近年來，有機鈣鈦礦太陽電池（PSC）的光電轉換效率（PCE）屢創新高，2025 年已達 27.0%，已相當接近矽晶太陽電池的 27.6%。這一成果顯示 PSC 不僅具備挑戰矽晶技術的潛力，更有望成為新一代具商業化前景的有機半導體太陽電池。然而，PSC 在大面積化發展過程中仍面臨多重瓶頸，尤其是對濕熱、水氧高度敏感，導致其在大氣環境下穩定性欠佳。隨著元件尺寸的增加，效率衰退與介面缺陷問題更趨嚴重。此外，應用端整合不足亦限制了鈣鈦礦技術的市場推進。如何在兼顧高效率的同時，實現長期穩定性與可規模化製作，已成為 PSC 商業化發展的核心課題。為此，本研究提出三大策略：結構工程、介面工程與應用整合，以全面應對各項關鍵技術挑戰，推動有機鈣鈦礦太陽模組從實驗室走向產業化應用。
於論文第4章，針對鈣鈦礦吸收層結構進行改良並引入無毒溶劑γ-丁內酯 (gamma-Butyrolactone，GBL) 至製程中。提出了雙層鈣鈦礦結構用於太陽電池中，開發出類似2D/3D異質結構的雙層鈣鈦礦吸收層。將單陽離子（Single cation）與多陽離子（Multiple cation）鈣鈦礦薄膜進行堆疊，證實以上層單陽離子薄膜可提升元件效率，並強化其在高溫條件下的穩定性。此外，本研究採用刮刀塗佈法（Doctor blade coating）實現大面積薄膜沉積，結合無毒溶劑與可規模化塗佈方式，有助於鈣鈦礦模組的發展。於第 5 章（5-1 與 5-2），聚焦於界面品質提升，採用麥角硫因（L-EGT）與組氨酸（L-His）自組裝分子層作為界面鈍化層。分子羧基與 TiO₂ 表面形成強鍵結，胺基則與鈣鈦礦層鉛離子與有機陽離子作用，降低界面缺陷與非輻射複合。此策略有效提升 25 cm² 大面積模組效率至 17.84%（L-EGT）與 16.5%（L-His），並於 720 小時老化測試後維持初始效率的 91%，展現長期穩定性與商業化潛力。在第 5-3 節的研究中，本研究針對電子傳輸層(Electron Transport Layer, ETL)與鈣鈦礦吸收層的界面進行結構改良，探討不同形式之電子傳輸層對於大面積模組的適配性。界面工程對於大面積元件的載流子提取與傳輸效率具有關鍵影響，同時引入紫外光皮秒雷射切割技術，提升模組元件串聯品質，降低模組內部串聯電阻與短路路徑(Shunting)，並有效減少死區(dead area)寬度，該技術不僅能提升鈣鈦礦太陽模組的商業化可行性，也能加速其市場應用，具有極高的產業價值與應用潛力。進入第 6 章的跨域應用探索，本研究將 PSC 與天線整合，開發出 PMMA 封裝的鈣鈦礦綠能天線（PVKSA）與共面波導（CPW）透明天線。PMMA 兼具優異絕緣性與阻隔水氧的封裝特性，同時作為天線介電層，可透過厚度與溶劑系統調控介電常數，優化天線性能。搭配 Pt 奈米層與 CPW 結構，顯著提升天線增益與輻射效率，開發出雙功能集成式綠能天線。最後在第 6-3 節，針對四端點（4T）鈣鈦礦/矽堆疊太陽電池模組應用，提出半穿透模組的圖形化電極策略。透過調控透明導電氧化物（TCO）濺鍍時的氧氣流量，達到電性與透光率的平衡，使模組效率達 13.8%。進一步採用 P2.5 金屬圖形化鍍金設計，降低接觸電阻與金屬遮蔽率，並提高底層矽電池的透光量，最終將模組效率提升至 15.9%，並將 4T 堆疊效率推高至 26.1%，展現堆疊型太陽電池模組推向商業應用的潛能。

In recent years, the power conversion efficiency (PCE) of organic perovskite solar cells (PSCs) has continued to set new records, reaching 27.0% in 2025—approaching the 27.6% benchmark of crystalline silicon solar cells. This achievement highlights PSCs as not only having the potential to rival silicon technology but also as a promising next-generation photovoltaic technology with strong commercialization prospects. However, scaling PSCs to large-area devices remains hindered by their pronounced sensitivity to moisture, heat, and oxygen, which results in poor stability under ambient conditions. As the device size increases, efficiency degradation and interfacial defects become increasingly severe. In addition, insufficient integration into application-oriented systems has further slowed their market adoption. Achieving high efficiency, long-term stability, and scalable manufacturing simultaneously has thus emerged as a core challenge for organic perovskite solar module commercialization. To address these issues, this study proposes three overarching strategies—structural engineering, interfacial engineering, and application integration—targeting the key technological bottlenecks in large-area PSC development.
Chapter 4 focuses on structural optimization of the perovskite absorber layer, incorporating the non-toxic solvent γ-butyrolactone (GBL) into the fabrication process. A bilayer perovskite structure was developed, analogous to a 2D/3D hybrid heterostructure, by stacking a single-cation perovskite top layer over a multi-cation base layer. This architecture was shown to improve device efficiency and enhance thermal stability. Moreover, the doctor blade coating method was employed for scalable large-area film deposition, which, when combined with GBL, provides a viable route toward practical PSC module fabrication. Chapters 5-1 and 5-2 address interfacial quality improvement via self-assembled monolayer of L-ergothioneine (L-EGT) and L-histidine (L-His). These molecules form strong bonds with the TiO₂ surface through their carboxyl groups, while their amino groups interact with lead ions and organic cations in the perovskite lattice, thereby reducing interfacial defects and suppressing nonradiative recombination. This strategy enhanced the efficiencies of large-area (25 cm²) modules to 17.84% (L-EGT) and 16.5% (L-His), retaining 91% of the initial efficiency after 720 h of aging, demonstrating excellent long-term stability and commercial potential. In Chapter 5-3, structural improvements were implemented at the interface between the electron transport layer (ETL) and the perovskite absorber. The compatibility of different ETL configurations for large-area modules was investigated, revealing that interfacial engineering plays a critical role in carrier extraction and transport. Furthermore, ultraviolet picosecond laser scribing (P1, P2, P3) was introduced to enhance module series interconnection quality, reduce series resistance and shunting pathways, and minimize the width of inactive dead areas. This approach not only improves the commercial viability of PSC modules but also accelerates their readiness for market deployment. Chapter 6 explores cross-domain functional integration by combining PSCs with transparent antenna systems. PMMA-encapsulated perovskite solar antennas (PVKSA) and coplanar waveguide (CPW) transparent antennas were developed. PMMA serves as both an encapsulation layer—providing excellent moisture and oxygen barrier properties—and a dielectric substrate whose dielectric constant can be tuned by adjusting its thickness or solvent system. Combined with a Pt nanolayer and optimized CPW architecture, this design significantly improves antenna gain and radiation efficiency, enabling dual-function, integrated green-energy antennas. Finally, in Chapter 6-3, a patterned electrode strategy was introduced for semi-transparent modules designed for four-terminal (4T) perovskite/silicon tandem applications. By optimizing the oxygen flow during transparent conductive oxide (TCO) sputtering, a balance between conductivity and optical transmittance was achieved, resulting in a module efficiency of 13.8%. Subsequent implementation of P2.5 patterned metallization reduced contact resistance and metal shading, improving light transmission to the underlying silicon cell. This strategy increased the module efficiency to 15.9% and raised the 4T tandem efficiency to 26.1%, demonstrating strong potential for commercial deployment of perovskite/silicon tandem solar modules.

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