有機-無機混成鈣鈦礦太陽能電池 (PSCs) 的光電轉換效率雖然已突破 25%，但環境水氣、光誘導相分離以及快速的離子遷移會導致元件嚴重衰退，這也是目前阻礙其商業化的主要瓶頸。本研究著重於混合陽離子與混合鹵素的 FA0.78Cs0.22Pb(I0.85Br0.15)3 寬能隙系統，此系統具有較好的熱穩定性，且其光吸收光譜非常適合用於串聯電池。為了抑制晶格扭曲與有害的離子遷移路徑引發的嚴重非輻射復合，本研究在鈣鈦礦中系統性地添加了四氟硼酸甲基銨 (MABF4) 與六氟磷酸甲基銨 (MAPF6)。 結果顯示，這種氟化擬鹵素添加劑 (特別是 PF6 陰離子) 能有效抑制離子遷移，不僅消除了電流-電壓 (I-V) 遲滯現象，還能在不影響短路電流密度的情況下提升元件的穩定性。過去文獻雖然常利用 MACl 來最佳化基礎晶體架構，但這類薄膜在高濕度環境下依舊脆弱。本研究發現，策略性引入大體積的氟化陰離子，能在環境大氣中產生極佳的「相鎖定」效應。對照組薄膜在濕氣下會迅速降解為無光活性的黃色 δ 相，而經氟化陰離子處理的薄膜則能抑制這種相轉變，在長期暴露於環境中的情況下，仍能保持完整、連續的晶體網路與高品質的薄膜形貌。
為了釐清背後的化學機制，我們透過一系列分析測試來追蹤這些離子的行為。研究發現，大體積的氟化添加劑會直接改變結晶動力學，藉由調整液相中的中間相或控制尺寸，讓晶體傾向均勻的二次晶粒生長，而非隨機成核。這些大體積物種會聚集在晶界或薄膜表面，透過奧斯特瓦爾德熟化 (Ostwald ripening) 減緩結晶速度；或者進入 體相 (Bulk) 晶格內鈍化未配位的 Pb2+ 缺陷；部分則會累積在底部埋入式界面。最關鍵的是，暗漏電流分析證實，大體積陰離子所形成的強多位點氟化氫鍵網路與強偶極矩，能有效固定可移動的離子、阻斷漏電路徑並提高分流電阻。本研究全面解析了氟化陰離子在化學鈍化與抑制離子遷移上的機制，為開發適合實際操作環境、兼具高穩定性與高效率的寬能隙太陽能電池，提供了一個非常實用的發展方向。

Organic-inorganic hybrid perovskite solar cells (PSCs) have achieved power conversion efficiencies exceeding 25%, yet severe performance degradation driven by ambient moisture, light-induced phase segregation, and rapid ion migration remains the primary obstacle blocking commercialization. This study focuses on the mixed-cation mixed-halide FA0.78Cs0.22Pb(I0.85Br0.15)3 wide-bandgap system, which offers enhanced thermal stability and a suitable light-absorption spectrum for tandem applications. To suppress lattice distortion and detrimental ion migration pathways that trigger severe non-radiative recombination, methylammonium tetrafluoroborate (MABF4) and methylammonium hexafluorophosphate (MAPF6) were systematically incorporated into perovskite. In this work, we demonstrate that fluorinated pseudo-halogen additives, especially PF6-, successfully suppress ion migration, thereby eliminating current-voltage hysteresis and enhancing operational stability without imparting any negative impacts on the short-circuit current density.
While previous literature has extensively investigated baseline crystalline frameworks pre-optimized with MACl, such films still exhibit vulnerability when exposed to high-humidity ambient environments. Herein, we discover that the strategic introduction of bulky fluorinated anions provides an exceptional phase-locking effect in the ambient atmosphere. While the control film suffers from rapid degradation into the non-photoactive yellow δ-phase, the fluorinated anion treatments reduce this moisture-triggered phase transition, effectively retaining the pristine, continuous crystalline network and high-quality film morphology over prolonged environmental exposure.
To elucidate the underlying chemical mechanisms, a series of characterizations were deployed to trace the behaviors of the foreign functional ions. The bulky fluorinated additives actively modulate crystallization kinetics, altering the intermediate phases or controlling colloidal cluster sizes in the liquid phase to favor uniform secondary grain growth over random nucleation. These bulky species are considered to segregate at grain boundaries or the film surfaces to slow down crystallization via Ostwald ripening, penetrate the bulk lattice to passivate uncoordinated Pb2+ defect sites, or accumulate at the buried bottom interface. Crucially, dark leakage current analysis reveals that the strong multi-site fluorinated hydrogen bonding networks and strong dipoles of the bulky anions effectively immobilize mobile ions, block leakage current pathways, and increase shunt resistance. This comprehensive understanding of chemical passivation and suppressed ion migration via fluorinated anions delivers a highly viable paradigm for engineering highly stable and efficient wide-bandgap photovoltaics tailored for realistic operational environments.

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