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Abstract:

Simultaneous control over both the energy levels and Fermi level, a key breakthrough for inorganic electronics, has yet to be shown for organic semiconductors. Here, energy level tuning and molecular doping are combined to demonstrate controlled shifts in ionisation potential and Fermi level of an organic thin film. This is achieved by p-doping a blend of two host molecules, zinc phthalocyanine and its eight-times fluorinated derivative, with tunable energy levels based on mixing ratio. The doping efficiency is found to depend on host mixing ratio, which is explained using a statistical model that includes both shifts of the host's ionisation potentials and, importantly, the electron affinity of the dopant. Therefore, the energy level tuning effect has a crucial impact on the molecular doping process. The practice of comparing host and dopant energy levels must consider the long-range electrostatic shifts to consistently explain the doping mechanism in organic semiconductors.

Abstract:

Carbon nanotube (CNT) solubilization via non-covalent wrapping of conjugated semiconducting polymers is a common technique used to produce stable dispersions for depositing CNTs from solution. Here, we report the use of a non-conjugated insulating polymer, ethylene vinyl acetate (EVA), to disperse multi- and single-walled CNTs (MWCNT and SWCNT) in organic solvents. We demonstrate that despite the insulating nature of the EVA, we can produce semitransparent films with conductivities of up to 34 S/cm. We show, using photoluminescence spectroscopy, that the EVA strongly binds to individual CNTs, thus making them soluble, preventing aggregation, and facilitating the deposition of high-quality films. To prove the good electronic properties of this composite, we have fabricated perovskite solar cells using EVA/SWCNTs and EVA/MWCNTs as selective hole contact, obtaining power conversion efficiencies of up to 17.1%, demonstrating that the insulating polymer does not prevent the charge transfer from the active material to the CNTs.

Abstract:

Colloidal quantum dot (CQD)-based photovoltaics are an emerging low-cost solar cell technology with power conversion efficiencies exceeding 10%, i.e., high enough to be interesting for commercialization. Well-controlled and understood charge carrier transport through the device stack is required to make the next step in efficiency improvements. In this paper, polymer-wrapped single-walled carbon nanotube (SWNT) films embedded in an insulating poly(methyl methacrylate) (PMMA) matrix and capped by a thermally evaporated Au electrode are investigated as a composite hole transport layer and optical spacer. Employing transient absorption spectroscopy we show that the SWNTs enhance the charge transfer rate from CQD to CQD, ZnO, or SWNT. In order to pinpoint the underlying mechanism for the improvement, we investigate the energetics of the junction by measuring the relative alignment of the band edges, using Kelvin probe and cyclic voltammetry. Measuring the external quantum efficiency and absorption we find that the improvement is not mainly from electronic improvements but from enhanced absorption of the CQD absorber. We demonstrate experimentally and theoretically, by employing a transfer-matrix model, that the transparent PMMA matrix acts as an optical spacer, which leads to an enhanced absorption in the absorber layer. With these electronic and optical enhancements, the efficiency of the PbS CQD solar cells improved from 4.0% to 6.0%.