DNA–Au (111) interactions and transverse charge transport properties for DNA-based electronic devices
DNA–Au (111) interactions and transverse charge transport properties for DNA-based electronic devices
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DNA-Au (111) 相互作用和基于 DNA 的电子器件的横向电荷传输特性
DOI：
10.1039/d2cp05009a
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发表时间：
2023
影响因子：
3.3
通讯作者：
Oren, Ersin Emre
中科院分区：
文献类型：
--
作者：
Demir, Busra;Mohammad, Hashem;Anantram, M. P.;Oren, Ersin Emre
DNA的电荷转移和自组装特性使其成为过去二十年来分子电子学的标志。基于DNA的纳米电子应用和器件需要使用DNA纳米结构的具有可编程特性的快速有效的电荷转移机制。在这个过程中，DNA与无机底物整合的能力变得至关重要。这种整合可能会影响DNA的构象，改变其电荷传输特性。因此，我们利用分子动力学模拟和第一性原理计算，结合绿色函数方法，探讨了Au（111）基底对DNA构象的影响，并分析了其对电荷输运的影响。我们的研究结果表明，DNA序列，导致其在Au衬底上的分子构象，是工程师的电荷传输性能的关键。我们证明，DNA波动的黄金基板上，随着时间的推移，采样各种不同的构象。在这些不同的构象之间，分子轨道的能级、空间位置和DNA/Au接触原子可以不同。根据序列的不同，在HOMO上，前十种构象之间的电荷传输差异高达60倍。我们证明了核碱基的相对位置是决定构象和轨道之间的耦合的关键。我们预计，这些结果可以扩展到其他无机表面，并为理解DNA-无机界面相互作用，为未来基于DNA的电子器件应用铺平了道路。
DNA's charge transfer and self-assembly characteristics have made it a hallmark of molecular electronics for the past two decades. A fast and efficient charge transfer mechanism with programmable properties using DNA nanostructures is required for DNA-based nanoelectronic applications and devices. The ability to integrate DNA with inorganic substrates becomes critical in this process. Such integrations may affect the conformation of DNA, altering its charge transport properties. Thus, using molecular dynamics simulations and first-principles calculations in conjunction with Green's function approach, we explore the impact of the Au (111) substrate on the conformation of DNA and analyze its effect on the charge transport. Our results indicate that DNA sequence, leading to its molecular conformation on the Au substrate, is critical to engineer charge transport properties. We demonstrate that DNA fluctuates on a gold substrate, sampling various distinct conformations over time. The energy levels, spatial locations of molecular orbitals and the DNA/Au contact atoms can differ between these distinct conformations. Depending on the sequence, at the HOMO, the charge transmission differs up to 60 times between the top ten conformations. We demonstrate that the relative positions of the nucleobases are critical in determining the conformations and the coupling between orbitals. We anticipate that these results can be extended to other inorganic surfaces and pave the way for understanding DNA–inorganic interface interactions for future DNA-based electronic device applications.