施加的電壓可得到合適晶粒尺寸的固態反應物，並在穩定熱源下進行鹵素交換形成連續的薄膜，此電噴塗技術並配合後續固態反應機制的成膜方法將有助於大面積化沉積鈣鈦礦層。第二項工作中，我們設計實驗並證明以氧化鎳取代poly (3,4-ethylenedioxythiophene) poly (styrenesulfonate) (PEDOT:PSS)當作p-i-n結構平板式鈣鈦礦太陽電池的電洞傳輸層，可同時促進載子解離與抑制載子再復合行為。經由不同施加偏壓下磁光電流、電場相依性光致發光以及光誘導電容-電壓特性的量測，我們證明內建場大小與減少鈣鈦礦/氧化鎳界面層的界面缺陷與增強界面極化之間有協同效應。此研究了解氧化鎳電洞傳輸層對載子解離、再復合和收集的影響，提供了界面合理設計的方針，期待能進一步推進鈣鈦礦太陽電池性能的提升。

This thesis focus on organometal halide perovskite solar cells, we investigated the preparation of perovskite active layer and the Influence of electrode interlayer on device performance, respectively. In the first part: we utilized the electrospray technique to deposit the solidified crystal precursors on the substrate and investigate the transition processes in forming the orthorhombic methylammonium lead iodide film for fabricating perovskite planar heterojunction solar cells. The formation of solidified crystal precursors by the electrospray technique improves the de-wetting of the perovskite film on the substrate. Judicious selection of the applied voltage in the electrospray process generates crystal precursors with appropriate dimensions. These as-electrosprayed crystals are the solid-state reactants for the halogen exchanging and form a uniformly covered film on substrate under suitable annealing conditions. The hybrid device prepared by the electrospray technique exhibits a power conversion efficiency of 9.3 %, a short-circuit current of 19.71 mA/cm2, an open-circuit voltage of 0.87 V, and a fill factor of 0.55. The electrospray technique with the solid-state reaction mechanism proposed in this manuscript would be ideal for large-area coating of a perovskite active layer, and thus has potential for using in real mass production. In the second part: we demonstrate that the NiOX HTL can simultaneously facilitate the bulk charge dissociation and suppress nonradiative/radiative recombination processes in the inverted perovskite solar cells By combining magneto-photocurrent measurements under external bias, time-resolved and field-dependent PL measurements, and photoinduced capacitance-voltage characterizations, we demonstrate that these synergistic effects can be attributed to the enhanced built-in field that essentially results from both the reduced interfacial traps and increased interfacial polarization at CH3NH3PbI3/NiOX interface as compared to CH3NH3PbI3/PEDOT:PSS interface. Clearly, revealing the effects of NiOX HTL on the bulk charge dissociation, recombination, and collection provides guidance on the rational design of interface engineering towards further advancement of photovoltaic actions in organo-metal halide perovskites.

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