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We use a Monte Carlo model to predict the effect of composition, domain size, and energetic disorder upon the mobility of carriers in an organic donor-acceptor blend. These simulations show that, for the changes in local morphology expected within the thickness of a typical bulk heterojunction photovoltaic device, changes in mobility of more than an order of magnitude are expected. The impact of nonuniform mobility upon space-charge-limited diode and photovoltaic (PV) device performance is examined using a drift-diffusion model. The current passing through a space-charge-limited diode is shown to depend upon the position of the layers with differing mobility. Accurate modeling of the current in such devices can only be achieved using a drift-diffusion model incorporating nonuniform mobility. Inserting a 20 nm thick layer in which the mobility is less by one order of magnitude than in the rest of the 70 nm thick PV device reduced the device efficiency by more than 20%. Therefore it seems vital to exert a high degree of control over the morphology throughout the entire blend PV device, otherwise potential PV performance may be lost. [ABSTRACT FROM AUTHOR]

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]

The rapid degradation of organic photovoltaic (OPV) devices compared to conventional inorganic solar cells is one of the critical issues that have to be solved in order to make OPV a competitive commercial technology. The understanding of the fundamental mechanisms that reduce the power con- version efficiency (PCE) over time is beneficial for the design of new materials with enhanced stability. This paper focuses on bulk heterojunction organic solar cells based on thieno [3,4-b] thiophene-alt-benzodithiophene (PTB7) mixed with [6,6]-phenyl-C71-butyric acid methyl esther ([70]PCBM). In spite of being promising in terms of PCE, devices based on this blend are unstable and have a short lifetime. When exposed to light in inert atmosphere, the PCE drops by 15% in less than 1 h and by 35% in 8 h; this degradation is induced by the ultraviolet (UV) part of the spectrum. This paper analyzes the effect induced by UV light on the transport of charges in PTB7:[70]PCBM. Contrary to expectations, the electron transport shows evidence of trapping, while the transport of holes appears unaffected. Furthermore, it is proven that the loss of PCE is due to a reaction between PTB7 and [70]PCBM, while the intrinsic instability of the polymer plays a marginal role. [ABSTRACT FROM AUTHOR]

To determine the role of photon energy on charge generation in bulk heterojunction solar cells, the bias voltage dependence of photocurrent for excitation with photon energies below and above the optical band gap is investigated in two structurally related polymer solar cells. Charges generated in (poly[2,6-(4,4-bis(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b′′]dithiophene)-alt-4,7-(2,1,3-benzothia­diazole)] (C-PCPDTBT):[6,6]-phenyl-C61-butyric acid methyl ester (PCBM) solar cells via excitation of the low-energy charge transfer (CT) state, situated below the optical band gap, need more voltage to be extracted than charges generated with excitation above the optical band gap. This indicates a lower effective binding energy of the photogenerated electrons and holes when the excitation is above the optical band gap than when excitation is to the bottom of the CT state. In blends of PCBM with the silicon-analogue, poly[(4,4-bis(2-ethylhexyl)dithieno[3,2- b:2 ′,3 ′- d]silole)-2,6-diyl- alt-(2,1,3-benzothiadiazole)-4,7-diyl] (Si-PCPDTBT), there is no effect of the photon energy on the electric field dependence of the dissociation efficiency of the CT state. C-PCPDTBT and Si-PCPDTBT have very similar electronic properties, but their blends with PCBM differ in the nanoscale phase separation. The morphology is coarser and more crystalline in Si-PCPDTBT:PCBM blends. The results demonstrate that the nanomorphological properties of the bulk heterojunction are important for determining the effective binding energy in the generation of free charges at the heterojunction. [ABSTRACT FROM AUTHOR]

The origin of the enhanced performance of bulk heterojunction solar cells based on slowly dried films of poly(3-hexylthiophene) (P3HT) and [6,6]-phenyl C61-butyric acid methyl ester is investigated, combining charge transport measurements with numerical device simulations. Slow drying leads to a 33-fold enhancement of the hole mobility up to 5.0×10-7 m2 V-1 s-1 in the P3HT phase of the blend, thereby balancing the transport of electrons and holes in the blend. The resulting reduction of space-charge accumulation enables the use of thick films (∼300 nm), absorbing most of the incoming photons, without losses in the fill factor and short-circuit current of the device. [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]

We present model calculations to explore the potential of polymer/fullerene bulk heterojunction solar cells. As a starting point, devices based on poly(3-hexylthiophene) and 6,6-phenyl C61-butyric acid methyl ester (PCBM), reaching 3.5% efficiency, are modeled. Lowering the polymeric band gap will lead to a device efficiency exceeding 6%. Tuning the electronic levels of PCBM in such a way that less energy is lost in the electron transfer process enhances the efficiency to values in excess of 8%. Ultimately, with an optimized level tuning, band gap, and balanced mobilities polymeric solar cells can reach power conversion efficiencies approaching 11%. [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]

An increase in the workfunction of the metal top electrode leads to a reduction of the open-circuit voltage, short-circuit current, and power conversion efficiency of organic bulk-heterojunction solar cells. It has been demonstrated that the photocurrent obtained from an active layer comprised of a blend of poly(2-methoxy-5-(3′,7′-dimethyloctyloxy)-p-phenylene vinylene) (OC1C10-PPV) and [6,6]-phenyl C61-butyric acid methyl ester (PCBM), with lithium fluoride topped aluminum, silver, gold, or palladium electrodes, shows a universal behavior when scaled against the effective voltage across the device. Indeed, model calculations confirm that the dependence of the photocurrent on the effective voltage is responsible for the observed variation in performance of each different electrode. Consequently, for any given metal, only the device’s open-circuit voltage is required in order to be able to predict the remaining solar cell parameters. [ABSTRACT FROM AUTHOR]

The performance of organic bulk heterojunction solar cells is strongly dependent on the donor/acceptor morphology. Morphological parameters, such as the extent and the composition of donor- and acceptor-rich domains, influence both the charge generation and the charge transport throughout the active layer. This work focuses on a polymer:fullerene system based on a small bandgap diketopyrrolopyrrole–quinquethiophene alternating copolymer (PDPP5T) mixed with [6,6]-phenyl-C 71 -butyric acid methyl ester ([70]PCBM) that is capable of efficiencies higher than 6%. By changing the processing conditions, the morphology can be varied from a coarse separated morphology, with fullerene domains (blobs) embedded in a polymer-rich matrix, to a completely mixed layer. The charge carrier transport and the strength of the bimolecular recombination in PDPP5T:[70]PCBM blends with different morphologies and fullerene concentrations are experimentally characterized. The large difference in electron and hole mobility and the electric field dependency of the electron mobility are identified as the causes that limit the performance of devices with low [70]PCBM content. These effects are not present if the concentration of [70]PCBM is increased while keeping a fine phase separation by the addition of ortho -dichlorobenzene as a cosolvent. For the phase-separated blends, a model is proposed, based on a drift–diffusion approach that combines electrical and morphological parameters; with this model the contribution of each phase to the total current is quantified. Under operating conditions, most of the current comes from the interfacial region between the phases, with holes traveling through the matrix and the electrons through the blobs. This device model consistently connects morphological features to overall device performance. [ABSTRACT FROM AUTHOR]