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Room-Temperature Solid-State Synthesis of Cs3Cu2I5 Thin Films and Formation Mechanism for Its Unique Local Structure
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-05-16 , DOI: 10.1021/jacs.3c01713 Masatake Tsuji 1 , Masato Sasase 1 , Soshi Iimura 1, 2, 3 , Junghwan Kim 1, 3, 4 , Hideo Hosono 1, 2
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-05-16 , DOI: 10.1021/jacs.3c01713 Masatake Tsuji 1 , Masato Sasase 1 , Soshi Iimura 1, 2, 3 , Junghwan Kim 1, 3, 4 , Hideo Hosono 1, 2
Affiliation
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Blue-emitting Cs3Cu2I5 has attracted attention owing to its near-unity PL quantum yield and applications in DUV photodetectors and scintillators. Its PL properties originate from the unique local structure around the luminescent center, the [Cu2I5]3– polyhedron iodocuprate anion consisting of the edge-shared CuI3 triangle and the CuI4 tetrahedron dimer, which is isolated by Cs+ ions. We found that solid-state reactions between CsI and CuI occur near room temperature (RT) to form Cs3Cu2I5 and/or CsCu2I3 phases. High-quality thin films of these phases were obtained by the sequential deposition of CuI and CsI by thermal evaporation. We elucidated that the formation of interstitial Cu+ and the antisite of I– at the Cs+ site in the CsI crystal through Cu+ and I– diffusion results in the RT synthesis of Cs3Cu2I5. The unique structure formation of the luminescent center was revealed using a model based on the low packing density of the CsCl-type crystal structure, similar sizes of Cs+ and I– ions, and the high diffusivity of Cu+. The self-aligned patterning of the luminous regions on thin films was demonstrated.
中文翻译：
Cs3Cu2I5 薄膜的室温固态合成及其独特局域结构的形成机制
蓝光Cs 3 Cu 2 I 5由于其近乎单位的PL量子产率以及在DUV光电探测器和闪烁体中的应用而受到关注。其 PL 特性源于发光中心周围独特的局部结构，即 [Cu 2 I 5 ] 3–多面体碘铜酸盐阴离子，由共享边缘的 CuI 3三角形和 CuI 4四面体二聚体组成，被 Cs +离子隔离。我们发现 CsI 和 CuI 之间的固态反应发生在室温 (RT) 附近，形成 Cs 3 Cu 2 I 5和/或 CsCu 2 I3个阶段。这些相的高质量薄膜是通过热蒸发连续沉积 CuI 和 CsI 获得的。我们阐明了通过 Cu +和 I –扩散在 CsI 晶体中的Cs +位点形成间隙Cu +和 I –反位，导致 Cs 3 Cu 2 I 5的逆转录合成。使用基于 CsCl 型晶体结构的低堆积密度、Cs +和 I -离子的相似尺寸以及 Cu +的高扩散率的模型揭示了发光中心的独特结构形成. 展示了薄膜上发光区域的自对准图案。
更新日期：2023-05-16
中文翻译：
Cs3Cu2I5 薄膜的室温固态合成及其独特局域结构的形成机制
蓝光Cs 3 Cu 2 I 5由于其近乎单位的PL量子产率以及在DUV光电探测器和闪烁体中的应用而受到关注。其 PL 特性源于发光中心周围独特的局部结构，即 [Cu 2 I 5 ] 3–多面体碘铜酸盐阴离子，由共享边缘的 CuI 3三角形和 CuI 4四面体二聚体组成，被 Cs +离子隔离。我们发现 CsI 和 CuI 之间的固态反应发生在室温 (RT) 附近，形成 Cs 3 Cu 2 I 5和/或 CsCu 2 I3个阶段。这些相的高质量薄膜是通过热蒸发连续沉积 CuI 和 CsI 获得的。我们阐明了通过 Cu +和 I –扩散在 CsI 晶体中的Cs +位点形成间隙Cu +和 I –反位，导致 Cs 3 Cu 2 I 5的逆转录合成。使用基于 CsCl 型晶体结构的低堆积密度、Cs +和 I -离子的相似尺寸以及 Cu +的高扩散率的模型揭示了发光中心的独特结构形成. 展示了薄膜上发光区域的自对准图案。
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