Transport and noise in organic field-effect devices K. Morawetz, 1,2,3 S. Gemming, 1 R. Luschtinetz, 4 T. Kunze, 1 P. Lipavský, 5,6 L. M. Eng, 7 G. Seifert, 4 V. Pankoke, 1 and P. Milde 7 1 Forschungszentrum Dresden-Rossendorf, PF 51 01 19, 01314 Dresden, Germany 2 International Center for Condensed Matter Physics, 70904-910 Brasília-DF, Brazil 3 Max-Planck-Institute for the Physics of Complex Systems, Nöthnitzer Strasse 38, 01187 Dresden, Germany 4 Institute of Physical Chemistry and Electrochemistry, TU Dresden, 01062 Dresden, Germany 5 Faculty of Mathematics and Physics, Charles University, Ke Karlovu 3, 12116 Prague 2, Czech Republic 6 Institute of Physics, Academy of Sciences, Cukrovarnická 10, 16253 Prague 6, Czech Republic 7 Institute of Applied Photophysics, TU Dresden, 01062 Dresden, Germany Received 2 October 2008; revised manuscript received 19 December 2008; published 4 February 2009 The transport and fluctuation properties of organic molecules ordered parallel between two Au contact leads are investigated by the method of surface Green’s function. From first-principles simulation the relevant hopping parameters are extracted and used to calculate nonlinear transport coefficients with respect to an external bias voltage. A staggering of conductance is found in dependence on the number of molecules squeezed in between the contacts. The thermal properties show an anomalous behavior whenever the voltage reaches the values of the molecular energy levels active for transport. The thermoelectric figure of merit shows a resonance allowing one to reach values even larger than one. DOI: 10.1103/PhysRevB.79.085405 PACS numbers: 73.63.Fg, 85.85.j, 87.15.hj, 73.23.b I. INTRODUCTION The goal to develop low-cost storage and microelectronic devices has triggered an enormous activity in the research of organic field-effect transistors OFETsbased on different polymers 13 and small organic molecules. 4 It is desirable that the molecular material possesses a high structural ordering 5,6 in order to reach high charge carrier mobilities and low re- sistive losses. Among the most promising materials are olig- othiophenes and their derivatives. 7 This is due to the variety of intra- and intermolecular interactions, which originates from the polarizability of the sulfur electrons and the embed- ding aromatic -electron system. 810 The performance of OFETs based on oligothiophenes 3 shows characteristic features, e.g., the current starts at a cer- tain threshold of gate voltage and reaches a saturation value for certain drain voltages. In general, the charge transport occurs in the direction perpendicular to the plane of the thiophene rings due to good stacking. This suggests a con- struction of devices with parallel ordered molecular rings. This is the perpendicular direction to the usually considered transport through various molecule classes ranging from transport dependent on the thickness 11 to metallic behavior independent of the thickness of molecules. 12 Thick-film de- vices based on thiophenes were reported several years ago. 13 Recently an OFET structure has been built from ultrathin self-assembled films made up from oligothiophenes, which are arranged in a highly-order lamellar stacking perpendicu- lar to the substrate surface 3 as illustrated in Figs. 1 and 2. The energy gap between the lowest unoccupied molecular orbital LUMOand the highest occupied molecular orbital HOMOlevels measures about 3 eV in quarterthiophene. For the molecular structure, see Fig. 1. In contrast to the conduction and valence band in semiconductors the transport is due to localized states dominated by hopping 14,15 rather than due to delocalized states limited by the scattering in semiconductors. If one considers the charge transport between the mol- ecules one can think of two extreme mechanisms. On one side one has either the ballistic transport through bonds or the hopping transport through space. The diffusive transport on the other side is present if the carriers meet scattering partners. For the present situation of parallel stacked mol- ecules the hopping transport by tunneling between the local- ized HOMO or LUMO states is the relevant one. A related mechanism of charge transfer due to the bending motion of molecules by touching might lead to shuttling transport 16 which could be investigated by resonant spectroscopy. 17 Of course, the most crucial question is the tilting of molecules triggered by the metal-molecule contacts 18 which requires a refined interface engineering. 19 FIG. 1. Color onlineThe thiophene molecules between two Au contacts. PHYSICAL REVIEW B 79, 085405 2009 1098-0121/2009/798/08540512©2009 The American Physical Society 085405-1