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Humidity-controlled rectification switching in ruthenium-complex molecular junctions
Nature Nanotechnology ( IF 38.3 ) Pub Date : 2017-12-04 , DOI: 10.1038/s41565-017-0016-8
Huseyin Atesci , Veerabhadrarao Kaliginedi , Jose A. Celis Gil , Hiroaki Ozawa , Joseph M. Thijssen , Peter Broekmann , Masa-aki Haga , Sense Jan van der Molen

Although molecular rectifiers were proposed over four decades ago1,2, until recently reported rectification ratios (RR) were rather moderate2,3,4,5,6,7,8,9,10,11 (RR ~ 101). This ceiling was convincingly broken using a eutectic GaIn top contact12 to probe molecular monolayers of coupled ferrocene groups (RR ~ 105), as well as using scanning tunnelling microscopy-break junctions13,14,15,16 and mechanically controlled break junctions17 to probe single molecules (RR ~ 102–103). Here, we demonstrate a device based on a molecular monolayer in which the RR can be switched by more than three orders of magnitude (between RR ~ 100 and RR ≥ 103) in response to humidity. As the relative humidity is toggled between 5% and 60%, the current–voltage (IV) characteristics of a monolayer of di-nuclear Ru-complex molecules reversibly change from symmetric to strongly asymmetric (diode-like). Key to this behaviour is the presence of two localized molecular orbitals in series, which are nearly degenerate in dry circumstances but become misaligned under high humidity conditions, due to the displacement of counter ions (PF6 ). This asymmetric gating of the two relevant localized molecular orbital levels results in humidity-controlled diode-like behaviour.



中文翻译:

钌-复杂分子结中的湿度控制整流开关

尽管在四十年前就提出了分子整流器1,2,但直到最近报道的整流比(RR)还是相当适中的2,3,4,5,6,7,8,9,10,11(RR〜10 1)。使用共晶GaIn顶部触点12令人信服地打破了天花板,以探测偶合的二茂铁基团的分子单分子层(RR〜10 5),以及使用扫描隧道显微镜-断裂连接点13、14、15、16和机械控制的断裂连接点17探测单个分子(RR〜10 2 –10 3)。在这里,我们演示了一种基于分子单分子层的器件,其中,响应湿度,可以将RR切换三个以上数量级(在RR〜10 0和RR≥10 3之间)。随着相对湿度为5%和60%时,电流-电压之间切换(- V)二核钌络合物分子的单层的特性可逆地从对称改变为强不对称(二极管等)。此行为的关键是存在两个串联的局部分子轨道,它们在干燥环境下几乎退化,但由于抗衡离子的置换,在高湿度条件下会失准(PF 6 )。两个相关的局部分子轨道能级的这种不对称门控导致湿度控制的类似二极管的行为。

更新日期:2017-12-05
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