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The morphology of the active layer in polymer:fullerene solar cells is a key parameter for the performance. We compare bilayer poly(3-hexylthiophene)/[6,6]-phenyl-C(61)-butyric acid methyl ester (P3HT/PCBM) solar cell devices produced from orthogonal solvents before and after thermal annealing with P3HT:PCBM bulk heterojunction solar cells produced from a single solvent. By comparing the spectral shape and magnitude of the experimental and theoretically modeled EQEs we show that P3HT/PCBM bilayers made via orthogonal solution processing do not lead to bilayers with a sharp interface but that partial intermixing has occurred. Thermal annealing of these diffusive P3HT/PCBM bilayers leads to increased mixing but does not result in the same mixed bulk heterojunction morphology that is obtained when P3HT and PCBM are cast simultaneously from single solution. For thicker layers, the annealed bilayers significantly outperform the bulk heterojunction devices with the same nominal composition and same total thickness.

Charge transport properties are investigated of blends of poly [2-methoxy-5-(3′, 7′-dimethyloctyloxy)-1,4-phenylene vinylene] (MDMO-PPV) and poly-[oxa-1,4-phenylene-(1-cyano-1,2-vinylene)-(2-methoxy-5-(3′, 7′-dimethyloctyloxy)-1,4-phenylene)-1,2-(2-cyanovinylene)-1,4-phenylene] (PCNEPV). The hole transport in the MDMO-PPV donor phase of the 1:1 weight ratio blend is trap-free space-charge limited, with a mobility identical to the pristine polymer. The electron current in the PCNEPV acceptor phase is strongly reduced by traps that are exponentially distributed in energy. The current in MDMO-PPV:PCNEPV bulk heterojunction solar cells is therefore unbalanced and dominated by the holes in the MDMO-PPV phase. [ABSTRACT FROM AUTHOR]

We determine and analyze the photocurrent Jph in polymer solar cells under conditions where, no, one, or two different charge carriers can be injected by choosing appropriate electrodes and compare the experimental results to simulations based on a drift-diffusion device model that accounts for photogeneration and Langevin recombination of electrons and holes. We demonstrate that accounting for the series resistance of the device is essential to determine Jph. Without such correction, the results are, even qualitatively, incorrect. We show that in solar cells with forward bias applied 7ph is reduced by recombination of photogenerated charge carriers with injected charge carriers. Self-selective contacts or band bending are not necessary to explain the effects. Without injecting contacts Jpb is symmetric around the compensation voltage. A simple analytical model shows that under high forward bias Jpt, scales inversely with 1 + ξγpre, in which γpre represents the extent of Langevin recombination and ξ is a positive constant. Under conditions where Langevin recombination is very low or when electron and hole mobility are a very different, photogenerated charge carriers can affect the space-charge field and modify the injection of charge carriers. We show by simulations and experimentally that under such conditions the photocurrent can exceed that charge generation such that, effectively, photocurrent multiplication occurs. [ABSTRACT FROM AUTHOR]

The efficiency of polymer solar cells critically depends on the intimacy of mixing of the donor and acceptor semiconductors used in these devices to create charges and on the presence of unhindered percolation pathways in the individual components to transport holes and electrons. The visualization of these bulk heterojunction morphologies in three dimensions has been challenging and has hampered progress in this area. Here, we spatially resolve the morphology of 2%-efficient hybrid solar cells consisting of poly(3-hexylthiophene) as the donor and ZnO as the acceptor in the nanometre range by electron tomography. The morphology is statistically analysed for spherical contact distance and percolation pathways. Together with solving the three-dimensional exciton-diffusion equation, a consistent and quantitative correlation between solar-cell performance, photophysical data and the three-dimensional morphology has been obtained for devices with different layer thicknesses that enables differentiating between generation and transport as limiting factors to performance. [ABSTRACT FROM AUTHOR]

We study the thickness dependence of the performance of bulk heterojunction solar cells based on poly[2-methoxy-5-(3′,7′-dimethyloctyloxy)-1,4-phenylenevinylene] as electron donor and [6,6]-phenyl C61 butyric acid methyl ester as electron acceptor. Typically, these devices have an active layer thickness of 100 nm at which only 60% of the incoming light is absorbed. Increasing device thickness results in a lower overall power conversion efficiency, mainly due to a lowering of the fill factor. We demonstrate that the decrease in fill factor and hence device efficiency is due to a combination of charge recombination and space-charge effects. [ABSTRACT FROM AUTHOR]

Bimolecular recombination in organic semiconductors is known to follow the Langevin expression, i.e., the rate of recombination depends on the sum of the mobilities of both carriers. We show that this does not hold for polymer/fullerene bulk heterojunction solar cells. The voltage dependence of the photocurrent reveals that the recombination rate in these blends is determined by the slowest charge carrier only, as a consequence of the confinement of both types of carriers to two different phases. [ABSTRACT FROM AUTHOR]

A typical feature of polymer/fullerene based solar cells is that the current density under short-circuit conditions (Jsc) does not scale exactly linearly with light intensity (I). Instead, a power law relationship is found given by Jsc∝Iα, where α ranges from 0.85 to 1. In a number of reports this deviation from unity is speculated to arise from the occurrence of bimolecular recombination. We demonstrate that the dependence of the photocurrent in bulk heterojunction solar cells is governed by the build-up of space-charge in the device as a consequence of a difference in electron- and hole mobility. We have verified this for an experimental model system in which the mobility difference can be tuned from one to three orders of magnitude by changing the annealing treatment. [ABSTRACT FROM AUTHOR]

Polymer solar cells have a promising future for applications in our day to day usage of energy in small appliances and portable devices. However, their performance in terms of efficiency is limited by a number of factors, among which is their low open circuit voltage (Voc). It is, therefore, understandable that much effort is channeled by the scientific community in improving the Voc. One way to achieve this goal is the development of novel materials, for example, polymers, through chemical structure modification. Typical examples are addition (chlorination, fluorination, or sulfonylation) and/or reduction (from alkyl‐ester to ketone substituents) mechanisms. This paper reports on the study of the effect of these structural changes for Voc enhancement on the performance of the polymers in polymer:fullerene solar cells. In particular, it looks at seven polymers of the polybenzodithiophene‐thienothiophene family, identifying the structural changes in the thienothiophene units or their moieties as a function of Voc behavior in relation to their UV‐stability. The findings reveal that the fluorination of the TT‐units or having alkyl‐ester groups as substituents on the TT‐units is bad for photostability. However, when these alkyl‐ester groups are reduced into ketone substituents, the photostability behavior improves. The reduction and/or the fluorination of the TT‐units of the PBDTT‐TT polymers have crucial effects on the photostability of their polymer:fullerene solar cells. Reduction improves the photostability of the solar cells while fluorination destabilizes the photostability. [ABSTRACT FROM AUTHOR]