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Organic Light-Emitting Transistors with Efficiency Out-performing the Equivalent LightEmitting Diodes by R. Capelli et al. SUPPLEMENTARY INFORMATION The Supplementary Information is composed of 6 figures with their captions and reports the quantitative determination of the optical properties of the tri-layer OLET. The figures show the electrical and morphological characteristics of the materials used as charge transport layers in the heterostructure OLETs, a sketch of the interdigitated top-contact source and drain configuration, the optical transmission spectrum of the tri-layer OLET, and the structure and external quantum efficiency of the tri-layer OLET with reduced channel length.

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Figure S1 Output electrical characteristics of single-layer field-effect transistors. a) OFET based on DH-4T and (b) OFET based on DFH-4T.

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a b

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10 m

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Figure S2 Topographical images of the n-type and p-type charge transporting layers grown on PMMA dielectric. Confocal laser scanning microscopy images (excitation wavelength 488 nm) of the active region of DH-4T (a) and DFH-4T (b) single-layer OFET devices.

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Figure S3 Device structure and electrical characteristics of the bi-layer OFET. a) Scheme of the OFET device based on a DFH-4T/DH-4T bi-layer structure. b) Output electrical characteristics measured by operating the device in p-type mode. c) Forward and backward transfer electrical characteristics measured in saturation regime (VDS = 90 V).

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doi: 10.1038/nmat2751

Figure S4 Sketch of the interdigitated source and drain structure used for the realization of the tri-layer OLET. Channel length and channel width are 150 m and 20 cm, respectively.

Quantitative analysis of the optical properties of the tri-layer OLET To quantitatively analyze the optical properties of the tri-layer OLET, we consider the following. 1. 2. 3. 4. In the perfectly ambipolar regime the number of injected electrons equals that of injected holes and all charges recombine, therefore Ids = Ie = Ih. The exciton formation rate for singlet states is 25%. The experimentally determined PL quantum yield (QY) of the Alq3:DCM layer is 74% [1]. The theoretical value of EQE for an optimized OLED based on Alq3:DCM is 3.7%, considering that exciton quenching is fully avoided and an outcoupling efficiency of 20% in an OLED with 100 nm thick ITO and Al electrodes [1]. 5. The EQE of the tri-layer OLET in the ambipolar regime is 5%.

The EQE (ext) of the OLET device can be expressed as: ext = PL out Where is the ratio of injected electrons to injected holes, PL is the photoluminescence quantum yield, is the fraction of singlet excitons formed, out is the light outcoupling efficiency.

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doi: 10.1038/nmat2751

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Given that = 1; PL = 74%; = 25% are fixed values, an EQE ext = 5% implies a light outcoupling efficiency out = 27%. The light outcoupling efficiency of the OLET is therefore improved by 30% with respect to that of the typical OLED structure (20%). In order to quantify the effect of the exciton-charge quenching on the EQE of the OLETs in case of overlap between the charge accumulation layer and exciton formation zone, the case of the single layer ambipolar OLET is considered. J. Zaumseil et al.[2] derived experimentally for an ambipolar single layer OLET with a device structure similar to the one reported here, but with a 15nm thick Au layer in place of the 100nm ITO, an EQE = 0,75%. In that case PL = 54% and = 25%. The outcoupling efficiency of the single layer OLET can be calculated by comparing the relative transmittance of the stack (gate electrode, dielectric layer, organic layer, glass substrate) with that of the tri-layer OLET. At the respective emission wavelength the transmission of the single layer OLET is 50%, [2] while that of the tri-layer is 84,4% (see Fig. S 5).

Figure S5 Optical transmission spectrum of the tri-layer OLET device. The red dot indicates the transmission of the complete of the stack (gate electrode, dielectric layer, organic layer, glass substrate) at the emission wavelength. This means that if the outcoupling efficiency of the tri-layer OLET is 27%, that of the single layer OLET is 16%.
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For the single layer OLET ext = PL out ext = 1 x 0,54 x 0,25 x 0,16 = 2,16%

doi: 10.1038/nmat2751

This value is to be compared with the experimentally derived EQE value, that is 0,75%. The difference between the expected EQE value in case of no exciton quenching (2,16%) and the experimentally derived EQE value (0,75%) gives the quantitative determination of the excitoncharge quenching in a single layer ambipolar OLET. The exciton-charge quenching decreases the EQE by a factor of 2,9. The value of the exciton-charge quenching calculated as = ( ext - EQEExperimental)/ ext is 65% Even though the EQE measurements reported in [2] were affected by the collection geometry, the exciton-charge quenching remains very high and cannot be compensated by the outcoupling efficiency. Any sizable exciton quenching in the tri-layer OLET, would result in an outcoupling efficiency much higher than 30%, which is unlikely because of the losses at the PMMA/ITO structure. Indeed it is known that values of the outcoupling efficiency exceeding 30% are possible only using an ultra-thin layer of ITO and/or a high refractive index glass substrate [3, 4]. An outcoupling efficiency of 27% in the tri-layer structure where the losses at the metal electrode have been removed is a realistic figure. Therefore, in the tri-layer OLET there is no sizable excitoncharge quenching. External quantum efficiency of tri-layer OLETs with reduced channel length In order to verify that a reduction in channel length has no major deleterious effect on light emission efficiency, a tri-layer OLET with channel length of 50 microns was fabricated maintaining all other features of the device structure unchanged.
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Figure S6 Tri-layer OLET with 50 m channel length. a) Structure of the tri-layer OLET device with reduced channel length. b) Transfer characteristic and External Quantum Efficiency as a function of VGS. A thorough optimization of the device structure with reduced channel length would require the use of a gate dielectric with increased capacitance, which is outside the scope of this work. References 1. Matsushima, T., Adachi, C. Extremely low voltage light-emitting diodes with p-doped alphasexithiophene hole transport and n-doped phenyldipyrenylphosphine oxide electron transport layers. Appl. Phys. Lett. 89, 253506 (2006). 2. Zaumseil, J. et al. Quantum efficiency of ambipolar light-emitting polymer field-effect transistors. J. Appl. Phys. 103, 064517 (2008). 3. Lu, M. H., Sturm, J. C. Optimization of external coupling and light emission in organic lightemitting devices: modelling and experiment J. Appl. Phys. 91, 595-604 (2002). 4. Reineke, S. et al. White organic light-emitting diodes with fluorescent tube efficiency Nature 459, 234-239 (2009)

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