期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 140, 期 44, 页码 15080-15088出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b10296
关键词
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资金
- NSF [CHE-1404922, CHE-1764256, 11-44155]
- Danish Council for Independent Research\Natural Sciences
- National Natural Science Foundation of China [21473113, 51502173, 21772123]
- Program of Shanghai Academic/Technology Research Leader [16XD1402700]
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning [2013-57]
- Shanghai Education Development Foundation
- Shuguang Program - Shanghai Municipal Education Commission [14SG40]
- Program for Changjiang Scholars, Innovative Research Team in University [IRT1269]
- International Joint Laboratory on Resource Chemistry (IJLRC)
Linear silanes are efficient molecular wires due to strong sigma-conjugation in the transoid conformation; however, the structure-function relationship for the conformational dependence of the single-molecule conductance of silanes remains untested. Here we report the syntheses, electrical measurements, and theoretical characterization of four series of functionalized cyclic and bicyclic silanes including a cyclotetrasilane, a cyclopentasilane, a bicyclo[2.2.1]heptasilane, and a bicyclo[2.2.2]octasilane, which are all extended by linear silicon linkers of varying length. We find an unusual variation of the single-molecule conductance among the four series at each linker length. We determine the relative conductance of the (bi)cyclic silicon structures by using the common length dependence of the four series rather than comparing the conductance at a single length. In contrast with the cyclic a pi-conjugated molecules, the conductance of sigma-conjugated (bi)cyclic silanes is dominated by a single path through the molecule and is controlled by the dihedral angles along this path. This strong sensitivity to molecular conformation dictates the single-molecule conductance of sigma-conjugated silanes and allows for systematic control of the conductance through molecular design.
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