Hybridising inorganic materials with fluorescent BOPHY dyes: A structural and optical comparative study.
Hybridising inorganic materials with fluorescent BOPHY dyes: A structural and optical comparative study.
复制标题
DOI：
10.3389/fchem.2022.921112
复制
发表时间：
2022
影响因子：
5.5
通讯作者：
中科院分区：
文献类型：
--
作者：
这项研究提出了新的单色光捕获系统的设计和表征的基础上，无机多孔材料与有机染料分子在其结构内杂交。制备了一种新的荧光BOPHY染料，其光学特征在于，并用作两种烷氧基硅烷衍生物的参考和合成前体，所述烷氧基硅烷衍生物分别并入二氧化硅结构内。的染料，一个轴承一个烷氧基硅烷基团和其他两个，共缩合与原硅酸四乙酯，形成一个混合的有机硅框架，其中它们被发现在特定的位置。通过粉末XRD和TEM分析了新材料的结构，证实了介孔MCM-41二氧化硅颗粒典型的六方孔排列的存在。稳态和时间分辨分析表明，染料最分散在框架内的颗粒保留最高的荧光量子产率，高达0.63，在可见光谱的绿黄色区域。另一方面，增加固体基质中BOPHY单元的含量似乎有利于非辐射失活途径和聚集现象，这降低了发光效率。这些材料还表现出有趣的性质，如双激发态衰减和荧光各向异性。短的荧光寿命，约2 ns，匹配典型的单重态寿命的BOPHY染料，而长的组件，高达20 ns，归因于延迟荧光，这可能会发生通过电荷复合。光学各向异性实验表明，所有的材料显示偏振光发射到一个显着的程度，对于大多数样品，它也可以确定一个偏振转移衰减轨迹，从400到800 ps这是归因于相邻的染料单元之间的二氧化硅结构内的能量迁移的发生。
This study presents the design and characterization of new monochromatic light-harvesting systems based on inorganic porous materials hybridized with organic dye molecules within their structure. A new fluorescent BOPHY dye was prepared, characterized optically and used as both reference and synthetic precursor for two alkoxysilane derivatives that were incorporated separately within a silica structure. The dyes, one bearing one alkoxysilane group and the other one two, were co-condensed with tetraethyl orthosilicate to form a hybrid organo-silica framework, where they are found at specific locations. The structure of the new materials was analysed by powder XRD and TEM, which confirmed the presence of the hexagonal pore arrangement typical of mesoporous MCM-41 silica particles. The steady-state and time-resolved analysis showed that the particles where the dyes are most dispersed within the framework retain the highest fluorescence quantum yield, up to 0.63, in the green-yellow region of the visible spectrum. On the other hand, increasing the content of BOPHY units in the solid matrix seem to favour non-radiative deactivation pathways and aggregation phenomena, which lower the efficiency of light emission. The materials also exhibit interesting properties, such as a dual excited-state decay and fluorescence anisotropy. The short fluorescence lifetime, about 2 ns, matches the typical singlet lifetime of BOPHY dyes, whereas the long component, up to 20 ns, is attributed to delayed fluorescence, which could take place via charge recombination. Optical anisotropy experiments revealed that all materials show polarised light emission to a significant extent and, for most samples, it was also possible to determine a polarisation transfer decay trace, from 400 to 800 ps This is ascribed to the occurrence of energy migration between neighbouring dye units within the silica structure.
登录
查看更多内容
影响因子：
8.6
作者：
Melde, BJ;Holland, BT;Stein, A
通讯作者：
Stein, A
影响因子：
4.4
作者：
BERBERANSANTOS, MN;PEREIRA, EJN;MARTINHO, JMG
通讯作者：
MARTINHO, JMG
影响因子：
4.4
作者：
BOULU, LG;PATTERSON, LK;KOZAK, JJ
通讯作者：
KOZAK, JJ
影响因子：
17.1
作者：
Calver, Christina F.;Schanze, Kirk S.;Cosa, Gonzalo
通讯作者：
Cosa, Gonzalo
影响因子：
--
作者：
Jeong, Eun-Young;Burri, Abhishek;Park, Sang-Eon
通讯作者：
Park, Sang-Eon