Temporal control of i-motif switch lifetimes for autonomous operation of transient DNA nanostructures
Temporal control of i-motif switch lifetimes for autonomous operation of transient DNA nanostructures
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DOI：
10.1039/c7sc00646b
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发表时间：
2017-05-01
期刊：
影响因子：
8.4
通讯作者：
Walther, A.
中科院分区：
文献类型：
--
作者：
Heinen, L.;Walther, A.
功能性DNA纳米技术创造了越来越复杂的行为，可用于传感，驱动或计算，通过整合动态和响应性结构DNA基序实现。然而，由于繁琐且非常系统特异性的序列设计，具有可编程寿命的时间控制和动态DNA结构能够自主操作并自恢复到起始状态，因此实现具有挑战性。在这里，我们提出了一个简单的概念，程序的瞬时寿命到DNA双链体的基础上的pH敏感的DNA i基序开关。我们使用合理设计的化学反应框架将i基序开关与内部非线性pH重置功能集成，通过该化学反应框架，开关自主地经历完整的“关-开-关”循环，而无需使用额外的外部触发器。激活的“开”状态（即，混合状态）的寿命可以在几个小时内系统地编程。该系统可以很容易地实现为更大长度尺度上的杂交DNA结构。专注于自主材料，我们展示了瞬态荧光信号的时间控制和金纳米粒子的临时聚集。
Functional DNA nanotechnology creates increasingly complex behaviors useful for sensing, actuation or computation, as enabled via the integration of dynamic and responsive structural DNA motifs. However, temporally controlled and dynamic DNA structures with programmable lifetimes, that are able to operate autonomously and self-revert to the starting state are challenging to achieve due to tedious and very system-specific sequence design. Here, we present a straightforward concept to program transient lifetimes into DNA duplexes based on the pH-sensitive DNA i-motif switch. We integrate the i-motif switch with an internal, non-linear pH-resetting function using a rationally designed chemical reaction framework, by which the switch autonomously undergoes a complete "off-on-off"-cycle without the use of additional external triggers. The lifetime of the activated "on"-state (i.e. the hybridized state) can be systematically programmed over several hours. The system can be readily implemented into hybrid DNA structures on larger length scales. Focusing on autonomous materials, we demonstrate temporal control of transient fluorescence signals and temporary aggregation of gold nanoparticles.