Moritz Riede

Abstract:

Electronic doping of organic semiconductors is essential for their usage in highly efficient optoelectronic devices. Although molecular and metal complex-based dopants have already enabled significant progress of devices based on organic semiconductors, there remains a need for clean, efficient and low-cost dopants if a widespread transition towards larger-area organic electronic devices is to occur. Here we report dimethyl sulfoxide adducts as p-dopants that fulfil these conditions for a range of organic semiconductors. These adduct-based dopants are compatible with both solution and vapour-phase processing. We explore the doping mechanism and use the knowledge we gain to 'decouple' the dopants from the choice of counterion. We demonstrate that asymmetric p-doping is possible using solution processing routes, and demonstrate its use in metal halide perovskite solar cells, organic thin-film transistors and organic light-emitting diodes, which showcases the versatility of this doping approach.

Abstract:

Organic solar cells (OSCs), also known as organic photovoltaics (OPVs), are an emerging solar cell technology composed of carbon-based, organic molecules, which convert energy from the sun into electricity. Key for their performance is the microstructure of the light-absorbing organic bulk heterojunction. To study this, organic solar films composed of both fullerene C60 as electron acceptor and different mole percentages of di-[4-(N,N-di-p-tolyl-amino)-phenyl]-cyclohexane (TAPC) as electron donor were evaporated in vacuum in different mixing ratios (5, 50 and 95 mol%) on an ITO-coated glass substrate held at room temperature and at 110 °C. The microstructure of the C60: TAPC heterojunction was studied by grazing incidence wide angle X-ray scattering to understand the effect of substrate heating. By increasing the substrate temperature from ambient to 110 °C, it was found that no significant change was observed in the crystal size for the C60: TAPC concentrations investigated in this study. In addition to the variation done in the substrate temperature, the variation of the mole percent of the donor (TAPC) was studied to conclude the effect of both the substrate temperature and the donor concentration on the microstructure of the OSC films. Bragg peaks were attributed to C60 in the pure C60 sample and in the blend with low donor mole percentage (5%), but the C60 peaks became nondiscernible when the donor mole percentage was increased to 50% and above, showing that TAPC interrupted the formation of C60 crystals.

Abstract:

<p>We use the electron spin as a probe to gain insight into the mechanism of molecular doping in a p-doped zinc phthalocyanine host across a broad range of temperatures (80–280 K) and doping concentrations (0–5 wt% of F6-TCNNQ).</p>

Abstract:

Stability is now a critical factor in the commercialization of organic photovoltaic (OPV) devices. Both extrinsic stability to oxygen and water and intrinsic stability to light and heat in inert conditions must be achieved. Triplet states are known to be problematic in both cases, leading to singlet oxygen production or fullerene dimerization. The latter is thought to proceed from unquenched singlet excitons that have undergone intersystem crossing (ISC). Instead, we show that in bulk heterojunction (BHJ) solar cells the photo-degradation of C₆₀ via photo-oligomerization occurs primarily via back-hole transfer (BHT) from a charge-transfer state to a C₆₀ excited triplet state. We demonstrate this to be the principal pathway from a combination of steady-state optoelectronic measurements, time-resolved electron paramagnetic resonance, and temperature-dependent transient absorption spectroscopy on model systems. BHT is a much more serious concern than ISC because it cannot be mitigated by improved exciton quenching, obtained for example by a finer BHJ morphology. As BHT is not specific to fullerenes, our results suggest that the role of electron and hole back transfer in the degradation of BHJs should also be carefully considered when designing stable OPV devices.