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Sulfide Boosting Near-Unity Photoluminescence Quantum Yield of Silver Nanocluster
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-09-28 , DOI: 10.1021/jacs.2c06093 Shan-Shan Zhang 1 , Shana Havenridge 2 , Chengkai Zhang 1 , Zhi Wang 1 , Lei Feng 1 , Zhi-Yong Gao 3 , Christine M Aikens 2 , Chen-Ho Tung 1 , Di Sun 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2022-09-28 , DOI: 10.1021/jacs.2c06093 Shan-Shan Zhang 1 , Shana Havenridge 2 , Chengkai Zhang 1 , Zhi Wang 1 , Lei Feng 1 , Zhi-Yong Gao 3 , Christine M Aikens 2 , Chen-Ho Tung 1 , Di Sun 1
Affiliation
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Silver nanoclusters have emerged as promising candidates for optoelectronic applications, but their room-temperature photoluminescence quantum yield (PLQY) is far from ideal to access cutting-edge device performance. Herein, two supertetrahedral silver nanoclusters with high PLQY in non-degassed solution at room temperature were constructed by interiorly supporting the core with multiple VO43– and E2– anions as structure-directing agents and exteriorly protecting the core with a rigid ligand shell of PhC≡C– and Ph2PE2– (E = S, Ag64-S; E = Se, Ag64-Se). Both clusters have similar outer Ag58 tetrahedral cages and [Ag6E4@(VO4)4] cores, forming a pair of comparable clusters to decrypt the origin of such a high PLQY, particularly in Ag64-S, where the PLQY reached up to 97%. The stronger suppression effect of inner sulfides for nonradiative decay is critical to boost the PLQY to near unity. Transient absorption spectroscopy is employed to confirm the phosphorescence nature. The quadruple-capping assembly mechanism involving Ag7 secondary building units on a Ag36 truncated tetrahedron was also established by collision-induced dissociation studies. This work not only provides a strategy of core engineering for the controlled syntheses of silver nanoclusters with high PLQY but also deciphers the origin of a near-unity PLQY, which lays a foundation for fabricating highly phosphorescent silver nanoclusters in the future.
中文翻译：
硫化物促进银纳米团簇的近单位光致发光量子产率
银纳米团簇已成为光电应用的有希望的候选者，但它们的室温光致发光量子产率 (PLQY) 远非理想，无法获得尖端的器件性能。在此，通过在内部用多个VO 4 3-和E 2-阴离子作为结构导向剂支撑核心并在外部用刚性配体壳保护核心构建了两个在室温下在非脱气溶液中具有高PLQY的超四面体银纳米团簇。PhC≡C –和 Ph 2 PE 2 – (E = S, Ag64-S ; E = Se, Ag64-Se )。两个星团具有相似的外部 Ag 58四面体笼和 [Ag 6 E 4 @(VO 4 ) 4 ] 核，形成一对可比较的簇来解密如此高 PLQY 的起源，特别是在Ag64-S中，PLQY 达到了 97%。内部硫化物对非辐射衰变的更强抑制作用对于将 PLQY 提高到接近统一至关重要。瞬态吸收光谱用于确认磷光性质。涉及 Ag 36上的 Ag 7二级构建单元的四重封盖组装机制截断四面体也通过碰撞诱导解离研究建立。该工作不仅为高PLQY银纳米团簇的可控合成提供了核心工程策略，还揭示了近统一PLQY的起源，为未来制备高磷光银纳米团簇奠定了基础。
更新日期：2022-09-28
中文翻译：
硫化物促进银纳米团簇的近单位光致发光量子产率
银纳米团簇已成为光电应用的有希望的候选者，但它们的室温光致发光量子产率 (PLQY) 远非理想，无法获得尖端的器件性能。在此，通过在内部用多个VO 4 3-和E 2-阴离子作为结构导向剂支撑核心并在外部用刚性配体壳保护核心构建了两个在室温下在非脱气溶液中具有高PLQY的超四面体银纳米团簇。PhC≡C –和 Ph 2 PE 2 – (E = S, Ag64-S ; E = Se, Ag64-Se )。两个星团具有相似的外部 Ag 58四面体笼和 [Ag 6 E 4 @(VO 4 ) 4 ] 核，形成一对可比较的簇来解密如此高 PLQY 的起源，特别是在Ag64-S中，PLQY 达到了 97%。内部硫化物对非辐射衰变的更强抑制作用对于将 PLQY 提高到接近统一至关重要。瞬态吸收光谱用于确认磷光性质。涉及 Ag 36上的 Ag 7二级构建单元的四重封盖组装机制截断四面体也通过碰撞诱导解离研究建立。该工作不仅为高PLQY银纳米团簇的可控合成提供了核心工程策略，还揭示了近统一PLQY的起源，为未来制备高磷光银纳米团簇奠定了基础。
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