A Structural Model for a Self-Assembled Nanotube Provides Insight into Its Exciton Dynamics.
A Structural Model for a Self-Assembled Nanotube Provides Insight into Its Exciton Dynamics.
复制标题
DOI：
10.1021/acs.jpcc.5b03398
复制
发表时间：
2015-06-18
影响因子：
3.7
通讯作者：
Jaroniec, Christopher P.
中科院分区：
文献类型：
--
作者：
Gao, Min;Paul, Subhradip;Schwieters, Charles D.;You, Zhi-Qiang;Shao, Hui;Herbert, John M.;Parquette, Jon R.;Jaroniec, Christopher P.
功能性自组装纳米结构的设计和合成通常是一个经验性的过程，充满了关于这些非共价体系中原子级结构的关键知识缺口。在这里，我们报告了一个半导体纳米管的结构模型，通过自组装的萘二酰亚胺-赖氨酸（NDI-Lys）的积木确定使用实验13 C-13 C和13 C-15 N的距离限制固态核磁共振补充电子显微镜和X-射线粉末衍射数据。该结构模型揭示了一个二维的晶体状结构的堆叠单层环，每个含有1050个NDI-Lys分子，与显着的π堆积相互作用发生在环的范围内和沿着管的长轴。基于含时密度泛函理论和非相干跳跃模型，模拟了纳米管的激发态离域和能量转移。值得注意的是，这些计算揭示了从激子亮态的有效能量迁移，这与先前使用荧光光谱观察到的NDI-Lys纳米管内的快速能量转移一致。
The design and synthesis of functional self-assembled nanostructures is frequently an empirical process fraught with critical knowledge gaps about atomic-level structure in these noncovalent systems. Here, we report a structural model for a semiconductor nanotube formed via the self-assembly of naphthalenediimide-lysine (NDI-Lys) building blocks determined using experimental 13C–13C and 13C–15N distance restraints from solid-state nuclear magnetic resonance supplemented by electron microscopy and X-ray powder diffraction data. The structural model reveals a two-dimensional-crystal-like architecture of stacked monolayer rings each containing ∼50 NDI-Lys molecules, with significant π-stacking interactions occurring both within the confines of the ring and along the long axis of the tube. Excited-state delocalization and energy transfer are simulated for the nanotube based on time-dependent density functional theory and an incoherent hopping model. Remarkably, these calculations reveal efficient energy migration from the excitonic bright state, which is in agreement with the rapid energy transfer within NDI-Lys nanotubes observed previously using fluorescence spectroscopy.
登录
查看更多内容
影响因子：
2.7
作者：
Helmus JJ;Jaroniec CP
通讯作者：
Jaroniec CP
影响因子：
5.6
作者：
BARLOW, DJ;THORNTON, JM
通讯作者：
THORNTON, JM
影响因子：
15
作者：
Helmus, Jonathan J.;Surewicz, Krystyna;Apostol, Marcin I.;Surewicz, Witold K.;Jaroniec, Christopher P.
通讯作者：
Jaroniec, Christopher P.
影响因子：
64.8
作者：
Loquet, Antoine;Sgourakis, Nikolaos G.;Gupta, Rashmi;Giller, Karin;Riedel, Dietmar;Goosmann, Christian;Griesinger, Christian;Kolbe, Michael;Baker, David;Becker, Stefan;Lange, Adam
通讯作者：
Lange, Adam
影响因子：
2.4
作者：
FORSTER, T
通讯作者：
FORSTER, T