Jonas Bergqvist

Structure–property relationships of oligothiophene–isoindigo polymers for efficient bulk-heterojunction solar cells

A series of alternating oligothiophene (nT)–isoindigo (I) copolymers (PnTI) were synthesized to investigate the influence of the oligothiophene block length on the photovoltaic (PV) properties of PnTI:PCBM bulk-heterojunction blends. Our study indicates that the number of thiophene rings (n) in the repeating unit alters both polymer crystallinity and polymer–fullerene interfacial energetics, which results in a decreasing open-circuit voltage (Voc) of the solar cells with increasing n. The short-circuit current density (Jsc) of P1TI:PCBM devices is limited by the absence of a significant driving force for electron transfer. Instead, blends based on P5TI and P6TI feature large polymer domains, which limit charge generation and thus Jsc. The best PV performance with a power conversion efficiency of up to 6.9% was achieved with devices based on P3TI, where a combination of a favorable morphology and an optimal interfacial energy level offset ensures efficient exciton separation and charge generation. The structure–property relationship demonstrated in this work would be a valuable guideline for the design of high performance polymers with small energy losses during the charge generation process, allowing for the fabrication of efficient solar cells that combine a minimal loss in Voc with a high Jsc.

A New Fullerene-Free Bulk-Heterojunction System for Efficient High-Voltage and High-Fill Factor Solution-Processed Organic Photovoltaics

Small molecule donor/polymer acceptor bulk-heterojunction films with both compounds strongly absorbing have great potential for further enhancement of the performance of organic solar cells. By employing a newly synthesized small molecule donor with a commercially available polymer acceptor in a solution-processed fullerene-free system, a high power conversion efficiency of close to 4% is reported.

A new tetracyclic lactam building block for thick, broad-bandgap photovoltaics.

A new tetracyclic lactam building block for polymer semiconductors is reported that was designed to combine the many favorable properties that larger fused and/or amide-containing building blocks can induce, including improved solid-state packing, high charge carrier mobility, and improved charge separation. Copolymerization with thiophene resulted in a semicrystalline conjugated polymer, PTNT, with a broad bandgap of 2.2 eV. Grazing incidence wide-angle X-ray scattering of PTNT thin films revealed a strong tendency for face-on π-stacking of the polymer backbone, which was retained in PTNT:fullerene blends. Corresponding solar cells featured a high open-circuit voltage of 0.9 V, a fill factor around 0.6, and a power conversion efficiency as high as 5% for >200 nm thick active layers, regardless of variations in blend stoichiometry and nanostructure. Moreover, efficiencies of >4% could be retained when thick active layers of ∼400 nm were employed. Overall, these values are the highest reported for a conjugated polymer with such a broad bandgap and are unprecedented in materials for tandem and particularly ternary blend photovoltaics. Hence, the newly developed tetracyclic lactam unit has significant potential as a conjugated building block in future organic electronic materials.

Fullerene mixtures enhance the thermal stability of a non-crystalline polymer solar cell blend

Printing of polymer:fullerene solar cells at high speed requires annealing at temperatures up to 140 C. However, bulk-heterojunction blends that comprise a non-crystalline donor polymer often suffer from insufficient thermal stability and hence rapidly coarsen upon annealing above the glass transition temperature of the blend. In addition, micrometer-sized fullerene crystals grow, which are detrimental for the solar cell performance. In this manuscript, we present a strategy to limit fullerene crystallization, which is based on the use of fullerene mixtures of the two most common derivatives, PC61BM and PC71BM, as the acceptor material. Blends of this fullerene mixture and a non-crystalline thiophene-quinoxaline copolymer display considerably enhanced thermal stability and largely retain their photovoltaic performance upon annealing at elevated temperatures as high as 170 C.

Inverted all-polymer solar cells based on a quinoxaline–thiophene/naphthalene-diimide polymer blend improved by annealing

We have investigated the effect of thermal annealing on the photovoltaic parameters of all-polymer solar cells based on a quinoxaline-thiophene donor polymer (TQ1) and a naphthalene diimide acceptor polymer (N2200). The annealed devices show a doubled power conversion efficiency compared to nonannealed devices, due to the higher short-circuit current (J(sc)) and fill factor (FF), but with a lower open circuit voltage (V-oc). On the basis of the morphology-mobility examination by several scanning force microscopy techniques, and by grazing-incidence wide-angle X-ray scattering, we conclude that better charge transport is achieved by higher order and better interconnected networks of the bulk heterojunction in the annealed active layers. The annealing improves charge transport and extends the conjugation length of the polymers, which do help in charge generation and meanwhile reduce recombination. Photoluminescence, electroluminescence, and light intensity dependence measurements reveal how this morphological change affects charge generation and recombination. As a result, the J(sc) and FF are significantly improved. However, the smaller band gap and the higher HOMO level of TQ1 upon annealing causes a lower V-oc. The blend of an amorphous polymer TQ1, and a semi-crystalline polymer N2200, can thus be modified by thermal annealing to double the power conversion efficiency.

Sub-glass transition annealing enhances polymer solar cell performance

Thermal annealing of non-crystalline polymer:fullerene blends typically results in a drastic decrease in solar cell performance. In particular aggressive annealing above the glass transition temperature results in a detrimental coarsening of the blend nanostructure. We demonstrate that mild annealing below the glass transition temperature is a viable avenue to control the nanostructure of a non-crystalline thiophene–quinoxaline copolymer:fullerene blend. Direct imaging methods indicate that coarsening of the blend nanostructure can be avoided. However, a combination of absorption and luminescence spectroscopy reveals that local changes in the polymer conformation as well as limited fullerene aggregation are permitted to occur. As a result, we are able to optimise the solar cell performance evenly across different positions of the coated area, which is a necessary criterion for large-scale, high throughput production.

Intermodulation electrostatic force microscopy for imaging surface photo-voltage

We demonstrate an alternative to Kelvin Probe Force Microscopy for imaging surface potential. The open-loop, single-pass technique applies a low-frequency AC voltage to the atomic force microscopy tip while driving the cantilever near its resonance frequency. Frequency mixing due to the nonlinear capacitance gives intermodulation products of the two drive frequencies near the cantilever resonance, where they are measured with high signal to noise ratio. Analysis of this intermodulation response allows for quantitative reconstruction of the contact potential difference. We derive the theory of the method, validate it with numerical simulation and a control experiment, and we demonstrate its utility for fast imaging of the surface photo-voltage on an organic photo-voltaic material.

Asymmetric photocurrent extraction in semitransparent laminated flexible organic solar cells

Scalable production methods and low-cost materials with low embodied energy are key to success for organic solar cells. PEDOT(PSS) electrodes meet these criteria and allow for low-cost and all solution-processed solar cells. However, such devices are prone to shunting. In this work we introduce a roll-to-roll lamination method to construct semitransparent solar cells with a PEDOT(PSS) anode and an polyethyleneimine (PEI) modified PEDOT(PSS) cathode. We use the polymer:PCBM active layer coated on the electrodes as the lamination adhesive. Our lamination method efficiently eliminates any shunting. Extended exposure to ambient degrades the laminated devices, which manifests in a significantly reduced photocurrent extraction when the device is illuminated through the anode, despite the fact that the PEDOT(PSS) electrodes are optically equivalent. We show that degradation-induced electron traps lead to increased trap-assisted recombination at the anode side of the device. By limiting the exposure time to ambient during production, degradation is significantly reduced. We show that lamination using the active layer as the adhesive can result in device performance equal to that of conventional sequential coating.Printing solar cell: yield enhanced by laminating the active layerThe manufacturing yield of the flexible organic solar cells is enhanced with a new lamination method by solving the shunting problem due to conductive inks. A collaborative team led by Olle Inganäs from Linköping University, Sweden fabricates polymer: PCBM all-organic solar cells in ambient conditions using the active layer as the lamination adhesive. The team shows that reduced exposure to ambient is critical to achieve high device efficiency and suppress degradation. The degraded devices generate asymmetric photocurrent due to the electron traps in the active layer. The reported active layer lamination method not only solves the shunting problem in a number of different polymer: PCBM combinations, but also provides wide tenability and control of the composition and vertical phase separation of the active layer.

Correction to "a new tetracyclic lactam building block for thick, broad-bandgap photovoltaics".

Page 11579. Further analysis of the spectroscopic data of the NT monomer suggested that the majority product is the Oalkylated instead of N-alkylated product. The amide functionality displays ambident reactivity, and the ratio of Nor Oalkylation is governed by factors such as the employed halide on the alkyl reactant and the thermodynamic stability of the final product. For amide-containing structures employed in conjugated polymers, the N-alkylated product is usually the majority product. However, recently He et al. reported a new conjugated building block that favored O-alkylation over Nalkylation under reaction conditions similar to those we employed. To unambiguously determine which isomer was formed, we synthesized a crystalline C8-NT unit under conditions similar to those used for the initial 2-hexyldecyl-substituted NT unit. Analysis by single-crystal X-ray diffraction and comparison of the other spectroscopic data confirmed that the majority product after alkylation is O-alkylated. The correct structures of the NT unit and PTNT are depicted in Figure 1.

Fully-solution-processed organic solar cells with a highly efficient paper-based light trapping element

We demonstrate the use of low cost paper as an efficient light-trapping element for thin film photovoltaics. We verify its use in fully-solution processed organic photovoltaic devices with the highest power conversion efficiency and the lowest internal electrical losses reported so far, the architecture of which – unlike most of the studied geometries to date – is suitable for upscaling, i.e. commercialization. The use of the paper-reflector enhances the external quantum efficiency (EQE) of the organic photovoltaic device by a factor of ≈1.5–2.5 over the solar spectrum, which rivals the light harvesting efficiency of a highly-reflective but also considerably more expensive silver mirror back-reflector. Moreover, by detailed theoretical and experimental analysis, we show that further improvements in the photovoltaic performance of organic solar cells employing PEDOT:PSS as both electrodes rely on the future development of high-conductivity and high-transmittance PEDOT:PSS. This is due optical losses in the PEDOT:PSS electrodes.