Electronic transport through single molecules has been studied extensively by academic and industrial research groups. Discrete tunnel junctions, or molecular diodes, have been reported using scanning probes, break junctions, metallic crossbars and nanopores. For technological applications, molecular tunnel junctions must be reliable, stable and reproducible. The conductance per molecule, however, typically varies by many orders of magnitude. Self-assembled monolayers (SAMs) may offer a promising route to the fabrication of reliable devices, and charge transport through SAMs of alkanethiols within nanopores is well understood, with non-resonant tunnelling dominating the transport mechanism. Unfortunately, electrical shorts in SAMs are often formed upon vapour deposition of the top electrode, which limits the diameter of the nanopore diodes to about 45 nm. Here we demonstrate a method to manufacture molecular junctions with diameters up to 100 microm with high yields (> 95 per cent). The junctions show excellent stability and reproducibility, and the conductance per unit area is similar to that obtained for benchmark nanopore diodes. Our technique involves processing the molecular junctions in the holes of a lithographically patterned photoresist, and then inserting a conducting polymer interlayer between the SAM and the metal top electrode. This simple approach is potentially low-cost and could pave the way for practical molecular electronics.

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For organic semiconductors to find ubiquitous electronics applications, the development of new materials with high mobility and air stability is critical. Despite the versatility of carbon, exploratory chemical synthesis in the vast chemical space can be hindered by synthetic and characterization difficulties. Here we show that in silico screening of novel derivatives of the dinaphtho[2,3-b:2′,3′-f]thieno[3,2-b]thiophene semiconductor with high hole mobility and air stability can lead to the discovery of a new high-performance semiconductor. On the basis of estimates from the Marcus theory of charge transfer rates, we identified a novel compound expected to demonstrate a theoretic twofold improvement in mobility over the parent molecule. Synthetic and electrical characterization of the compound is reported with single-crystal field-effect transistors, showing a remarkable saturation and linear mobility of 12.3 and 16 cm2 V−1 s−1, respectively. This is one of the very few organic semiconductors with mobility greater than 10 cm2 V−1 s−1 reported to date.

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The electrical transport through self-assembled monolayers of alkanedithiols was studied in large-area molecular junctions and described by the Simmons model [Simmons JG (1963) J Appl Phys 34:1793-1803 and 2581-2590] for tunneling through a practical barrier, i.e., a rectangular barrier with the image potential included. The strength of the image potential depends on the value of the dielectric constant. A value of 2.1 was determined from impedance measurements. The large and well defined areas of these molecular junctions allow for a simultaneous study of the capacitance and the tunneling current under operational conditions. Electrical transport for octanedithiol through tetradecanedithiol self-assembled monolayers up to 1 V can simultaneously be described by a single effective mass and a barrier height. There is no need for additional fit constants. The barrier heights are in the order of 4 -5 eV and vary systematically with the length of the molecules. Irrespective of the length of the molecules, an effective mass of 0.28 was determined, which is in excellent agreement with theoretical predictions. and consist of a saturated carbon backbone with one (or two) thiol end groups. Experimentally, the tunneling current through a monolayer of alkane(di)thiols was shown to be temperatureindependent and to decrease exponentially with increasing molecular length (4, 5). The transport has been interpreted in terms of the classical tunneling model through a thin insulating film as provided by Simmons (24,25). In this model the tunneling current depends on the mean value of the barrier height, allowing for a simplification of the problem of an arbitrarily shaped potential barrier to that of a rectangular barrier. This model has been applied to junctions based on SAMs (4, 26), but an extra fit parameter ␣ is needed to obtain a fit to the measured data. However, as already explained by Simmons (24, 25), for a practical tunnel junction the image potential has to be taken into account. This effect has been neglected in the literature so far.The system studied in this article is a tunnel junction with an alkanedithiol SAM as the insulating film, a bottom gold electrode, and a highly conducting polymer as a top contact. The polymeric top contact allows for the fabrication of devices with a yield of almost unity for areas up to 100 m in diameter (5). The highly conducting polymer used is PEDOT:PSS, a waterbased suspension of poly(3,4-ethylenedioxythiophene) stabilized with poly(4-styrenesulfonic acid). The polymer acts as a cushion for the thermally evaporated metal atoms to land on and prevents the metal atoms from penetration into the molecular layer. Consequently, the formation of electrical shorts is prevented (27). Simmons ModelThe tunneling current density J through a rectangular potential barrier with height 0 is given by (4, 24, 26):wherewhere ⌬s is the barrier width at the Fermi level of the electrodes, here equal to the total length s of the tunneling path between the electrodes, m e is the bare electron mass, V is th...

To realize the potential of artificial intelligence in medical imaging, improvements in imaging capabilities are required, as well as advances in computing power and algorithms. Hybrid inorganic–organic metal halide perovskites, such as methylammonium lead triiodide (MAPbI3), offer strong X-ray absorption, high carrier mobilities (µ) and long carrier lifetimes (τ), and they are promising materials for use in X-ray imaging. However, their incorporation into pixelated sensing arrays remains challenging. Here we show that X-ray flat-panel detector arrays based on microcrystalline MAPbI3 can be created using a two-step manufacturing process. Our approach is based on the mechanical soft sintering of a freestanding absorber layer and the subsequent integration of this layer on a pixelated backplane. Freestanding microcrystalline MAPbI3 wafers exhibit a sensitivity of 9,300 µC Gyair–1 cm–2 with a μτ product of 4 × 10–4 cm2 V–1, and the resulting X-ray imaging detector, which has 508 pixels per inch, combines a high spatial resolution of 6 line pairs per millimetre with a low detection limit of 0.22 nGyair per frame.

The ultimate target of molecular electronics is to combine different types of functional molecules into integrated circuits, preferably through an autonomous self-assembly process. Charge transport through self-assembled monolayers has been investigated previously, but problems remain with reliability, stability and yield, preventing further progress in the integration of discrete molecular junctions. Here we present a technology to simultaneously fabricate over 20,000 molecular junctions-each consisting of a gold bottom electrode, a self-assembled alkanethiol monolayer, a conducting polymer layer and a gold top electrode-on a single 150-mm wafer. Their integration is demonstrated in strings where up to 200 junctions are connected in series with a yield of unity. The statistical analysis on these molecular junctions, for which the processing parameters were varied and the influence on the junction resistance was measured, allows for the tentative interpretation that the perpendicular electrical transport through these monolayer junctions is factorized.

Take-down policy If you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediately and investigate your claim. The orientation of alkanedithiol molecules in self-assembled monolayers (SAMs) is of vital importance for their transport properties in molecular junctions. It is demonstrated that a too-low concentration of long alkanedithiols in ethanol leads to the formation of looped molecules, resulting in a 50-fold increase of the current through the SAM. X-ray photoelectron spectroscopy measurements show that high-concentration dithiol solutions result in a preferential standing-up phase. To obtain an almost full standing-up phase of 1,14-tetradecanedithiol (C14) a 30 mm concentration in ethanol is required, whereas a 0.3 mm concentration leads to a highly looped monolayer. The conduction through the full standing-up phase of C14 and C16 is in accordance with the exponential dependence on molecule length as obtained from shorter alkanedithiols.