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Inverse Square-Root Field Dependence of Conductivity in Organic Field-Effect Transistors

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 Added by Jianhua Wei
 Publication date 2008
  fields Physics
and research's language is English




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Two-dimensional atomic crystals are extensively studied in recent years due to their exciting physics and device applications. However, a molecular counterpart, with scalable processability and competitive device performance, is still challenging. Here, we demonstrate that high-quality few-layer dioctylbenzothienobenzothiophene molecular crystals can be grown on graphene or boron nitride substrate via van der Waals epitaxy, with precisely controlled thickness down to monolayer, large-area single crystal, low process temperature and patterning capability. The crystalline layers are atomically smooth and effectively decoupled from the substrate due to weak van der Waals interactions, affording a pristine interface for high-performance organic transistors. As a result, monolayer dioctylbenzothienobenzothiophene molecular crystal field-effect transistors on boron nitride show record-high carrier mobility up to 10cm2V-1s-1 and aggressively scaled saturation voltage around 1V. Our work unveils an exciting new class of two-dimensional molecular materials for electronic and optoelectronic applications.
The surface conductivity is measured by a four-probe technique for pentacene and rubrene single-crystals laminated on polarized and nearly unpolarized molecular monolayers with application of perpendicular electric fields. The polarization of the self-assembled monolayers (SAMs) shifts the threshold gate voltage, while maintaining a very low subthreshold swing of the single-crystal devices (0.11 V/decade). The results, excluding influences of parasitic contacts and grain boundaries, demonstrate SAM-induced nanoscale charge injection up to ~10^12 cm^-2 at the surface of the organic single crystals.
We demonstrate controllable shift of the threshold voltage and the turn-on voltage in pentacene thin film transistors and rubrene single crystal field effect transistors (FET) by the use of nine organosilanes with different functional groups. Prior to depositing the organic semiconductors, the organosilanes were applied to the SiO2 gate insulator from solution and form a self assembled monolayer (SAM). The observed shift of the transfer characteristics range from -2 to 50 V and can be related to the surface potential of the layer next to the transistor channel. Concomitantly the mobile charge carrier concentration at zero gate bias reaches up to 4*10^12/cm^2. In the single crystal FETs the measured transfer characteristics are also shifted, while essentially maintaining the high quality of the subthreshold swing. The shift of the transfer characteristics is governed by the built-in electric field of the SAM and can be explained using a simple energy level diagram. In the thin film devices, the subthreshold region is broadened, indicating that the SAM creates additional trap states, whose density is estimated to be of order 1*10^12/cm^2.
Organic semiconductors have generated considerable interest for their potential for creating inexpensive and flexible devices easily processed on a large scale [1-11]. However technological applications are currently limited by the low mobility of the charge carriers associated with the disorder in these materials [5-8]. Much effort over the past decades has therefore been focused on optimizing the organisation of the material or the devices to improve carrier mobility. Here we take a radically different path to solving this problem, namely by injecting carriers into states that are hybridized to the vacuum electromagnetic field. These are coherent states that can extend over as many as 10^5 molecules and should thereby favour conductivity in such materials. To test this idea, organic semiconductors were strongly coupled to the vacuum electromagnetic field on plasmonic structures to form polaritonic states with large Rabi splittings ca. 0.7 eV. Conductivity experiments show that indeed the current does increase by an order of magnitude at resonance in the coupled state, reflecting mostly a change in field-effect mobility as revealed when the structure is gated in a transistor configuration. A theoretical quantum model is presented that confirms the delocalization of the wave-functions of the hybridized states and the consequences on the conductivity. While this is a proof-of-principle study, in practice conductivity mediated by light-matter hybridized states is easy to implement and we therefore expect that it will be used to improve organic devices. More broadly our findings illustrate the potential of engineering the vacuum electromagnetic environment to modify and to improve properties of materials.
We report low temperature scanning tunneling microscopy characterization of MoSe2 crystals, and the fabrication and electrical characterization of MoSe2 field-effect transistors on both SiO2 and parylene-C substrates. We find that the multilayer MoSe2 devices on parylene-C show a room temperature mobility close to the mobility of bulk MoSe2 (100 cm2V-1s-1 - 160 cm2V-1s-1), which is significantly higher than that on SiO2 substrate (~50 cm2V-1s-1). The room temperature mobility on both types of substrates are nearly thickness independent. Our variable temperature transport measurements reveal a metal-insulator transition at a characteristic conductivity of e2/h. The mobility of MoSe2 devices extracted from the metallic region on both SiO2 and parylene-C increases up to ~ 500 cm2V-1s-1 as the temperature decreases to ~ 100 K, with the mobility of MoSe2 on SiO2 increasing more rapidly. In spite of the notable variation of charged impurities as indicated by the strongly sample dependent low temperature mobility, the mobility of all MoSe2 devices on SiO2 converges above 200 K, indicating that the high temperature (> 200 K) mobility in these devices is nearly independent of the charged impurities. Our atomic force microscopy study of SiO2 and parylene-C substrates further rule out the surface roughness scattering as a major cause of the substrate dependent mobility. We attribute the observed substrate dependence of MoSe2 mobility primarily to the surface polar optical phonon scattering originating from the SiO2 substrate, which is nearly absent in MoSe2 devices on parylene-C substrate.
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