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Molecular Orbital Gating Surface-Enhanced Raman Scattering
ACS Nano ( IF 15.8 ) Pub Date : 2018-10-15 00:00:00 , DOI: 10.1021/acsnano.8b05826
Chenyang Guo 1 , Xing Chen 2 , Song-Yuan Ding 3 , Dirk Mayer 4 , Qingling Wang 1 , Zhikai Zhao 1, 5 , Lifa Ni 1, 6 , Haitao Liu 1 , Takhee Lee 5 , Bingqian Xu 6 , Dong Xiang 1
Affiliation  

One of the promising approaches to meet the urgent demand for further device miniaturization is to create functional devices using single molecules. Although various single-molecule electronic devices have been demonstrated recently, single-molecule optical devices which use external stimulations to control the optical response of a single molecule have rarely been reported. Here, we propose and demonstrate a field-effect Raman scattering (FERS) device with a single molecule, an optical counterpart to field-effect transistors (a key component of modern electronics). With our devices, the gap size between electrodes can be precisely adjusted at subangstrom accuracy to form single molecular junctions as well as to reach the maximum performance of Raman scattering via plasmonic enhancement. Based on this maximum performance, we demonstrated that the intensity of Raman scattering can be further enhanced by an additional ∼40% if the orbitals of the molecules bridged two electrodes were shifted by a gating voltage. This finding not only provides a method to increase the sensitivity of Raman scattering beyond the limit of plasmonic enhancement, but also makes it feasible to realize addressable functional FERS devices with a gate electrode array.

中文翻译:

分子轨道门控表面增强拉曼散射

满足对进一步的设备小型化的迫切需求的有前途的方法之一是使用单分子创建功能性设备。尽管最近已经证明了各种单分子电子设备,但是很少报道了使用外部刺激来控制单个分子的光学响应的​​单分子光学设备。在这里,我们提出并演示了一种具有单个分子的场效应拉曼散射(FERS)装置,它是场效应晶体管(现代电子学的关键组件)的光学对应物。使用我们的设备,电极之间的间隙尺寸可以精确到亚埃精度进行调整,以形成单个分子结,并通过等离激元增强达到拉曼散射的最大性能。基于此最高性能,我们证明,如果跨接两个电极的分子的轨道因门控电压而移位,则拉曼散射的强度可进一步提高约40%。该发现不仅提供了一种将拉曼散射的灵敏度提高到超过等离子体增强极限的方法,而且使得实现具有栅电极阵列的可寻址功能性FERS器件成为可行。
更新日期:2018-10-15
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