Adhesion of Photon-Driven Molecular Motors to Surfaces via 1,3-Dipolar Cycloadditions: Effect of Interfacial Interactions on Molecular Motion

Adhesion of Photon-Driven Molecular Motors to Surfaces via 1,3-Dipolar Cycloadditions: Effect of Interfacial Interactions on Molecular Motion
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DOI:
10.1021/nn102876j
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发表时间:
2011-01-01
期刊:
影响因子:
17.1
通讯作者:
Feringa, Ben L.
Feringa, Ben L.
中科院分区:
材料科学1区
文献类型:
--
作者:
Carroll, Gregory T.;London, Gabor;Feringa, Ben L.

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我们报道了利用1,3-偶极环加成反应将垂直光驱动的分子马达连接到表面。分子马达被设计成含有叠氮化物或炔基团,用于连接到炔或叠氮化物改性的表面。通过紫外可见光谱、红外光谱、X射线光电子能谱和椭偏仪等测试手段对表面结合进行了表征。发现表面结合的马达会发生光化学和热异构化,与溶液中的单向旋转一致。限制在一个表面被发现,以减少热异构化过程的速率。热异构化的速率也取决于马达的表面覆盖度。在溶液中,伴随热异构化的UV-vis信号的变化可以用单个单指数衰减拟合。与此相反,热异构化的表面结合的电机不遵循一个单一的单指数衰减,并被发现适合双指数衰减。单腿和双腿马达都附着在表面上。热异构化的动力学不受影响的化合价的附件,表明动力学的变化,从溶液到表面系统的表面结合电机之间的相互作用。
We report the attachment of altitudinal light-driven molecular motors to surfaces using 1,3-dipolar cycloaddition reactions. Molecular motors were designed containing azide or alkyne groups for attachment to alkyne- or azide-modified surfaces. Surface attachment was characterized by UV-vis, IR, XPS, and ellipsometry measurements. Surface-bound motors were found to undergo photochemical and thermal isomerizations consistent with unidirectional rotation in solution. Confinement at a surface was found to reduce the rate of the thermal isomerization process. The rate of thermal isomerization was also dependent on the surface coverage of the motors. In solution, changes in the UV-vis signal that accompany thermal isomerization can be fit with a single monoexponential decay. In contrast, thermal isomerization of the surface-bound motors does not follow a single monexponential decay and was found to fit a biexponential decay. Both one- and two-legged motors were attached to surfaces. The kinetics of thermal isomerization was not affected by the valency of attachment, indicating that the change in kinetics from solution to surface systems are related to interactions between the surface-bound motors.