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Modulation of Broadband Emissions in Two-Dimensional ⟨100⟩-Oriented Ruddlesden–Popper Hybrid Perovskites
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-05-28 , DOI: 10.1021/acsenergylett.0c01047 Jun Yin 1 , Rounak Naphade 1 , Luis Gutiérrez Arzaluz 1 , Jean-Luc Brédas 2 , Osman M. Bakr 1 , Omar F. Mohammed 1
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-05-28 , DOI: 10.1021/acsenergylett.0c01047 Jun Yin 1 , Rounak Naphade 1 , Luis Gutiérrez Arzaluz 1 , Jean-Luc Brédas 2 , Osman M. Bakr 1 , Omar F. Mohammed 1
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Two-dimensional (2D) Ruddlesden–Popper (RP) perovskites are emerging materials for light-emitting applications. Unfortunately, their desirable narrowband emission coexists with broadband emissions, which limits the color quality and performance of the light source. However, the origin of such broadband emission in ⟨100⟩-oriented perovskites is still under debate. Here, we experimentally and theoretically demonstrate that unlike ⟨110⟩-oriented RP perovskites, the broadband emission of the 2D ⟨100⟩-oriented RP (PEA)2PbI4 (PEA = C6H5C2H4NH3+) perovskites originates from defect-related luminescence centers. We find that the broadband emission of this prototype 2D structure can be largely suppressed by using excess PEAI treatment. Density functional theory (DFT) calculations indicate that iodine (I) vacancies both in the bulk and on the surface are responsible for the broadband emission. We attribute the decreased broadband emission after PEAI treatment to the passivation of both undercoordinated Pb2+ ions on the surface and I vacancies in the bulk through I– ion migration.
中文翻译：
二维⟨100⟩取向的Ruddlesden-Pop混合钙钛矿中宽带发射的调制
二维（2D）Ruddlesden-Popper（RP）钙钛矿是新兴的发光应用材料。不幸的是，它们理想的窄带发射与宽带发射并存，这限制了光源的颜色质量和性能。然而，这种以emission100⟩为取向的钙钛矿中宽带发射的起源仍在争论中。在这里，我们通过实验和理论证明，与⟨110⟩定向RP钙钛矿不同，二维D100⟩定向RP（PEA）2 PbI 4的宽带发射（PEA = C 6 H 5 C 2 H 4 NH 3 +钙钛矿起源于与缺陷相关的发光中心。我们发现，通过使用过量的PEAI处理，可以大大抑制此原型2D结构的宽带发射。密度泛函理论（DFT）计算表明，大量和表面上的碘（I）空位均是宽带发射的原因。我们认为宽带发射Peai相互治疗后两者undercoordinated Pb组成的钝化降低2+的表面上的离子和我的空缺在本体通过I -离子迁移。
更新日期：2020-07-10
中文翻译：
二维⟨100⟩取向的Ruddlesden-Pop混合钙钛矿中宽带发射的调制
二维（2D）Ruddlesden-Popper（RP）钙钛矿是新兴的发光应用材料。不幸的是，它们理想的窄带发射与宽带发射并存，这限制了光源的颜色质量和性能。然而，这种以emission100⟩为取向的钙钛矿中宽带发射的起源仍在争论中。在这里，我们通过实验和理论证明，与⟨110⟩定向RP钙钛矿不同，二维D100⟩定向RP（PEA）2 PbI 4的宽带发射（PEA = C 6 H 5 C 2 H 4 NH 3 +钙钛矿起源于与缺陷相关的发光中心。我们发现，通过使用过量的PEAI处理，可以大大抑制此原型2D结构的宽带发射。密度泛函理论（DFT）计算表明，大量和表面上的碘（I）空位均是宽带发射的原因。我们认为宽带发射Peai相互治疗后两者undercoordinated Pb组成的钝化降低2+的表面上的离子和我的空缺在本体通过I -离子迁移。
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