Strong enhancement of the two-photon absorption of organic molecules near silver nanoparticle fractal clusters has been observed and has been exploited to yield composite materials with very strong two-photon absorption and two-photon-excited fluorescence properties. Measurements on cluster films coated with chromophoric polymer or with thiol-bound chromophores give spatially-averaged enhancements of 1000 and 20 000, respectively. Two-photon fluorescence microscopy studies show that the enhancements are spatially inhomogeneous, with peak-enhancement factors of g 10 000 (polymer/cluster) and g 160 000 (thiol chromophore/cluster), and excitation frequency dependent. These results are in accord with theoretical predictions of local-field effects due to strong localization of collective plasmon modes in fractal metal clusters, and demonstrate an approach to ultrasensitive two-photon processes.
3D free‐standing and embedded metallic structures with a height of 100 μm (see Figure and also cover) have been microfabricated and characterized. Polymer nanocomposites containing metal nanoparticles, a metal salt, and an appropriate photoreducing dye are found to be efficient precursors for direct laser writing of continuous metal structures. The authors offer a versatile new approach to the 2D and 3D patterning of metals on different length scales.
An asymmetric n-alkyl substitution pattern was realized in 2-tridecyl[1]benzothieno[3,2-b][1]benzothiophene (C(13)-BTBT) in order to improve the charge transport properties in organic thin-film transistors. We obtained large hole mobilities up to 17.2 cm(2)/(V·s) in low-voltage operating devices. The large mobility is related to densely packed layers of the BTBT π-systems at the channel interface dedicated to the substitution motif and confirmed by X-ray reflectivity measurements. The devices exhibit promising stability in continuous operation for several hours in ambient air.
We report a quantitative study that describes and correlates the threshold voltage of low-voltage organic field-effect transistors with the molecular structure of self-assembled monolayer dielectrics. We have observed that the component of the dipole moment of such self-assembled molecules perpendicular to the surface correlates linearly with the threshold voltage shift in devices. The model was validated using three different organic semiconductors (pentacene, α,α'-dihexylsexithiophene, and fullerene-C(60)) on six different self-assembled monolayers. The correlation found can help optimize future devices, by tuning the dipole moments of the molecules that constitute the self-assembled monolayer.
We report on p- and n-type organic self-assembled monolayer field effect transistors. On the base of quaterthiophene and fullerene units, multifunctional molecules were synthesized, which have the ability to self-assemble and provide multifunctional monolayers. The self-assembly approach, based on phosphonic acids, is very robust and allows the fabrication of functional devices even on larger areas. The p- and n-type transistor devices with only one molecular active layer were demonstrated for transistor channel lengths up to 10 μm. The monolayer composition is proven by electrical experiments and by high-resolution transmission electron microscopy, electron energy loss spectroscopy, XPS, and AFM experiments. Because of the molecular design and the contribution of isolating alkyl chains to the hybrid dielectric, our devices operate at low supply voltages (-4 V to +4 V), which is a key requirement for practical use and simplifies the integration in standard applications. The monolayer devices operate in ambient air and show hole and electron mobilities of 10(-5) cm(2)/(V s) and 10(-4) cm(2)/(V s) respectively. In particular the n-type operation of self-assembled monolayer transistors has not been reported before. Hereby, structure-property relations of the SAMs have been studied. Furthermore an approach to protect the sensitive C(60) from immediate degradation within the molecular design is provided.
Self-assembled monolayer field-effect transistors (SAMFETs) of BTBT functionalized phosphonic acids are fabricated. The molecular design enables device operation with charge carrier mobilities up to 10(-2) cm(2) V(-1) s(-1) and for the first time SAMFETs which operate on rough, flexible PEN substrates even under mechanical substrate bending.
Silver nanoparticles coated with a self-assembled layer of approximately 2500 chromophoric alkylthiol ligands, that exhibit a huge per particle two-photon absorption cross section (2.7 x 10-45 cm4 s photon-1) and a high fluorescence quantum yield (0.33), are reported. Polyfunctionalized variants of these nanoparticles have been produced that show reasonable solubility in water/ethanol mixtures. By virtue of the large number of tethered chromophores, these particles act as strongly two-photon absorbing nanobeacons and may have applications in fluorescence imaging and sensing.
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