【學術亮點】透過離液劑調控錫鉛鹵化物鈣鈦礦晶體生長
【學術亮點】Crystal Growth Modulation of Tin–Lead Halide Perovskites via Chaotropic Agent
Facility Agriculture: Application of Solar Facilities in Agriculture【Department of Chemical Engineering / Lin, Chieh-Ting / Associate Professor】
設施農業：光能設施於農業固碳之應用【化學工程學系/林玠廷 副教授】
論文篇名 英文：Crystal Growth Modulation of Tin–Lead Halide Perovskites via Chaotropic Agent
中文：透過離液劑調控錫鉛鹵化物鈣鈦礦晶體生長
期刊名稱 Journal of the American Chemical Society
發表年份,卷數,起迄頁數 2025, 147(35), 31578–31590
作者 Dong, Yueyao; Zhu, Wen-Xian; Wu, Dong-Tai; Li, Xuan; Westbrook, Robert J. E.; Huang, Chi-Jing; Min, Zeyin; Hong, Weiying; Wang, Boyuan; Min, Ganghong; Sathasivam, Sanjayan; Palma, Matteo; Dimitrov, Stoichko; Lin, Chieh-Ting(林玠廷)*; Macdonald, Thomas J.
DOI 10.1021/jacs.5c05772
中文摘要 具有可調能隙（1.2–1.4 eV）的錫–鉛（Sn–Pb）鹵化物鈣鈦礦在高效率全鈣鈦礦串疊式太陽能電池的發展中展現出巨大潛力。然而，要實現商業可行性並保持高效率的 Sn-Pb 鈣鈦礦太陽能電池仍面臨許多挑戰。在多種優化策略中，添加劑的引入已被證明對於調控 Sn-Pb 鈣鈦礦的結晶過程至關重要。儘管添加劑被廣泛應用以改善元件性能，但其詳細的光物理機制仍不明確。本研究闡明了硫氰酸胍這種離液劑（chaotropic agent）在 Sn-Pb 鈣鈦礦結晶過程中的機制作用。我們結合高光譜成像與原位時間解析的光致發光光譜，探究 Sn-Pb 鈣鈦礦的結晶過程。結果顯示，離液劑能在鈣鈦礦結晶期間調控晶體成長速率，生成更均勻的薄膜並降低非輻射復合。我們透過觀察冷卻過程中的光致發光變化，挑戰了「結晶在溶劑揮發後即終止」的傳統假設。最終形成的薄膜具有7.28% 的光致發光量子效率與超過 11 μs 的載子壽命，使元件效率達到 22.34%、填充因子超過 80%。本研究對添加劑調控的晶體成長與冷卻動力學提供了基礎理解，推進了高品質 Sn-Pb 鈣鈦礦在高效率、穩定光電元件設計上的應用。
英文摘要 Mixed tin–lead (Sn-Pb) halide perovskites, with their tunable bandgaps (1.2–1.4 eV), show great promise for the development of highly efficient all-perovskite tandem solar cells. However, achieving commercial viability and stabilized high efficiency for Sn-Pb perovskite solar cells (PSCs) presents numerous challenges. Among various optimization strategies, the incorporation of additives has proven critical in modulating the crystallization of Sn-Pb perovskites. Despite the widespread use of additives to improve performance, detailed photophysical mechanisms remain unclear. In this work, we elucidate the mechanistic role of guanidinium thiocyanate, a chaotropic agent, in the crystallization of Sn-Pb perovskites. We combine hyperspectral imaging with real-time in situ photoluminescence spectroscopy to study the crystallization process of Sn-Pb perovskites. Our findings reveal that the chaotropic agent modulates the crystal growth rate during perovskite crystallization, resulting in more homogeneous films with reduced nonradiative recombination. We challenge the common assumption that crystallization stops once the solvent evaporates by identifying photoluminescence variations during the cooldown process. The resulting films exhibit a photoluminescence quantum yield of 7.28% and a charge carrier lifetime exceeding 11 μs, leading to a device efficiency of 22.34% and a fill factor of over 80%. This work provides a fundamental understanding of additive-mediated crystal growth and transient cooldown dynamics, advancing the design of high-quality Sn–Pb perovskites for efficient and stable optoelectronics.
發表成果與本中心研究主題相關性 本研究針對錫–鉛鈣鈦礦材料的結晶行為進行機制性探討，提出利用離液劑（chaotropic agent）調控成核與成長過程，成功提升薄膜均勻性並降低非輻射復合損失，進而實現高效率與穩定的鈣鈦礦太陽能電池。此技術有助於開發高效率、低能耗的光電元件，對於未來在農業設施（如溫室與感測網）中導入低成本、可大面積製作的鈣鈦礦光電模組具有潛在應用價值，契合本中心推動「永續農業與能源技術整合應用」的研究主軸。