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Here we show that the charge transfer (CT) absorption signal in bulk-heterojunction solar cell blends, measured by photothermal deflection spectroscopy, is directly proportional to the density of molecular donor:acceptor interfaces. Since the optical transitions from the ground state to the interfacial CT state are weakly allowed at photon energies below the optical gap of both the donor and acceptor, we can exploit the use of this sensitive linear absorption spectroscopy for such quantification. Moreover, we determine the absolute molar extinction coefficient of the CT transition for an archetypical polymer:fullerene interface. The latter is â¼100 times lower than the extinction coefficient of the donor chromophore involved, allowing us to experimentally estimate the transition dipole moment as 0.3 D and the electronic coupling between the ground and CT states to be on the order of 30 meV.
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Broad spectral coverage over the solar spectrum is necessary for photovoltaic technologies and is a focus for organic solar cells. We report a series of small-molecule, nonfullerene electron acceptors containing the [(benzo[c][1,2,5]thiadiazol-4-yl)methylene]malononitrile unit as a high electron affinity component. The optoelectronic properties of these molecules were fine-tuned with the objective of attaining strong absorption at longer wavelengths by changing the low-ionization-potential moiety. The electron-accepting function of these materials was investigated with poly(3-n-hexylthiophene) (P3HT) as a standard electron donor. Significant photocurrent generation in the near infrared region, with an external quantum yield reaching as high as 22 % at 700 nm and an onset >800 nm was achieved. The results support efficient hole transfer to P3HT taking place after light absorption by the acceptor molecules. A Channel II-dominated power conversion efficiency of up to 1.5 % was, thus, achieved.
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A facile ligand exchange method for dispersing Cu2ZnSnS4 (CZTS) nanocrystals (NCs) in environmentally benign polar solvents, such as ethanol or n-propanol, at high concentrations (up to 200 mg/mL) is demonstrated. This approach has been applied to CZTS nanocrystals synthesized via scalable, noninjection methods to formulate colloidally stable inks that are suitable for the solution processing of solar cell devices. Unlike other inks currently used to fabricate NC solar cells, the CZTS nanocrystal ink developed here circumvents the need for hydrazine, pyridine, or thiol coordinating solvents. By combining our polar CZTS inks with optimized selenization procedures, substrate CZTSSe solar cells have been successfully fabricated with device efficiencies of 7.7%.
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Extensive efforts have been made to develop novel conjugated polymers that give improved performance in organic photovoltaic devices. The use of polymers based on alternating electron-donating and electron-accepting units not only allows the frontier molecular orbitals to be tuned to maximize the open-circuit voltage of the devices but also controls the optical band gap to increase the number of photons absorbed and thus modifies the other critical device parameter-the short circuit current. In fact, varying the nonchromophoric components of a polymer is often secondary to the efforts to adjust the intermolecular aggregates and improve the charge-carrier mobility. Here, we introduce an approach to polymer synthesis that facilitates simultaneous control over both the structural and electronic properties of the polymers. Through the use of a tailored multicomponent acceptor-donor-acceptor (A-D-A) intermediate, polymers with the unique structure A-D1-A-D2 can be prepared. This approach enables variations in the donor fragment substituents such that control over both the polymer regiochemistry and solubility is possible. This control results in improved intermolecular π-stacking interactions and therefore enhanced charge-carrier mobility. Solar cells using the A-D1-A-D2 structural polymer show short-circuit current densities that are twice that of the simple, random analogue while still maintaining an identical open-circuit voltage. The key finding of this work is that polymers with an A-D1-A-D2 structure offer significant performance benefits over both regioregular and random A-D polymers. The chemical synthesis approach that enables the preparation of A-D1-A-D2 polymers therefore represents a promising new route to materials for high-efficiency organic photovoltaic devices.
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Solar cells made by high temperature and vacuum processes from inorganic semiconductors are at a perceived cost disadvantage when compared with solution-processed systems such as organic and dye-sensitized solar cells. We demonstrate that totally solution processable solar cells can be fabricated from inorganic nanocrystal inks in air at temperature as low as 300 °C. Focusing on a CdTe/ZnO thin-film system, we report solar cells that achieve power conversion efficiencies of 6.9% with greater than 90% internal quantum efficiency. In our approach, nanocrystals are deposited from solution in a layer-by-layer process. Chemical and thermal treatments between layers induce large scale grain formation, turning the 4 nm CdTe particles into pinhole-free films with an optimized average crystallite size of â¼70 nm. Through capacitance-voltage measurements we demonstrate that the CdTe layer is fully depleted which enables the charge carrier collection to be maximized.
Asunto(s)
Compuestos de Cadmio/química , Suministros de Energía Eléctrica , Nanoestructuras/química , Energía Solar , Telurio/química , Óxido de Zinc/química , Membranas Artificiales , Nanotecnología , Tamaño de la Partícula , Semiconductores , Soluciones , Propiedades de Superficie , Temperatura , VacioRESUMEN
We report the synthesis and polymerization of a novel thieno[3,2-b]thiophene-diketopyrrolopyrrole-based monomer. Copolymerization with thiophene afforded a polymer with a maximum hole mobility of 1.95 cm(2) V(-1) s(-1), which is the highest mobility from a polymer-based OFET reported to date. Bulk-heterojunction solar cells comprising this polymer and PC(71)BM gave a power conversion efficiency of 5.4%.
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High-performance, solution-processed transistors fabricated from semiconducting polymers containing indacenodithiohene repeat units are described. The bridging functions on the backbone contribute to suppressing large-scale crystallization in thin films. However, charge carrier mobilities of up to 1 cm(2)/(V s) for a benzothiadiazole copolymer were reported and, coupled with both ambient stability and long-wavelength absorption, make this family of polymers particularly attractive for application in next-generation organic optoelectronics.
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Polímeros/química , Tiofenos/química , Transistores Electrónicos , Aire , Estructura Molecular , SemiconductoresRESUMEN
The electrical performance of organic semiconducting polymers in field-effect transistor devices is now sufficient for initial low complexity circuit applications. To achieve high performance, either operation in an inert atmosphere or a hydrophobic surface treatment and annealing step is typically required. In this communication we report a strategy to prepare fully air stable, amorphous semiconducting polymers which can achieve charge carrier mobilities in the range of 0.04 cm(2)/(V s), remaining over a period of over 3 months in ambient conditions.
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We report a spray deposition technique as a screening tool for solution processed solar cells. A dual-feed spray nozzle is introduced to deposit donor and acceptor materials separately and to form blended films on substrates in situ. Using a differential pump system with a motorised spray nozzle, the effect of film thickness, solution flow rates and the blend ratio of donor and acceptor materials on device performance can be found in a single experiment. Using this method, polymer solar cells based on poly(3-hexylthiophene) (P3HT):(6,6)-phenyl C61 butyric acid methyl ester (PC61BM) are fabricated with numerous combinations of thicknesses and blend ratios. Results obtained from this technique show that the optimum ratio of materials is consistent with previously reported values confirming this technique is a very useful and effective screening method. This high throughput screening method is also used in a single-feed configuration. In the single-feed mode, methylammonium iodide solution is deposited on lead iodide films to create a photoactive layer of perovskite solar cells. Devices featuring a perovskite layer fabricated by this spray process demonstrated a power conversion efficiencies of up to 7.9%.
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We report the first soluble poly(3-dodecyl tellurophenylene-vinylene) polymer (P3TeV) by Stille copolymerization and compare its properties to the analogous thiophene and selenophene containing polymers. The optical band gap of the polymers is shown to systematically decrease as the size of the heteroatom is increased, mainly as a result of a stabilization of the LUMO energy, resulting in a small band gap of 1.4 eV for P3TeV. Field effect transistors measurements in variety of architectures demonstrate that the selenophene polymer exhibits the highest mobility, highlighting that increasing the size of the heteroatom is not always beneficial for charge transport.
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The photo- and electroluminescence properties of a series of novel, heteroleptic, mer-cyclometallated iridium complexes have been fine-tuned from green to blue by changing the substituents on the pyridyl ring of the phenylpyridyl ligand. The X-ray crystal structures of two Ir-based triazolyl complexes are reported.
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The preparation of the 3,6-disubstituted dibenzosilole monomers , and by two different routes is described; Suzuki copolymerisation afforded poly(9,9-dioctyl-3,6-dibenzosilole) which has a sufficiently high triplet energy (2.55 eV) to function as a host for green electrophosphorescent emitters.
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Fully printed perovskite solar cells are demonstrated with slot-die coating, a scalable printing method. A sequential slot-die coating process is developed to produce efficient perovskite solar cells and to be used in a large-scale roll-to-roll printing process. All layers excluding the electrodes are printed and devices demonstrate up to 11.96% power conversion efficiency. It is also demonstrated that the new process can be used in roll-to-roll production.
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A high molecular weight donor-acceptor conjugated polymer is synthesized using the Suzuki polycondensation method. Using this polymer, a single-junction bulk-heterojunction solar cell is fabricated giving a power conversion efficiency of 9.4% using a fullerene-modified ZnO interlayer at the cathode contact.
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Light-emitting electrochemical cells (LECs) consists of a thin film of an ionic organic semiconductor sandwiched between two electrodes. Because of the large density of ions, LECs are often reported to perform independently on the electrodes work function. Here we use metal oxides as charge injection layers and demonstrate that, although electroluminescence is observed independently of the electrodes used, the device performances are strongly dependent on the choice of the interface materials. Relying on metal oxide charge injection layers, such hybrid devices are of interest for real lighting applications and could pave the way for new efficient, stable, low-cost lighting sources.
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Detailed electrochemical studies have been undertaken on molecular aggregation of the organic semiconductor 7,14-bis((triisopropylsilyl)-ethynyl)dibenzo[b,def]chrysene (TIPS-DBC), which is used as an electron donor material in organic solar cells. Intermolecular association of neutral TIPS-DBC molecules was established by using (1)H NMR spectroscopy as well as by the pronounced dependence of the color of TIPS-DBC solutions on concentration. Diffusion limited current data provided by near steady-state voltammetry also reveal aggregation. Furthermore, variation of concentration produces large changes in shapes of transient DC and Fourier transformed AC (FTAC) voltammograms for oxidation of TIPS-DBC in dichloromethane. Subtle effects of molecular aggregation on the reduction of TIPS-DBC are also revealed by the highly sensitive FTAC voltammetric method. Simulations of FTAC voltammetric data provide estimates of the kinetic and thermodynamic parameters associated with oxidation and reduction of TIPS-DBC. Significantly, aggregation of TIPS-DBC facilitates both one-electron oxidation and reduction by shifting the reversible potentials to less and more positive values, respectively. EPR spectroscopy is used to establish the identity of one-electron oxidized and reduced forms of TIPS-DBC. Implications of molecular aggregation on the HOMO energy level in solution are considered with respect to efficiency of organic photovoltaic devices utilizing TIPS-DBC as an electron donor material.
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Vide infra: Two boron-dipyrromethene (BODIPY)-type infrared sensitizers are investigated for use in titania-based dye-sensitized solar cells (DSCs). The DSCs use a solution of dimethylferrocene (Me2 Fc) in nitromethane as electrolyte. The titania conduction band edge is fine-tuned by adding lithium ions from LiTFSI, while the choice of dimethylferrocene as redox shuttle provides the ideal driving force for dye regeneration, allowing the BODIPY-based DSCs to reach unprecedented quantum efficiencies in the near-infrared.
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Colorantes/química , Suministros de Energía Eléctrica , Compuestos Ferrosos/química , Rayos Infrarrojos , Luz Solar , Titanio/química , Oxidación-ReducciónRESUMEN
Efficient low-band-gap polymers are one key component for constructing tandem solar cells with other higher-band-gap materials to harvest wide absorption of the solar spectrum. The N-acyldithieno[3,2-b:2',3'-d]pyrrole (DTP) building block is used for making low-band-gap polymers. It is attractive because of its strong donating ability and relatively low highest-occupied-molecular-orbital level in comparison with the N-alkyl DTP building block. However, additional solubilizing groups on the accepting units are needed for soluble donor-acceptor polymers based on the N-alkanoyl DTP building block. Combining N-benzoyl DTP with a 4,7-dithieno-2,1,3-benzothiadiazole building block, a polymer with a low band gap of 1.44 eV, delivers a high short-circuit current of 17.1 mA/cm(2) and a power conversion efficiency of 3.95%, which are the highest for the devices with DTP-containing materials. Herein, an alcohol-soluble diamine-modified fullerene cathode interfacial layer improved the device efficiency significantly more than the mono-amine analogue.
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An alcohol-soluble hyperbranched conjugated polymer HBPFN with a dimethylamino moiety is synthesized and used as a cathode interlayer. A PCE of 7.7% is obtained for PBDTTT-C-T/PC71 BM based solar cells. No obvious interfacial dipole is found at the interface between the active layer and HBPFN however, an interfacial dipole with the cathode could be one of the reasons for the enhanced performance.
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Polímeros/química , Energía Solar , Suministros de Energía Eléctrica , Electrodos , Fluorenos/química , Poliestirenos/química , Teoría Cuántica , Tiofenos/químicaRESUMEN
A structure-device performance correlation in bulk heterojunction solar cells for new indandione-derived small molecule electron acceptors, FEHIDT and F8IDT, is presented. Devices based on the former exhibit higher power conversion efficiency (2.4%) and higher open circuit voltage, a finding consistent with reduced intermolecular interactions.