Organic conductors are being evaluated for potential use in waste heat recovery through lightweight and flexible thermoelectric generators manufactured using cost-effective printing processes. Assessment of the potentiality of organic materials in real devices still requires a deeper understanding of the physics behind their thermoelectric properties, which can pave the way toward further development of the field. This article reports a detailed thermoelectric study of a set of highly conducting inkjet-printed films of commercially available poly(3,4-ethylenedioxythiophene) polystyrene sulfonate formulations characterized by in-plane electrical conductivity, spanning the interval 10-500 S/cm. The power factor is maximized for the formulation showing an intermediate electrical conductivity. The Seebeck coefficient is studied in the framework of Mott's relation, assuming a (semi-)classical definition of the transport function. Ultraviolet photoelectron spectroscopy at the Fermi level clearly indicates that the shape of the density of states alone is not sufficient to explain the observed Seebeck coefficient, suggesting that carrier mobility is important in determining both the electrical conductivity and thermopower. Finally, the cross-plane thermal conductivity is reliably extracted thanks to a scaling approach that can be easily performed using typical pump-probe spectroscopy.
Solution-processed organic semiconductors enable the fabrication of large-area and flexible electronics by means of cost-effective, solution-based mass manufacturing techniques.However, for many applications an insoluble active layer can offer technological advantages in terms of robustness to processing solvents. This is particularly relevant in field-effect transistors (FET), where processing of dielectrics or barriers from solution on top of the semiconductor layer typically imposes the use of orthogonal solvents in order not to interfere with the nanometer thick accumulation channel. To this end, the use of latent pigments, highly soluble molecules which can produce insoluble films after a post-deposition thermal cleavage of solubilizing groups, is a very promising strategy. In this contribution, we demonstrate the use of tert-Butyloxycarbonyl (t-Boc) functionalized diketopyrrolopyrrole and perylene-diimide small molecules for good hole and electron transporting films. t-Boc thermal cleavage produces a densification of the films, along with a strong structural rearrangement of the deprotected molecules, strongly improving charge mobility in both p-and n-type FET. We also highlight the robustness of these highly insoluble semiconducting layers to typical and aggressive processing solvents. These results can greatly enhance the degree of freedom in the manufacturing of multi-layered organic electronic devices, offering enhanced stability to harsh processing steps.
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