The electronic nature of metal-semiconductor contacts is a fundamental issue in the understanding of semiconductor device physics, because such contacts control charge injection, and therefore play a major role in determining the electron/hole population in the semiconductor itself. This role is particularly important for organic semiconductors as they are generally used in their pristine, undoped form. Here, we review our progress in the understanding of the energy level line-up in finished, blue-emitting, polyfluorene-based light-emitting diodes, which exploit LiF and CsF thin films in combination with Ca and Al to obtain cathodes with low injection barriers. We have used electroabsorption measurements, as they allow the noninvasive determination of the built-in potential when changing the cathode. This provides precious experimental information on the alteration of the polymer/cathode interfacial energy level line-up. The latter is found to depend strongly on the electrode work function. Thus, the Schottky–Mott model for the energy level alignment is found to be a better first-order approximation than those models where strong pinning or large interface dipoles determine the alignment (e.g., Bardeen model), except for electrodes that extensively react with the polymer, and introduce deep gap states. In addition, we show results that validate the approximation of rigid tilting of polymer energy levels with bias (for biases for which no significant injection of carriers occurs). To investigate further the consequences of the electronic line-up on device operation, we complemented the electroabsorption measurements with characterization of the emissive and transport properties of the light-emitting diodes, and confirmed that the cathodic barrier lowering in CsF/Ca/Al and LiF/Ca/Al electrodes leads to the best improvements in electron injection. We found that luminance and overall current are greatly affected by the barrier-reducing cathodes, indicating a truly bipolar transport, with comparable electron and hole currents. We also found significant indications of CsF/Ca/Al cathodes strongly reacting with the polymer, which is suggestive of CsF dissociation and diffusion in the bulk of the polymer.
We report electroabsorption and electroluminescence investigations of polymer light-emitting diodes featuring a LiF/Ca/Al cathode, for efficient electron injection into the electroluminescent polymer layer. Our measurement of the built-in potential gives direct evidence of a sizeable reduction of the cathodic barrier height not only with respect to Ca, but also versus LiF/Al or CsF/Al bilayer cathodes, currently amongst the most efficient electron injectors for low electron affinity polymers. In blue-emitting (∼2.7 at peak) polyfluorene-based LEDs, with poly(ethylenedioxythiophene)/poly(styrene sulphonic acid) anodes and LiF/Ca/Al cathodes, we measure a built-in potential of 2.7 V, a luminance of ∼1600 cd/m2 (the highest among the devices studied here) at a driving voltage of 5 V, and efficiencies as high as ∼3 lm/W. We also find that the turn-on voltage essentially coincides with the built-in potential within the experimental error.
We report the characteristics of a series of polymer light-emitting diodes, fabricated with LiF/Al cathodes and differing only by the thickness of the LiF interlayer (0 nm⩽d⩽11 nm). Electroabsorption studies of the internal electrostatic potential give direct evidence of a sizable reduction of the cathodic barrier height brought about by the LiF films. These results also correlate with photoemission experiments [S. E. Shaheen, G. E. Jabbour, M. M. Morrell, Y. Kawabe, B. Kippelen, N. Peyghambarian, M. F. Nabor, R. Schlaf, E. A. Mash, and N. R. Armstrong, J. Appl. Phys. 84, 2324 (1998)] and with the electroluminescence performance of the diodes.
We have studied the fractional and integer quantum Hall effect in high mobility double layer 2D hole gas systems. The large hole effective mass inhibits tunneling, allowing us to investigate the regime in which the interlayer and intralayer interactions are comparable without significant interlayer tunneling
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