Zang Yaping, Ray Suman, Fung E-Dean, Borges Anders, Garner Marc H, Steigerwald Michael L, Solomon Gemma C, Patil Satish, Venkataraman Latha
Department of Applied Physics and Applied Mathematics , Columbia University , New York , New York 10027 , United States.
Solid State and Structural Chemistry Unit , Indian Institute of Science , Bangalore 560012 , India.
J Am Chem Soc. 2018 Oct 17;140(41):13167-13170. doi: 10.1021/jacs.8b06964. Epub 2018 Oct 5.
We study the single-molecule transport properties of small bandgap diketopyrrolopyrrole oligomers (DPP n, n = 1-4) with lengths varying from 1 to 5 nm. At a low bias voltage, the conductance decays exponentially as a function of length indicative of nonresonant transport. However, at a high bias voltage, we observe a remarkably high conductance close to 10 G with currents reaching over 0.1 μA across all four oligomers. These unique transport properties, together with density functional theory-based transport calculations, suggest a mechanism of resonant transport across the highly delocalized DPP backbones in the high bias regime. This study thus demonstrates the unique properties of diketopyrrolopyrrole derivatives in achieving highly efficient long-range charge transport in single-molecule devices.
我们研究了长度在1至5纳米之间变化的小带隙二酮吡咯并吡咯低聚物(DPP n,n = 1 - 4)的单分子输运性质。在低偏置电压下,电导随长度呈指数衰减,这表明是非共振输运。然而,在高偏置电压下,我们观察到所有四种低聚物的电导都非常高,接近10 G,电流超过0.1 μA。这些独特的输运性质,结合基于密度泛函理论的输运计算,表明在高偏置状态下,通过高度离域的DPP主链存在共振输运机制。因此,本研究证明了二酮吡咯并吡咯衍生物在单分子器件中实现高效长程电荷输运方面的独特性质。