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Impact of Mesoporous Silicon Template Pore Dimension and Surface Chemistry on Methylammonium Lead Trihalide Perovskite Photophysics
Advanced Materials Interfaces ( IF 4.3 ) Pub Date : 2020-09-13 , DOI: 10.1002/admi.202001138 Viviana C.P. da Costa 1 , Roberto Gonzalez‐Rodriguez 1 , Kyle Frohna 2 , Géraud Delport 2 , Samuel D. Stranks 2, 3 , Leigh T. Canham 4 , Jeffery L. Coffer 1
Advanced Materials Interfaces ( IF 4.3 ) Pub Date : 2020-09-13 , DOI: 10.1002/admi.202001138 Viviana C.P. da Costa 1 , Roberto Gonzalez‐Rodriguez 1 , Kyle Frohna 2 , Géraud Delport 2 , Samuel D. Stranks 2, 3 , Leigh T. Canham 4 , Jeffery L. Coffer 1
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In influencing fundamental properties—and ultimately device performance—of lead halide perovskites, interfacial interactions play a major role, notably with regard to carrier diffusion and recombination. Here anodized porous Si (pSi) as well as porous silica particles are employed as templates for formation of methylammonium lead trihalide nanostructures. This allows synthesis of relatively small perovskite domains and comparison of associated interfacial chemistry between as‐prepared hydrophobic hydrideterminated functionalities and hydrophilic oxide‐terminated surfaces. While physical confinement of MAPbBr3 has a uniform effect on carrier lifetime, pore size (7–18 nm) of the silicon‐containing template has a sensitive influence on perovskite photoluminescence (PL) wavelength maximum. Furthermore, identity of the surface functionality of the template significantly alters the PL quantum efficiency, with lowest PL intensity associated with the H‐terminated pSi and the most intense PL affiliated with the oxideterminated pSi surface. These effects are explored for green‐emitting MAPbBr3 as well as infrared‐emitting MAPbI3. In addition, the role of silicon surface chemistry on the time‐dependent stability of these perovskites packaged within a given mesoporous template is also evaluated, specifically, a lack of miscibility between MAPbI3 and the H‐terminated pSi template results in a diffusion of this specific perovskite composition eluting from this porous matrix over time.
中文翻译：
介孔硅模板孔尺寸和表面化学性质对甲基铵三卤化铅钙钛矿光物理的影响
在影响卤化钙钛矿的基本性能以及最终的器件性能时，界面相互作用起着主要作用，特别是在载流子扩散和复合方面。在这里，采用阳极氧化的多孔硅（pSi）以及多孔的二氧化硅颗粒作为模板，用于形成甲基铵铅三卤化物纳米结构。这样可以合成相对较小的钙钛矿结构域，并可以比较制备的疏水性氢化末端官能团和亲水性氧化物末端表面的相关界面化学。物理限制MAPbBr 3对载流子寿命有均匀的影响，含硅模板的孔径（7-18 nm）对钙钛矿光致发光（PL）最大波长有敏感影响。此外，模板表面功能的一致性显着改变了PL量子效率，与H端接的pSi相关的PL强度最低，而与氧化端接的pSi表面相关的PL强度最高。探索了绿色发射的MAPbBr 3和红外发射的MAPbI 3的这些效应。此外，还评估了硅表面化学对包装在给定介孔模板中的这些钙钛矿的时间依赖性稳定性的作用，特别是，MAPbI 3之间缺乏互溶性 H端接的pSi模板会导致这种特定的钙钛矿成分随时间从该多孔基质中洗脱出来。
更新日期：2020-11-06
中文翻译：
介孔硅模板孔尺寸和表面化学性质对甲基铵三卤化铅钙钛矿光物理的影响
在影响卤化钙钛矿的基本性能以及最终的器件性能时，界面相互作用起着主要作用，特别是在载流子扩散和复合方面。在这里，采用阳极氧化的多孔硅（pSi）以及多孔的二氧化硅颗粒作为模板，用于形成甲基铵铅三卤化物纳米结构。这样可以合成相对较小的钙钛矿结构域，并可以比较制备的疏水性氢化末端官能团和亲水性氧化物末端表面的相关界面化学。物理限制MAPbBr 3对载流子寿命有均匀的影响，含硅模板的孔径（7-18 nm）对钙钛矿光致发光（PL）最大波长有敏感影响。此外，模板表面功能的一致性显着改变了PL量子效率，与H端接的pSi相关的PL强度最低，而与氧化端接的pSi表面相关的PL强度最高。探索了绿色发射的MAPbBr 3和红外发射的MAPbI 3的这些效应。此外，还评估了硅表面化学对包装在给定介孔模板中的这些钙钛矿的时间依赖性稳定性的作用，特别是，MAPbI 3之间缺乏互溶性 H端接的pSi模板会导致这种特定的钙钛矿成分随时间从该多孔基质中洗脱出来。
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