Polycrystalline Organic Transistors Research Articles

Hall Effect in Polycrystalline Organic Semiconductors: The Effect of Grain Boundaries

AbstractHighly crystalline thin films in organic semiconductors are important for applications in high‐performance organic optoelectronics. Here, the effect of grain boundaries on the Hall effect and charge transport properties of organic transistors based on two exemplary benchmark systems is elucidated: (1) solution‐processed blends of 2,7‐dioctyl[1]benzothieno[3,2‐b][1]benzothiophene (C8‐BTBT) small molecule and indacenodithiophene‐benzothiadiazole (C16IDT‐BT) conjugated polymer, and (2) large‐area vacuum evaporated polycrystalline thin films of rubrene (C42H28). It is discovered that, despite the high field‐effect mobilities of up to 6 cm2 V−1 s−1 and the evidence of a delocalized band‐like charge transport, the Hall effect in polycrystalline organic transistors is systematically and significantly underdeveloped, with the carrier coherence factor α < 1 (i.e., yields an underestimated Hall mobility and an overestimated carrier density). A model based on capacitively charged grain boundaries explaining this unusual behavior is described. This work significantly advances the understanding of magneto‐transport properties of organic semiconductor thin films.

Microscopic gate-modulation imaging of charge and field distribution in polycrystalline organic transistors

In this work, a high-resolution microscopic gate-modulation imaging (μ-GMI) technique is successfully developed to visualize inhomogeneous charge and electric field distributions in operating organic thin-film transistors (TFTs). We conduct highly sensitive and diffraction-limit gate-modulation sensing for acquiring difference images of semiconducting channels between at gate-on and gate-off states that are biased at an alternate frequency of 15 Hz. As a result, we observe unexpectedly inhomogeneous distribution of positive and negative local gate-modulation (GM) signals at a probe photon energy of 1.85 eV in polycrystalline pentacene TFTs. Spectroscopic analyses based on a series of μ-GMI at various photon energies reveal that two distinct effects appear, simultaneously, within the polycrystalline pentacene channel layers: Negative GM signals at 1.85 eV originate from the second-derivative-like GM spectrum which is caused by the effect of charge accumulation, whereas positive GM signals originate from the first-derivative-like GM spectrum caused by the effect of leaked gate fields. Comparisons with polycrystalline morphologies indicate that grain centers are predominated by areas with high leaked gate fields due to the low charge density, whereas grain edges are predominantly high-charge-density areas with a certain spatial extension as associated with the concentrated carrier traps. Consequently, it is reasonably understood that larger grains lead to higher device mobility, but with greater inhomogeneity in charge distribution. These findings provide a clue to understand and improve device characteristics of polycrystalline TFTs.

Electric Field Confinement Effect on Charge Transport in Organic Field-Effect Transistors

While it is known that the charge-carrier mobility in organic semiconductors is only weakly dependent on the electric field at low fields, the experimental mobility in organic field-effect transistors using silylethynyl-substituted pentacene is found to be surprisingly field dependent at low source-drain fields. Corroborated by scanning Kelvin probe measurements, we explain this observation by the severe difference between local conductivities within grains and at grain boundaries. Redistribution of accumulated charges creates very strong local lateral fields in the latter regions. We further confirm this picture by verifying that the charge mobility in channels having no grain boundaries, made from the same organic semiconductor, is not significantly field dependent. We show that our model allows us to quantitatively model the source-drain field dependence of the mobility in polycrystalline organic transistors.

Correlation between interdomain carrier hopping and apparent mobility in polycrystalline organic transistors as investigated by electron spin resonance

Microscopic charge dynamics inside microcrystal domains and across domain boundaries in polycrystalline organic thin-film transistors (OTFTs) were resolved by angle- and temperature-dependent field-induced electron spin resonance (FI-ESR) spectroscopy. We utilized small-molecule and polymer-based polycrystalline OTFTs, both of which are composed of planar microdomains oriented uniaxially on the substrates. Two types of motional narrowing effect are observed at magnetic fields perpendicular and parallel to the substrate: In the former, we observed the motional narrowing effect due to intradomain transport, while in the latter, we observed another motional narrowing effect due to the carrier hopping across the domain boundaries, which averaged out the variation in $g$ factors between respective microdomains. The analyses revealed that the activation energies for the intradomain transport are between 5 and 21 meV, while those for the interdomain carrier hopping are between 45 and 90 meV. The latter ones coincide with those for the apparent mobility for the respective OTFTs. These results demonstrate that the charge transport is limited by the domain boundaries, which form rate-determining barrier potential both in small-molecule and polymer-based polycrystalline OTFTs.

Shedding light on organic transistors: insights could lead to brighter and cheaper displays

The first single-crystal organic transistor that can be switched on and off by light is giving physicists a unique peek into the way photons interact with organic semiconductors. For the makers of organic light-emitting diode (OLED) displays, which are used in everything from cameras to mobile phones, poor understanding of light's interactions with material properties becomes a problem. Today's amorphous or polycrystalline organic transistors are just not up to the job because bathing them in light generates unwanted photo-induced currents. In this paper, the author explains why the mobility drops as the temperature falls. In silicon transistors, the mobility increases as the material is cooled because electrons move more easily at low temperatures.