The electronic properties of silicon, such as the conductivity, are largely dependent on the density of the mobile charge carriers, which can be tuned by gating and impurity doping. When the device size scales down to the nanoscale, routine doping becomes problematic due to inhomogeneities. Here we report that a molecular monolayer, covalently grafted atop a silicon channel, can play a role similar to gating and impurity doping. Charge transfer occurs between the silicon and the molecules upon grafting, which can influence the surface band bending, and makes the molecules act as donors or acceptors. The partly charged end-groups of the grafted molecular layer may act as a top gate. The doping- and gating-like effects together lead to the observed controllable modulation of conductivity in pseudometal-oxide-semiconductor field-effect transistors (pseudo-MOSFETs). The molecular effects can even penetrate through a 4.92-mum thick silicon layer. Our results offer a paradigm for controlling electronic characteristics in nanodevices at the future diminutive technology nodes.

Nanoelectronic molecular and magnetic tunnel junction (MTJ) MRAM crossbar memory systems have the potential to present significant area advantages (4 to 6F(2)) compared to CMOS-based systems. The scalability of these conductivity-switched RAM arrays is examined by establishing criteria for correct functionality based on the readout margin. Using a combined circuit theoretical modelling and simulation approach, the impact of both the device and interconnect architecture on the scalability of a conductivity-state memory system is quantified. This establishes criteria showing the conditions and on/off ratios for the large-scale integration of molecular devices, guiding molecular device design. With 10% readout margin on the resistive load, a memory device needs to have an on/off ratio of at least 7 to be integrated into a 64 x 64 array, while an on/off ratio of 43 is necessary to scale the memory to 512 x 512.

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Silicon devices bearing grafted molecular monolayers have their conductance reversibly modulated. By alternately illuminating the samples with visible and near‐UV light, threshold‐voltage shifts occur to the negative and positive directions, respectively. This corresponds to charge transfer/redistribution between the silicon device and the grafted molecules.

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