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In recent years, the efficiency of organic solar cells (OSCs) has increased to more than 13%, although different barriers are on the way for reaching higher efficiencies. One crucial barrier is the recombination of charge carriers, which can either occur as the bulk recombination of photogenerated charges or the recombination of photogenerated charges and electrodic induced charges (EICs). This work studies the impact of EICs on the recombination lifetime in OSCs. To this end, the net recombination lifetime of photogenerated charge carriers in the presence of EICs is measured by means of conventional and newly developed transient photovoltage techniques. Moreover, a new approach has been introduced to exclusively measure the bulk recombination lifetime, i.e., in the absence of EICs; this approach was conducted by depositing transparent insulating layers on both sides of the OSC active layer. An examination of these approaches on OSCs with different active layer materials, thicknesses, and varying light intensities determined that the EICs can only reduce the recombination lifetime of the photogenerated charges in OSCs with very weak recombination strength. This work supports that for OSCs with highly reduced recombination strength, eliminating the recombination of photogenerated charges and EICs is critical for achieving better performance. Therefore, the use of a proper blocking layer suppresses EIC recombination in systems with very weak recombination.

N-doping of conjugated polymers either requires a high dopant fraction or yields a low electrical conductivity because of their poor compatibility with molecular dopants. We explore n-doping of the polar naphthalenediimide-bithiophene copolymer p(gNDI-gT2) that carries oligoethylene glycol-based side chains and show that the polymer displays superior miscibility with the benzimidazole-dimethylbenzenamine-based n-dopant N-DMBI. The good compatibility of p(gNDI-gT2) and N-DMBI results in a relatively high doping efficiency of 13% for n-dopants, which leads to a high electrical conductivity of more than 10 -1 S cm -1 for a dopant concentration of only 10 mol % when measured in an inert atmosphere. We find that the doped polymer is able to maintain its electrical conductivity for about 20 min when exposed to air and recovers rapidly when returned to a nitrogen atmosphere. Overall, solution coprocessing of p(gNDI-gT2) and N-DMBI results in a larger thermoelectric power factor of up to 0.4 μW K -2 m -1 compared to other NDI-based polymers., Competing Interests: The authors declare no competing financial interest.

The parallel-plate capacitor equation is widely used in contemporary material research for nanoscale applications and nanoelectronics. To apply this equation, flat and smooth electrodes are assumed for a capacitor. This essential assumption is often violated for thin-film capacitors because the formation of nanoscale roughness at the electrode interface is very probable for thin films grown via common deposition methods. In this work, we experimentally and theoretically show that the electrical capacitance of thin-film capacitors with realistic interface roughness is significantly larger than the value predicted by the parallel-plate capacitor equation. The degree of the deviation depends on the strength of the roughness, which is described by three roughness parameters for a self-affine fractal surface. By applying an extended parallel-plate capacitor equation that includes the roughness parameters of the electrode, we are able to calculate the excess capacitance of the electrode with weak roughness. Moreover, we introduce the roughness parameter limits for which the simple parallel-plate capacitor equation is sufficiently accurate for capacitors with one rough electrode. Our results imply that the interface roughness beyond the proposed limits cannot be dismissed unless the independence of the capacitance from the interface roughness is experimentally demonstrated. The practical protocols suggested in our work for the reliable use of the parallel-plate capacitor equation can be applied as general guidelines in various fields of interest.

Trap-assisted recombination, despite being lower as compared with traditional inorganic solar cells, is still the dominant recombination mechanism in perovskite solar cells (PSCs) and limits their efficiency. We investigate the attributes of the primary trap-assisted recombination channels (grain boundaries and interfaces) and their correlation to defect ions in PSCs. We achieve this by using a validated device model to fit the simulations to the experimental data of efficient vacuum-deposited p-i-n and n-i-p CH 3 NH 3 PbI 3 solar cells, including the light intensity dependence of the open-circuit voltage and fill factor. We find that, despite the presence of traps at interfaces and grain boundaries (GBs), their neutral (when filled with photogenerated charges) disposition along with the long-lived nature of holes leads to the high performance of PSCs. The sign of the traps (when filled) is of little importance in efficient solar cells with compact morphologies (fused GBs, low trap density). On the other hand, solar cells with noncompact morphologies (open GBs, high trap density) are sensitive to the sign of the traps and hence to the cell preparation methods. Even in the presence of traps at GBs, trap-assisted recombination at interfaces (between the transport layers and the perovskite) is the dominant loss mechanism. We find a direct correlation between the density of traps, the density of mobile ionic defects, and the degree of hysteresis observed in the current-voltage ( J - V ) characteristics. The presence of defect states or mobile ions not only limits the device performance but also plays a role in the J - V hysteresis.

One of the most commonly used cathode interlayers for increasing the efficiency of electron injection/extraction in organic electronic devices is an ultrathin layer of LiF. Our capacitance measurements and electrical conductivity analysis show that thin films of fullerene derivatives and their mixtures with polymers are unintentionally doped upon deposition of LiF. The level of doping depends on the chemical structure of the fullerene derivatives. The doping effect on polymer/fullerene mixtures is significant only for blends in which the fullerene content is greater than the polymer content by weight. Our finding has profound implications for the development and characterization of organic photovoltaic devices, including a negative impact of doping on the stability of the device and erroneous estimations of properties such as charge carrier mobility and the dielectric constant.

We show that charge recombination in ordered heterojunctions depends sensitively on the degree of coherent delocalization of charges at the donor-acceptor interface. Depending on the relative sign of the electron and hole transfer integrals, such delocalization can dramatically suppress recombination through destructive quantum interference. This could explain why measured recombination rates are significantly lower than predictions based on Langevin theory for a variety of organic bulk heterojunctions. Moreover, it opens up a design strategy for photovoltaic devices with enhanced efficiencies through coherently suppressed charge recombination.

Dielectric interfaces are important in organic electronic devices, as they dominate charge generation and recombination dynamics and set the tone for efficiency of the device. In a charge separation scenario across the interface, we calculate the binding energy of a charge carrier for variations in dielectric mismatch (i.e., the ratio of the dielectric constant of materials forming the interface), interface shape and size, and dielectric anisotropy. We find that dielectric mismatch results in binding of the charge carrier to the interface with energies on the order of several kT. For the variation in interface shape and size, epitomized by the device morphology, we show that the assumption of a planar interface overestimates the attractive potential. The change in the interface curvature affects the binding energy of the charge carrier by order of kT. Anisotropy is shown to affect critically the electric field along the principal axis, while the binding energy of the charge is altered by more than 5 kT. We are able to give an upper limit on the change in the binding energy for the variations in the above interfacial factors. These limits can serve as guidelines for optimization, interface engineering, and design of high efficiency organic electronic devices.

Hybrid phototransistors of graphene and the organic semiconductor poly(3-hexylthiophene-2,5-diyl) (P3HT) are presented. Two types of phototransistors are demonstrated with a charge carrier transit time that differs by more than 6 orders of magnitude. High transit time devices are fabricated using a photoresist-free recipe to create large-area graphene transistors made out of graphene grown by chemical vapor deposition. Low transit time devices are fabricated out of mechanically exfoliated graphene on top of mechanically exfoliated hexagonal boron nitride using standard e-beam lithography. Responsivities exceeding 10(5) A/W are obtained for the low transit time devices.

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.