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Colloidal Synthesis of Shape-Controlled Cs2NaBiX6 (X = Cl, Br) Double Perovskite Nanocrystals: Discrete Optical Transition by Non-Bonding Characters and Energy Transfer to Mn Dopants
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-06-10 , DOI: 10.1021/acs.chemmater.0c01315 Wonseok Lee 1 , Doowon Choi 2 , Sungjee Kim 1, 2
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-06-10 , DOI: 10.1021/acs.chemmater.0c01315 Wonseok Lee 1 , Doowon Choi 2 , Sungjee Kim 1, 2
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As an alternative to lead halide perovskites, various types of lead-free perovskites have been recently studied for optoelectronic materials. This paper reports the synthesis of highly phase-pure Cs2NaBiX6 (X = Cl, Br) double perovskite (DP) nanocrystals (NCs). They show characteristic absorption features of sharp and discrete peaks mostly originating from the Bi3+ s–p transition (6s2 → 6s1p1) in [BiX6]3– units within the crystal lattice of the elpasolite structure. Such unique optical properties are attributed to the non-bonding character of electropositive sodium and electronically isolated [BiX6]3– units in crystals. The shape of Cs2NaBiX6 NCs could be quantitatively controlled by adjusting the reaction temperature. Reaction temperatures above 180 °C favor development of a cuboctahedral (CO) shape, whereas development of a cuboidal (CB) shape is favored below 170 °C. CB NCs can be subsequently converted to CO NCs by heating to 200 °C. The CO NCs promote the growth of heterostructure adducts on the (111) facets; these adducts could be posteliminated by etching. Mn-doped Cs2NaBiCl6 NCs are synthesized; they show efficient energy transfer from the NC host to the dopants. The synthesis and shape control of Cs2NaBiX6 NCs and Mn-doped Cs2NaBiCl6 NCs could expand a new class of lead-free DP NCs applicable to optoelectronic applications.
中文翻译：
形状控制的Cs 2 NaBiX 6（X = Cl，Br）双钙钛矿纳米晶体的胶体合成：通过非键合特征的离散光学跃迁和能量转移至Mn掺杂剂
作为卤化钙钛矿的替代品，最近已经研究了用于光电材料的各种类型的无铅钙钛矿。本文报道了高相纯Cs 2 NaBiX 6（X = Cl，Br）双钙钛矿（DP）纳米晶体（NCs）的合成。它们在锐钛矿结构晶格内的[BiX 6 ] 3–单元中表现出尖峰和离散峰的特征吸收特征，这些峰主要来自Bi 3+ s–p跃迁（6s 2 →6s 1 p 1）。这种独特的光学性质归因于电正性钠和电子隔离的[BiX 6 ]的非键合特性3 –晶体单位。通过调节反应温度可以定量控制Cs 2 NaBiX 6 NC的形状。高于180°C的反应温度有利于形成立方八面体（CO）形状，而低于170°C则有利于形成立方（CB）形状。随后可以通过加热到200°C将CB NC转换为CO NC。CO NCs促进（111）面上的异质结构加合物的生长；这些加合物可以通过蚀刻后消除。合成了Mn掺杂的Cs 2 NaBiCl 6 NCs；它们显示了从NC主体到掺杂剂的有效能量转移。Cs 2 NaBiX 6 NCs和Mn掺杂的Cs 2的合成与形状控制NaBiCl 6 NC可以扩展适用于光电应用的新型无铅DP NC。
更新日期：2020-06-10
中文翻译：
形状控制的Cs 2 NaBiX 6（X = Cl，Br）双钙钛矿纳米晶体的胶体合成：通过非键合特征的离散光学跃迁和能量转移至Mn掺杂剂
作为卤化钙钛矿的替代品，最近已经研究了用于光电材料的各种类型的无铅钙钛矿。本文报道了高相纯Cs 2 NaBiX 6（X = Cl，Br）双钙钛矿（DP）纳米晶体（NCs）的合成。它们在锐钛矿结构晶格内的[BiX 6 ] 3–单元中表现出尖峰和离散峰的特征吸收特征，这些峰主要来自Bi 3+ s–p跃迁（6s 2 →6s 1 p 1）。这种独特的光学性质归因于电正性钠和电子隔离的[BiX 6 ]的非键合特性3 –晶体单位。通过调节反应温度可以定量控制Cs 2 NaBiX 6 NC的形状。高于180°C的反应温度有利于形成立方八面体（CO）形状，而低于170°C则有利于形成立方（CB）形状。随后可以通过加热到200°C将CB NC转换为CO NC。CO NCs促进（111）面上的异质结构加合物的生长；这些加合物可以通过蚀刻后消除。合成了Mn掺杂的Cs 2 NaBiCl 6 NCs；它们显示了从NC主体到掺杂剂的有效能量转移。Cs 2 NaBiX 6 NCs和Mn掺杂的Cs 2的合成与形状控制NaBiCl 6 NC可以扩展适用于光电应用的新型无铅DP NC。
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