Mapping orientational order of charge-probed domains in a semiconducting polymer.

Structure-property relationships are of fundamental importance to develop quantitative models describing charge transport in organic semiconductor based electronic devices, which are among the best candidates for future portable and lightweight electronic applications. While microstructural investigations, such as those based on X-rays, electron microscopy, or polarized optical probes, provide necessary information for the rationalization of transport in macromolecular solids, a general model predicting how charge accommodates within structural maps is not yet available. Therefore, techniques capable of directly monitoring how charge is distributed when injected into a polymer film and how it correlates to structural domains can help fill this gap. Supported by density functional theory calculations, here we show that polarized charge modulation microscopy (p-CMM) can unambiguously and selectively map the orientational order of the only conjugated segments that are probed by mobile charge in the few nanometer thick accumulation layer of a high-mobility polymer-based field-effect transistor . Depending on the specific solvent-induced microstructure within the accumulation layer, we show that p-CMM can image charge-probed domains that extend from submicrometer to tens of micrometers size, with markedly different degrees of alignment. Wider and more ordered p-CMM domains are associated with improved carrier mobility, as extracted from device characteristics. This observation evidences the unprecedented opportunity to correlate, directly in a working device, electronic properties with structural information on those conjugated segments involved in charge transport at the buried semiconductor-dielectric interface of a field-effect device.

Dielectrophoretic assembly of high-density arrays of individual graphene devices for rapid screening.

We establish the use of dielectrophoresis for the directed parallel assembly of individual flakes and nanoribbons of few-layer graphene into electronic devices. This is a bottom-up approach where source and drain electrodes are prefabricated and the flakes are deposited from a solution using an alternating electric field applied between the electrodes. These devices are characterized by scanning electron microscopy, atomic force microscopy, Raman spectroscopy, and electron transport measurements. They are electrically active and their current carrying capacity and subsequent failure mechanism is revealed. Akin to carbon nanotubes, we show that the dielectrophoretic deposition is self-limiting to one flake per device and is scalable to ultralarge-scale integration densities, thereby enabling the rapid screening of a large number of devices.

Molecular packing effects on the optical spectra and triplet dynamics in oligofluorene films.

We report on the triplet spectra and dynamics in two types of oligomeric films deposited by two different techniques: thermal evaporation and spin coating. The different molecular arrangement in both films is manifested in a red shift of the absorption, PL, and T1-Tn absorption spectra of the sublimated film relative to the spin-coated one. Triplet recombination dynamics studied with steady-state photoinduced absorption (PA) spectroscopy follow a dispersive bimolecular recombination model away from the trap filling regime. We obtained values for the triplet bimolecular recombination ratio (beta) of 3.4 x 10 (-14) and 1.1 x 10 (-15) cm3 s (-1) for evaporated and spin-coated film, respectively, the difference being attributed to diverse molecular arrangement in both films.