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  • 1.
    Abramavicius, V.
    et al.
    Vilnius University, Lithuania; Centre Phys Science and Technology, Lithuania.
    Pranculis, V.
    Centre Phys Science and Technology, Lithuania.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gulbinas, V.
    Centre Phys Science and Technology, Lithuania.
    Abramavicius, D.
    Vilnius University, Lithuania.
    Role of coherence and delocalization in photo-induced electron transfer at organic interfaces2016In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 6, no 32914Article in journal (Refereed)
    Abstract [en]

    Photo-induced charge transfer at molecular heterojunctions has gained particular interest due to the development of organic solar cells (OSC) based on blends of electron donating and accepting materials. While charge transfer between donor and acceptor molecules can be described by Marcus theory, additional carrier delocalization and coherent propagation might play the dominant role. Here, we describe ultrafast charge separation at the interface of a conjugated polymer and an aggregate of the fullerene derivative PCBM using the stochastic Schrodinger equation (SSE) and reveal the complex time evolution of electron transfer, mediated by electronic coherence and delocalization. By fitting the model to ultrafast charge separation experiments, we estimate the extent of electron delocalization and establish the transition from coherent electron propagation to incoherent hopping. Our results indicate that even a relatively weak coupling between PCBM molecules is sufficient to facilitate electron delocalization and efficient charge separation at organic interfaces.

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  • 2.
    Andersson, Mattias L
    et al.
    Lund University, Sweden .
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Infahasaeng, Yingyot
    Lund University, Sweden .
    Tang, Zheng
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Yartsev, Arkady
    Lund University, Sweden .
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Sundstrom, Villy
    Lund University, Sweden .
    Unified Study of Recombination in Polymer:Fullerene Solar Cells Using Transient Absorption and Charge-Extraction Measurements2013In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 4, no 12, p. 2069-2072Article in journal (Refereed)
    Abstract [en]

    Recombination in the well-performing bulk heterojunction solar cell blend between the conjugated polymer TQ-1 and the substituted fullerene PCBM has been investigated with pump-probe transient absorption and charge extraction of photo-generated carriers (photo-CELIV). Both methods are shown to generate identical and overlapping data under appropriate experimental conditions. The dominant type of recombination is bimolecular with a rate constant of 7 x 10(-12) cm(-3) s(-1). This recombination rate is shown to be fully consistent with solar cell performance. Deviations from an ideal bimolecular recombination process, in this material system only observable at high pump fluences, are explained with a time-dependent charge-carrier mobility, and the implications of such a behavior for device development are discussed.

  • 3.
    Bergqvist, Jonas
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Andersson, Olof
    Linköping University, Department of Physics, Chemistry and Biology, Chemical and Optical Sensor Systems. Linköping University, Faculty of Science & Engineering.
    Lindqvist, Camilla
    INTERACT, Department of Engineering and Physics, Karlstad University, Karlstad, Sweden.
    Musumeci, Chiara
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Time-resolved morphology formation of solution cast polymer: fullerene blends revealed by in-situ photoluminescence spectroscopy2015Manuscript (preprint) (Other academic)
    Abstract [en]

    The nanoscale morphology of the photo-active layer in organic solar cells is critical for device efficiency. The photoactive layer is cast from solution and during drying both the polymer and the fullerene self-assemble to form a blend. Here, we introduce in-situ spectroscopic photoluminescence (PL) combined with laser reflectometry to monitor the drying process of an amorphous polymer:fullerene blend. When casting only the pristine components (polymer or PCBM only), the strength of PL emission is proportional to the solid content of the drying solution, and both kinetics reveal a rapid aggregation onset at the final stage of film drying. On the contrary, when casting polymer:fullerene blends, the strength of PL emission is proportional to the wet film thickness and reveals polymer/fullerene charge transfer (CT) already at the earliest stages of film drying, i.e. in dilute solutions. The proposed method allows to detect polymer/fullerene phase separation during film casting – from a reduction in the PL quenching rate as the film dries. Poor solvents lead to phase separation already at early stages of film drying (low solid content), resulting in a coarse final morphology as confirmed by atomic force microscopy (AFM). We therefore anticipate that the proposed method will be an important tool in the future development of processing inks, not only for solution-cast polymer:fullerene solar cells but also for organic heterojunctions in general.

  • 4.
    Bergqvist, Jonas
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tress, Wolfgang
    Laboratory of Photonics and Interfaces, Swiss Federal Institute of Technology (EPFL), Lausanne, Switzerland.
    Forchheimer, Daniel
    Nanostructure Physics, KTH Royal Institute of Technology, Stockholm, Sweden.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tang, Zheng
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Haviland, David
    Nanostructure Physics, KTH Royal Institute of Technology, Stockholm, Sweden.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    New method for lateral mapping of bimolecular recombination in thin film organic solar cells2016In: Progress in Photovoltaics, ISSN 1062-7995, E-ISSN 1099-159X, Vol. 24, no 8, p. 1096-1108Article in journal (Refereed)
    Abstract [en]

    The best organic solar cells are limited by bimolecular recombination. Tools to study these losses are available; however, they are only developed for small area (laboratory-scale) devices and are not yet available for large area (production-scale) devices. Here we introduce the Intermodulation Light Beam-Induced Current (IMLBIC) technique, which allows simultaneous spatial mapping of both the amount of extracted photocurrent and the bimolecular recombination over the active area of a solar cell. We utilize the second-order non-linear dependence on the illumination intensity as a signature for bimolecular recombination. Using two lasers modulated with different frequencies, we record the photocurrent response at each modulation frequency and the bimolecular recombination in the second-order intermodulation response at the sum and difference of the two frequencies. Drift-diffusion simulations predict a unique response for different recombination mechanisms. We successfully verify our approach by studying solar cells known to have mainly bimolecular recombination and thus propose this method as a viable tool for lateral detection and characterization of the dominant recombination mechanisms in organic solar cells. We expect that IMLBIC will be an important future tool for characterization and detection of recombination losses in large area organic solar cells.

  • 5.
    Bergqvist, Jonas
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics.
    Österberg, Thomas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics.
    Ever Aguirre, Luis
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics.
    Tang, Zheng
    Dresden Integrated Center for Applied Physics and Photonic Materials (IAPP) and Institute for Applied Physics, Technische Universität Dresden, Nöthnitzer Str. 61, Dresden, 01187, Germany.
    Cai, Wanzhu
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics.
    Ma, Zaifei
    Dresden Integrated Center for Applied Physics and Photonic Materials (IAPP) and Institute for Applied Physics, Technische Universität Dresden, Nöthnitzer Str. 61, Dresden, 01187, Germany.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices.
    Gedefaw, Desta
    Flinders Centre for Nanoscale Science and Technology, Flinders University, Sturt Road, Bedford Park, Adelaide, 5042, Australia.
    Andersson, Mats R.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics.
    Asymmetric photocurrent extraction in semitransparent laminated flexible organic solar cells2018In: npj Flexible Electronics, ISSN 2397-4621, Vol. 2, no 1Article in journal (Refereed)
    Abstract [en]

    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.

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  • 6.
    Diaz de Zerio Mendaza, Amaia
    et al.
    Chalmers, Sweden.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Nugroho, Ferry A. A.
    Chalmers, Sweden.
    Backe, Olof
    Chalmers, Sweden.
    Olsson, Eva
    Chalmers, Sweden.
    Langhammer, Christoph
    Chalmers, Sweden.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Mueller, Christian
    Chalmers, Sweden.
    A fullerene alloy based photovoltaic blend with a glass transition temperature above 200 degrees C2017In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 5, no 8, p. 4156-4162Article in journal (Refereed)
    Abstract [en]

    Organic solar cells with a high degree of thermal stability require bulk-heterojunction blends that feature a high glass transition, which must occur considerably above the temperatures encountered during device fabrication and operation. Here, we demonstrate for the first time a polymer : fullerene blend with a glass transition temperature above 200 degrees C, which we determine by plasmonic nanospectroscopy. We achieve this strong tendency for glass formation through the use of an alloy of neat, unsubstituted C-60 and C-70, which we combine with the fluorothieno-benzodithiophene copolymer PTB7. A stable photovoltaic performance of PTB7 : C60 : C70 ternary blends is preserved despite annealing the active layer at up to 180 degrees C, which coincides with the onset of the glass transition. Rapid deterioration of the power conversion efficiency from initially above 5% only occurs upon exceeding the glass transition temperature of 224 degrees C of the ternary blend.

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  • 7.
    Diaz de Zerio Mendaza, Amaia
    et al.
    Chalmers, Sweden.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Rossbauer, Stephan
    University of London Imperial Coll Science Technology and Med, England; University of London Imperial Coll Science Technology and Med, England.
    Backe, Olof
    Chalmers, Sweden.
    Nordstierna, Lars
    Chalmers, Sweden.
    Erhart, Paul
    Chalmers, Sweden.
    Olsson, Eva
    Chalmers, Sweden.
    Anthopoulos, Thomas D.
    University of London Imperial Coll Science Technology and Med, England; University of London Imperial Coll Science Technology and Med, England.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Muller, Christian
    Chalmers, Sweden.
    High-Entropy Mixtures of Pristine Fullerenes for Solution-Processed Transistors and Solar Cells2015In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 27, no 45, p. 7325-Article in journal (Refereed)
    Abstract [en]

    The solubility of pristine fullerenes can be enhanced by mixing C-60 and C-70 due to the associated increase in configurational entropy. This "entropic dissolution" allows the preparation of field-effect transistors with an electron mobility of 1 cm(2) V-1 s(-1) and polymer solar cells with a highly reproducible power-conversion efficiency of 6%, as well as a thermally stable active layer.

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  • 8.
    Felekidis, Nikolaos
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering. Stanford University, CA 94305 USA.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
    Design Rule for Improved Open-Circuit Voltage in Binary and Ternary Organic Solar Cells2017In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 9, no 42, p. 37070-37077Article in journal (Refereed)
    Abstract [en]

    Mixing different compounds to improve functionality is one of the pillars of the organic electronics field. Here, the degree to which the charge transport properties of the constituent materials are simply additive when materials are mixed is quantified. It is demonstrated that in bulk heterojunction organic solar cells, hole mobility in the donor phase depends critically on the choice of the acceptor material, which may alter the energetic disorder of the donor. The same holds for electron mobility and disorder in the acceptor. The associated mobility differences can exceed an order of magnitude compared to pristine materials. Quantifying these effects by a state-filling model for the open-circuit voltage (V-oc) of ternary Donor:Acceptor(l):Acceptor(2) (D:A(1):A(2)) organic solar cells leads to a physically transparent description of the surprising, nearly linear tunability of the Voc with the A(1):A(2) weight ratio. It is predicted that in binary OPV systems, suitably chosen donor and acceptor materials can improve the device power conversion efficiency (PCE) by several percentage points, for example from 11 to 13.5% for a hypothetical state-ofthe-art organic solar cell, highlighting the importance of this design rule.

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  • 9.
    Felekidis, Nikolaos
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
    Nonequilibrium drift-diffusion model for organic semiconductor devices2016In: PHYSICAL REVIEW B, ISSN 2469-9950, Vol. 94, no 3, article id 035205Article in journal (Refereed)
    Abstract [en]

    Two prevailing formalisms are currently used to model charge transport in organic semiconductor devices. Drift-diffusion calculations, on the one hand, are time effective but assume local thermodynamic equilibrium, which is not always realistic. Kinetic Monte Carlo models, on the other hand, do not require this assumption but are computationally expensive. Here, we present a nonequilibrium drift-diffusion model that bridges this gap by fusing the established multiple trap and release formalism with the drift-diffusion transport equation. For a prototypical photovoltaic system the model is shown to quantitatively describe, with a single set of parameters, experiments probing (1) temperature-dependent steady-state charge transport-space-charge limited currents, and (2) time-resolved charge transport and relaxation of nonequilibrated photocreated charges. Moreover, the outputs of the developed kinetic drift-diffusion model are an order of magnitude, or more, faster to compute and in good agreement with kinetic Monte Carlo calculations.

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  • 10.
    Jasiunas, Rokas
    et al.
    Ctr Phys Sci and Technol, Lithuania.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering. Stanford Univ, CA 94305 USA.
    Xia, Yuxin
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Felekidis, Nikolaos
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
    Gulbinas, Vidmantas
    Ctr Phys Sci and Technol, Lithuania.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
    Dead Ends Limit Charge Carrier Extraction from All-Polymer Bulk Heterojunction Solar Cells2018In: ADVANCED ELECTRONIC MATERIALS, ISSN 2199-160X, Vol. 4, no 8, article id 1800144Article in journal (Refereed)
    Abstract [en]

    Extraction of photocreated charge carriers from a prototypical all-polymer organic solar cell is investigated by combining transient photocurrent and time-delayed collection field experiments with numerical simulations. It is found that extraction is significantly hampered by charges getting trapped in spatial traps that are tentatively attributed to dead ends in the intermixed polymer networkin photovoltaic devices based on the same donor polymer and a fullerene acceptor this effect is much weaker. The slow-down in charge extraction leads to enhanced recombination and associated performance losses. These effects are observed in addition to the dispersive behavior that is characteristic of charge motion in energetically disordered media. Upon annealing the effects of spatial traps diminish, rationalizing the doubling in device power conversion efficiency after annealing.

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  • 11.
    Karuthedath, Safakath
    et al.
    KAUST, Saudi Arabia.
    Gorenflot, Julien
    KAUST, Saudi Arabia.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kan, Zhipeng
    KAUST, Saudi Arabia.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Laquai, Frederic
    KAUST, Saudi Arabia.
    Buildup of Triplet-State Population in Operating TQ1:PC71BM Devices Does Not Limit Their Performance2020In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 11, no 8, p. 2838-2845Article in journal (Refereed)
    Abstract [en]

    Triplet generation in organic solar cells has been considered a major loss channel. Determining the density of the triplet-state population in an operating device is challenging. Here, we employ transient absorption (TA) spectroscopy on the quinoxaline-thiophene copolymer TQ1 blended with PC71BM, quantify the transient charge and tripletstate densities, and parametrize their generation and recombination dynamics. The charge recombination parameters reproduce the experimentally measured current-voltage characteristics in charge carrier drift-diffusion simulations, and they yield the steady-state charge densities. We demonstrate that triplets are formed by both geminate and nongeminate recombination of charge carriers and decay primarily by triplet-triplet annihilation. Using the charge densities in the rate equations describing triplet-state dynamics, we find that triplet-state densities in devices are in the range of charge carrier densities. Despite this substantial triplet-state buildup, TQ1:PC71BM devices exhibit only moderate geminate recombination and significantly reduced nongeminate charge recombination, with reduction factors between 10(-4) and 10(-3) compared to Langevin recombination.

  • 12.
    Karuthedath, Safakath
    et al.
    KAUST, Saudi Arabia.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering. Stanford Univ, CA 94305 USA.
    Kan, Zhipeng
    KAUST, Saudi Arabia.
    Pranculis, Vytenis
    Ctr Phys Sci and Technol, Lithuania.
    Wohlfahrt, Markus
    KAUST, Saudi Arabia.
    Khan, Jafar I.
    KAUST, Saudi Arabia.
    Gorenflot, Julien
    KAUST, Saudi Arabia.
    Xia, Yuxin
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gulbinas, Vidmantas
    Ctr Phys Sci and Technol, Lithuania.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
    Laquai, Frederic
    KAUST, Saudi Arabia.
    Thermal annealing reduces geminate recombination in TQ1:N2200 all-polymer solar cells2018In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 6, no 17, p. 7428-7438Article in journal (Refereed)
    Abstract [en]

    combination of steady-state and time-resolved spectroscopic measurements is used to investigate the photophysics of the all-polymer bulk heterojunction system TQ1:N2200. Upon thermal annealing a doubling of the external quantum efficiency and an improved fill factor (FF) is observed, resulting in an increase in the power conversion efficiency. Carrier extraction is similar for both blends, as demonstrated by time-resolved electric-field-induced second harmonic generation experiments in conjunction with transient photocurrent studies, spanning the ps-mu s time range. Complementary transient absorption spectroscopy measurements reveal that the different quantum efficiencies originate from differences in charge carrier separation and recombination at the polymer-polymer interface: in as-spun samples similar to 35% of the charges are bound in interfacial charge-transfer states and recombine geminately, while this pool is reduced to similar to 7% in thermally-annealed samples, resulting in higher short-circuit currents. Time-delayed collection field experiments demonstrate a field-dependent charge generation process in as-spun samples, which reduces the FF. In contrast, field-dependence of charge generation is weak in annealed films. While both devices exhibit significant non-geminate recombination competing with charge extraction, causing low FFs, our results demonstrate that the donor/acceptor interface in all-polymer solar cells can be favourably altered to enhance charge separation, without compromising charge transport and extraction.

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  • 13.
    Kroon, Renee
    et al.
    University of S Australia, Australia; Chalmers, Sweden.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zhuang, Wenliu
    Chalmers, Sweden.
    Bergqvist, Jonas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Diaz de Zerio Mendaza, Amaia
    Chalmers, Sweden.
    Steckler, Timothy T.
    Chalmers, Sweden.
    Yu, Liyang
    King Abdullah University of Science and Technology, Saudi Arabia.
    Bradley, Siobhan J.
    University of S Australia, Australia.
    Musumeci, Chiara
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gedefaw, Desta
    Chalmers, Sweden.
    Nann, Thomas
    University of S Australia, Australia.
    Amassian, Aram
    King Abdullah University of Science and Technology, Saudi Arabia.
    Muller, Christian
    Chalmers, Sweden.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Andersson, Mats R.
    University of S Australia, Australia; Chalmers, Sweden.
    Comparison of selenophene and thienothiophene incorporation into pentacyclic lactam-based conjugated polymers for organic solar cells2015In: Polymer Chemistry, ISSN 1759-9954, E-ISSN 1759-9962, Vol. 6, no 42, p. 7402-7409Article in journal (Refereed)
    Abstract [en]

    In this work, we compare the effect of incorporating selenophene versus thienothiophene spacers into pentacyclic lactam-based conjugated polymers for organic solar cells. The two cyclic lactam-based copolymers were obtained via a new synthetic method for the lactam moiety. Selenophene incorporation results in a broader and red-shifted optical absorption while retaining a deep highest occupied molecular orbital level, whereas thienothienophene incorporation results in a blue-shifted optical absorption. Additionally, grazing-incidence wide angle X-ray scattering data indicates edge- and face-on solid state order for the selenophene-based polymer as compared to the thienothiophene-based polymer, which orders predominantly edge-on with respect to the substrate. In polymer : PC71BM bulk heterojunction solar cells both materials show a similar open-circuit voltage of similar to 0.80-0.84 V, however the selenophene-based polymer displays a higher fill factor of similar to 0.70 vs. similar to 0.65. This is due to the partial face-on backbone orientation of the selenophene-based polymer, leading to a higher hole mobility, as confirmed by single-carrier diode measurements, and a concomitantly higher fill factor. Combined with improved spectral coverage of the selenophene-based polymer, as confirmed by quantum efficiency experiments, it offers a larger short-circuit current density of similar to 12 mA cm(-2). Despite the relatively low molecular weight of both materials, a very robust power conversion efficiency similar to 7% is achieved for the selenophene-based polymer, while the thienothiophene-based polymer demonstrates only a moderate maximum PCE of similar to 5.5%. Hence, the favorable effects of selenophene incorporation on the photovoltaic performance of pentacyclic lactam-based conjugated polymers are clearly demonstrated.

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  • 14. Order onlineBuy this publication >>
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Non-Equilibrium Charge Motion in Organic Solar Cells2017Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    Organic photovoltaic (OPV) devices based on semiconducting polymers and small molecules allow for a low cost alternative to inorganic solar cells. Recent developments show power conversion efficiencies as high as 10-12%, highlighting the potential of this technology. Nevertheless, further improvements are necessary to achieve commercialization.

    To a large extent the performance of these devices is dictated by their ability to extract the photo-generated charge, which is related to the charge carrier mobility. Various time-resolved and steady-state techniques are available to probe the charge carrier mobility in OPVs but often lead to different mobility values for one and the same system. Despite such conflicting observations it is generally assumed that charge transport in OPV devices can be described by well-defined charge carrier mobilities, typically obtained using a single steady-state technique. This thesis shows that the relevance of such well-defined mobilities for the charge separation and extraction processes is very limited.

    Although different transient techniques probe different time scales after photogeneration, they are mutually consistent as they probe the same physical mechanism governing charge motion – gradual thermalization of the photo-generated carriers in the disorder broadened density of states (DOS). The photo-generated carriers gradually lose their excess energy during transport to the extracting electrodes, but not immediately. Typically not all excess energy is dissipated as the photo-generated carriers tend to be extracted from the OPV device before reaching quasi-equilibrium.

    Carrier motion is governed by thermalization, leading to a time-dependent carrier mobility that is significantly higher than the steady-state mobility. This picture is confirmed by several transient techniques: Time-resolved Terahertz Spectroscopy (TRTS), Time-resolved Microwave Conductance (TRMC) combined with Transient Absorption (TA), electrical extraction of photo-induced charges (photo-CELIV). The connection between transient and steady-state mobility measurements (space-charge limited conductivity, SCLC) is described. Unification of transient opto-electric techniques to probe charge motion in OPVs is presented.

    Using transient experiments the distribution of extraction times of photo-generated charges in an operating OPV device has been determined and found to be strongly dispersive, spanning several decades in time. In view of the strong dispersion in extraction times the relevance of even a well-defined time-dependent mean mobility is limited.

    In OPVs a continuous ‘percolating’ donor network is often considered necessary for efficient hole extraction, whereas if the network is discontinuous, hole transport is thought to deteriorate significantly, limiting device performance. Here, it is shown that even highly diluted donor sites (5.7-10 %) in a buckminsterfullerene (C60) matrix enable reasonably efficient hole transport. Using transient measurements it is demonstrated that hole transport between isolated donor sites can occur by long-range hole tunneling (over distances of ~4 nm) through several C60 molecules – even a discontinuous donor network enables hole transport

    List of papers
    1. Unified Study of Recombination in Polymer:Fullerene Solar Cells Using Transient Absorption and Charge-Extraction Measurements
    Open this publication in new window or tab >>Unified Study of Recombination in Polymer:Fullerene Solar Cells Using Transient Absorption and Charge-Extraction Measurements
    Show others...
    2013 (English)In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 4, no 12, p. 2069-2072Article in journal (Refereed) Published
    Abstract [en]

    Recombination in the well-performing bulk heterojunction solar cell blend between the conjugated polymer TQ-1 and the substituted fullerene PCBM has been investigated with pump-probe transient absorption and charge extraction of photo-generated carriers (photo-CELIV). Both methods are shown to generate identical and overlapping data under appropriate experimental conditions. The dominant type of recombination is bimolecular with a rate constant of 7 x 10(-12) cm(-3) s(-1). This recombination rate is shown to be fully consistent with solar cell performance. Deviations from an ideal bimolecular recombination process, in this material system only observable at high pump fluences, are explained with a time-dependent charge-carrier mobility, and the implications of such a behavior for device development are discussed.

    Place, publisher, year, edition, pages
    American Chemical Society, 2013
    National Category
    Engineering and Technology
    Identifiers
    urn:nbn:se:liu:diva-95964 (URN)10.1021/jz4009745 (DOI)000320979400014 ()
    Note

    Funding Agencies|Swedish Research Council||Swedish Energy Agency (STEM)||Knut and Alice Wallenberg Foundation||ERC (VISCHEM)|226136|Wallenberg Scholar grant from the Knut and Alice Wallenberg Foundation||

    Available from: 2013-08-19 Created: 2013-08-12 Last updated: 2017-12-06
    2. Dispersion-Dominated Photocurrent in Polymer:Fullerene Solar Cells
    Open this publication in new window or tab >>Dispersion-Dominated Photocurrent in Polymer:Fullerene Solar Cells
    Show others...
    2014 (English)In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 24, no 28, p. 4507-4514Article in journal (Refereed) Published
    Abstract [en]

    Organic bulk heterojunction solar cells are often regarded as near-equilibrium devices, whose kinetics are set by well-defined charge carrier mobilities, and relaxation in the density of states is commonly ignored or included purely phenomenologically. Here, the motion of photocreated charges is studied experimentally with picosecond time resolution by a combination of time-resolved optical probing of electric field and photocurrent measurements, and the data are used to define parameters for kinetic Monte Carlo modelling. The results show that charge carrier motion in a prototypical polymer:fullerene solar cell under operational conditions is orders of magnitude faster than would be expected on the basis of corresponding near-equilibrium mobilities, and is extremely dispersive. There is no unique mobility. The distribution of extraction times of photocreated charges in operating organic solar cells can be experimentally determined from the charge collection transients measured under pulsed excitation. Finally, a remarkable distribution of the photocurrent over energy is found, in which the most relaxed charge carriers in fact counteract the net photocurrent.

    Place, publisher, year, edition, pages
    Weinheim, Germany: Wiley-VCH Verlagsgesellschaft, 2014
    Keywords
    solar cell; organic solar cell; dispersion; photocurrent; charge carrier relaxation; Monte Carlo simulations
    National Category
    Condensed Matter Physics
    Identifiers
    urn:nbn:se:liu:diva-108324 (URN)10.1002/adfm.201400404 (DOI)000339713900015 ()
    Note

    Funding agencies|Swedish Science Council (VR); Swedish Energy Agency; Knut and Alice Wallenberg foundation; European Social Fund under Global Grant measure

    Available from: 2014-06-26 Created: 2014-06-26 Last updated: 2017-12-05Bibliographically approved
    3. Photo-generated carriers lose energy during extraction from polymer-fullerene solar cells
    Open this publication in new window or tab >>Photo-generated carriers lose energy during extraction from polymer-fullerene solar cells
    Show others...
    2015 (English)In: Nature Communications, ISSN 2041-1723, E-ISSN 2041-1723, Vol. 6, no 8778Article in journal (Refereed) Published
    Abstract [en]

    In photovoltaic devices, the photo-generated charge carriers are typically assumed to be in thermal equilibrium with the lattice. In conventional materials, this assumption is experimentally justified as carrier thermalization completes before any significant carrier transport has occurred. Here, we demonstrate by unifying time-resolved optical and electrical experiments and Monte Carlo simulations over an exceptionally wide dynamic range that in the case of organic photovoltaic devices, this assumption is invalid. As the photo-generated carriers are transported to the electrodes, a substantial amount of their energy is lost by continuous thermalization in the disorder broadened density of states. Since thermalization occurs downward in energy, carrier motion is boosted by this process, leading to a time-dependent carrier mobility as confirmed by direct experiments. We identify the time and distance scales relevant for carrier extraction and show that the photo-generated carriers are extracted from the operating device before reaching thermal equilibrium.

    Place, publisher, year, edition, pages
    Nature Publishing Group, 2015
    National Category
    Biological Sciences Physical Sciences
    Identifiers
    urn:nbn:se:liu:diva-123824 (URN)10.1038/ncomms9778 (DOI)000366294700004 ()26537357 (PubMedID)
    Note

    Funding Agencies|Swedish Science Council and Energimyndigheten; Knut and Alice Wallenberg foundation; Deutsche Forschungsgemeinschaft [SPP1355]

    Available from: 2016-01-11 Created: 2016-01-11 Last updated: 2017-12-01
    4. Photogenerated Carrier Mobility Significantly Exceeds Injected Carrier Mobility in Organic Solar Cells
    Open this publication in new window or tab >>Photogenerated Carrier Mobility Significantly Exceeds Injected Carrier Mobility in Organic Solar Cells
    Show others...
    2017 (English)In: Advanced Energy Materials, ISSN 1614-6840, Vol. 7, no 9, article id 1602143Article in journal (Refereed) Published
    Abstract [en]

    Charge transport in organic photovoltaic (OPV) devices is often characterized by space-charge limited currents (SCLC). However, this technique only probes the transport of charges residing at quasi-equilibrium energies in the disorder-broadened density of states (DOS). In contrast, in an operating OPV device the photogenerated carriers are typically created at higher energies in the DOS, followed by slow thermalization. Here, by ultrafast time-resolved experiments and simulations it is shown that in disordered polymer/fullerene and polymer/polymer OPVs, the mobility of photogenerated carriers significantly exceeds that of injected carriers probed by SCLC. Time-resolved charge transport in a polymer/polymer OPV device is measured with exceptionally high (picosecond) time resolution. The essential physics that SCLC fails to capture is that of photo­generated carrier thermalization, which boosts carrier mobility. It is predicted that only for materials with a sufficiently low energetic disorder, thermalization effects on carrier transport can be neglected. For a typical device thickness of 100 nm, the limiting energetic disorder is σ ≈71 (56) meV for maximum-power point (short-circuit) conditions, depending on the error one is willing to accept. As in typical OPV materials the disorder is usually larger, the results question the validity of the SCLC method to describe operating OPVs.

    Place, publisher, year, edition, pages
    John Wiley & Sons, 2017
    Keywords
    charge carrier relaxation, charge carrier transport, organic photovoltaics, space-charge limited currents (SCLC), time-dependent mobility
    National Category
    Condensed Matter Physics Chemical Process Engineering Atom and Molecular Physics and Optics Physical Chemistry
    Identifiers
    urn:nbn:se:liu:diva-135770 (URN)10.1002/aenm.201602143 (DOI)000401719900010 ()
    Note

    Funding agencies: Research Council of Lithuania [MIP-085/2015]; Science Council; Knut and Alice Wallenberg foundation through a Wallenberg Scholar grant

    Available from: 2017-03-21 Created: 2017-03-21 Last updated: 2017-06-13Bibliographically approved
    5. Charge Transport in Pure and Mixed Phases in Organic Solar Cells
    Open this publication in new window or tab >>Charge Transport in Pure and Mixed Phases in Organic Solar Cells
    Show others...
    2017 (English)In: Advanced Energy Materials, ISSN 1614-6840, Vol. 7, no 20Article in journal (Refereed) Published
    Abstract [en]

    In organic solar cells continuous donor and acceptor networks are considered necessary for charge extraction, whereas discontinuous neat phases and molecularly mixed donor–acceptor phases are generally regarded as detrimental. However, the impact of different levels of domain continuity, purity, and donor–acceptor mixing on charge transport remains only semiquantitatively described. Here, cosublimed donor–acceptor mixtures, where the distance between the donor sites is varied in a controlled manner from homogeneously diluted donor sites to a continuous donor network are studied. Using transient measurements, spanning from sub-picoseconds to microseconds photogenerated charge motion is measured in complete photovoltaic devices, to show that even highly diluted donor sites (5.7%–10% molar) in a buckminsterfullerene matrix enable hole transport. Hopping between isolated donor sites can occur by long-range hole tunneling through several buckminsterfullerene molecules, over distances of up to ≈4 nm. Hence, these results question the relevance of “pristine” phases and whether a continuous interpenetrating donor–acceptor network is the ideal morphology for charge transport.

    Place, publisher, year, edition, pages
    John Wiley & Sons, 2017
    Keywords
    charge carrier transport, fullerene domains, low donor concentration, organic photovoltaics, tunneling
    National Category
    Physical Chemistry Condensed Matter Physics Biophysics Medical Biotechnology (with a focus on Cell Biology (including Stem Cell Biology), Molecular Biology, Microbiology, Biochemistry or Biopharmacy)
    Identifiers
    urn:nbn:se:liu:diva-139690 (URN)10.1002/aenm.201700888 (DOI)000413695300018 ()
    Note

    Funding agencies: German Federal Ministry for Education and Research (BMBF) through the InnoProfille project "Organische p-i-n Bauelemente 2.2"; Research Council of Lithuania [MIP-85/2015]; Science Council of Sweden; Knut and Alice Wallenberg foundation; Wallenberg Scholar

    Available from: 2017-08-09 Created: 2017-08-09 Last updated: 2017-11-13Bibliographically approved
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    Non-Equilibrium Charge Motion in Organic Solar Cells
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  • 15.
    Melianas, Armantas
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Etzold, Fabian
    Max Planck Institute Polymer Research, Germany.
    Savenije, Tom J.
    Delft University of Technology, Netherlands.
    Laquai, Frederic
    Max Planck Institute Polymer Research, Germany; King Abdullah University of Science and Technology, Saudi Arabia.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering. Eindhoven University of Technology, Netherlands.
    Photo-generated carriers lose energy during extraction from polymer-fullerene solar cells2015In: Nature Communications, ISSN 2041-1723, E-ISSN 2041-1723, Vol. 6, no 8778Article in journal (Refereed)
    Abstract [en]

    In photovoltaic devices, the photo-generated charge carriers are typically assumed to be in thermal equilibrium with the lattice. In conventional materials, this assumption is experimentally justified as carrier thermalization completes before any significant carrier transport has occurred. Here, we demonstrate by unifying time-resolved optical and electrical experiments and Monte Carlo simulations over an exceptionally wide dynamic range that in the case of organic photovoltaic devices, this assumption is invalid. As the photo-generated carriers are transported to the electrodes, a substantial amount of their energy is lost by continuous thermalization in the disorder broadened density of states. Since thermalization occurs downward in energy, carrier motion is boosted by this process, leading to a time-dependent carrier mobility as confirmed by direct experiments. We identify the time and distance scales relevant for carrier extraction and show that the photo-generated carriers are extracted from the operating device before reaching thermal equilibrium.

    Download full text (pdf)
    fulltext
  • 16.
    Melianas, Armantas
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Felekidis, Nikolaos
    Dept Phys Chem and Biol, Complex Mat and Devices, S-58183 Linkoping, Sweden.
    Puttisong, Yuttapoom
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Meskers, Stefan C. J.
    Eindhoven Univ Technol, Netherlands.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Chen, Weimin
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Nonequilibrium site distribution governs charge-transfer electroluminescence at disordered organic heterointerfaces2019In: Proceedings of the National Academy of Sciences of the United States of America, ISSN 0027-8424, E-ISSN 1091-6490, Vol. 116, no 47, p. 23416-23425Article in journal (Refereed)
    Abstract [en]

    The interface between electron-donating (D) and electron-accepting (A) materials in organic photovoltaic (OPV) devices is commonly probed by charge-transfer (CT) electroluminescence (EL) measurements to estimate the CT energy, which critically relates to device open-circuit voltage. It is generally assumed that during CT-EL injected charges recombine at close-to-equilibrium energies in their respective density of states (DOS). Here, we explicitly quantify that CT-EL instead originates from higher-energy DOS site distributions significantly above DOS equilibrium energies. To demonstrate this, we have developed a quantitative and experimentally calibrated model for CT-EL at organic D/A heterointerfaces, which simultaneously accounts for the charge transport physics in an energetically disordered DOS and the Franck-Condon broadening. The 0-0 CT-EL transition lineshape is numerically calculated using measured energetic disorder values as input to 3-dimensional kinetic Monte Carlo simulations. We account for vibrational CT-EL overtones by selectively measuring the dominant vibrational phonon-mode energy governing CT luminescence at the D/A interface using fluorescence line-narrowing spectroscopy. Our model numerically reproduces the measured CT-EL spectra and their bias dependence and reveals the higher-lying manifold of DOS sites responsible for CT-EL. Lowest-energy CT states are situated similar to 180 to 570 meV below the 0-0 CT-EL transition, enabling photogenerated carrier thermalization to these low-lying DOS sites when the OPV device is operated as a solar cell rather than as a light-emitting diode. Nonequilibrium site distribution rationalizes the experimentally observed weak current-density dependence of CT-EL and poses fundamental questions on reciprocity relations relating light emission to photovoltaic action and regarding minimal attainable photovoltaic energy conversion losses in OPV devices.

  • 17.
    Melianas, Armantas
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Pranculis, Vytenis
    Center for Physical Sciences and Technology, Lithuania.
    Devižis, Andrius
    Center for Physical Sciences and Technology, Lithuania.
    Gulbinas, Vidmantas
    Center for Physical Sciences and Technology, Lithuania.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, The Institute of Technology. Department of Applied Physics, Eindhoven University of Technology, MB, Eindhoven, The Netherlands.
    Dispersion-Dominated Photocurrent in Polymer:Fullerene Solar Cells2014In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 24, no 28, p. 4507-4514Article in journal (Refereed)
    Abstract [en]

    Organic bulk heterojunction solar cells are often regarded as near-equilibrium devices, whose kinetics are set by well-defined charge carrier mobilities, and relaxation in the density of states is commonly ignored or included purely phenomenologically. Here, the motion of photocreated charges is studied experimentally with picosecond time resolution by a combination of time-resolved optical probing of electric field and photocurrent measurements, and the data are used to define parameters for kinetic Monte Carlo modelling. The results show that charge carrier motion in a prototypical polymer:fullerene solar cell under operational conditions is orders of magnitude faster than would be expected on the basis of corresponding near-equilibrium mobilities, and is extremely dispersive. There is no unique mobility. The distribution of extraction times of photocreated charges in operating organic solar cells can be experimentally determined from the charge collection transients measured under pulsed excitation. Finally, a remarkable distribution of the photocurrent over energy is found, in which the most relaxed charge carriers in fact counteract the net photocurrent.

  • 18.
    Melianas, Armantas
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Pranculis, Vytenis
    Center for Physical Sciences and Technology, Vilnius, Lithuania.
    Spoltore, Donato
    Dresden Integrated Center for Applied Physics and Photonic Materials (IAPP) and Institute for Applied Physics, Technische Universität Dresden, Dresden, Germany.
    Benduhn, Johannes
    Dresden Integrated Center for Applied Physics and Photonic Materials (IAPP) and Institute for Applied Physics, Technische Universität Dresden, Dresden, Germany.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gulbinas, Vidmantas
    Center for Physical Sciences and Technology, Vilnius, Lithuania / Department of General Physics and Spectroscopy, Faculty of Physics, Vilnius University, Vilnius, Lithuania.
    Vandewal, Koen
    Dresden Integrated Center for Applied Physics and Photonic Materials (IAPP) and Institute for Applied Physics, Technische Universität Dresden, Dresden, Germany.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
    Charge Transport in Pure and Mixed Phases in Organic Solar Cells2017In: Advanced Energy Materials, ISSN 1614-6840, Vol. 7, no 20Article in journal (Refereed)
    Abstract [en]

    In organic solar cells continuous donor and acceptor networks are considered necessary for charge extraction, whereas discontinuous neat phases and molecularly mixed donor–acceptor phases are generally regarded as detrimental. However, the impact of different levels of domain continuity, purity, and donor–acceptor mixing on charge transport remains only semiquantitatively described. Here, cosublimed donor–acceptor mixtures, where the distance between the donor sites is varied in a controlled manner from homogeneously diluted donor sites to a continuous donor network are studied. Using transient measurements, spanning from sub-picoseconds to microseconds photogenerated charge motion is measured in complete photovoltaic devices, to show that even highly diluted donor sites (5.7%–10% molar) in a buckminsterfullerene matrix enable hole transport. Hopping between isolated donor sites can occur by long-range hole tunneling through several buckminsterfullerene molecules, over distances of up to ≈4 nm. Hence, these results question the relevance of “pristine” phases and whether a continuous interpenetrating donor–acceptor network is the ideal morphology for charge transport.

    Download full text (pdf)
    fulltext
  • 19.
    Melianas, Armantas
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Pranculis, Vytenis
    Center for Physical Sciences and Technology Savanoriu, Lithuania.
    Xia, Yuxin
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Felekidis, Nikolaos
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gulbinas, Vidmantas
    Center for Physical Sciences and Technology Savanoriu, Lithuania.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
    Photogenerated Carrier Mobility Significantly Exceeds Injected Carrier Mobility in Organic Solar Cells2017In: Advanced Energy Materials, ISSN 1614-6840, Vol. 7, no 9, article id 1602143Article in journal (Refereed)
    Abstract [en]

    Charge transport in organic photovoltaic (OPV) devices is often characterized by space-charge limited currents (SCLC). However, this technique only probes the transport of charges residing at quasi-equilibrium energies in the disorder-broadened density of states (DOS). In contrast, in an operating OPV device the photogenerated carriers are typically created at higher energies in the DOS, followed by slow thermalization. Here, by ultrafast time-resolved experiments and simulations it is shown that in disordered polymer/fullerene and polymer/polymer OPVs, the mobility of photogenerated carriers significantly exceeds that of injected carriers probed by SCLC. Time-resolved charge transport in a polymer/polymer OPV device is measured with exceptionally high (picosecond) time resolution. The essential physics that SCLC fails to capture is that of photo­generated carrier thermalization, which boosts carrier mobility. It is predicted that only for materials with a sufficiently low energetic disorder, thermalization effects on carrier transport can be neglected. For a typical device thickness of 100 nm, the limiting energetic disorder is σ ≈71 (56) meV for maximum-power point (short-circuit) conditions, depending on the error one is willing to accept. As in typical OPV materials the disorder is usually larger, the results question the validity of the SCLC method to describe operating OPVs.

    Download full text (pdf)
    fulltext
  • 20.
    Murthy, D H K
    et al.
    Delft University of Technology, Netherlands .
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Tang, Zheng
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Juska, Gytis
    Vilnius University, Lithuania .
    Arlauskas, Kestutis
    Vilnius University, Lithuania .
    Zhang, Fengling
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Siebbeles, Laurens D A
    Delft University of Technology, Netherlands .
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Savenije, Tom J
    Delft University of Technology, Netherlands .
    Origin of Reduced Bimolecular Recombination in Blends of Conjugated Polymers and Fullerenes2013In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 23, no 34, p. 4262-4268Article in journal (Refereed)
    Abstract [en]

    Bimolecular charge carrier recombination in blends of a conjugated copolymer based on a thiophene and quinoxaline (TQ1) with a fullerene derivative ((6,6)-phenyl-C-71-butyric acidmethyl ester, PC71BM) is studied by two complementary techniques. TRMC (time-resolved microwave conductance) monitors the conductance of photogenerated mobile charge carriers locally on a timescale of nanoseconds, while using photo-CELIV (charge extraction by linearly increasing voltage) charge carrier dynamics are monitored on a macroscopic scale and over tens of microseconds. Despite these significant differences in the length and time scales, both techniques show a reduced Langevin recombination with a prefactor close to 0.05. For TQ1:PC71BM blends, the value is independent of temperature. On comparing TRMC data with electroluminescence measurements it is concluded that the encounter complex and the charge transfer state have very similar energetic properties. The value for annealed poly(3-hexylthiophene) (P3HT):(6,6)-phenyl-C-61-butyric acid methyl ester (PC61BM) is approximately 10(-4), while for blend systems containing an amorphous polymer values are close to 1. These large differences can be related to the extent of charge delocalization of opposite charges in an encounter complex. Insight is provided into factors governing the bimolecular recombination process, which forms a major loss mechanism limiting the efficiency of polymer solar cells.

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  • 21.
    Roland, Steffen
    et al.
    Univ Potsdam, Germany; UP Transfer GmbH, Germany.
    Kniepert, Juliane
    Univ Potsdam, Germany.
    Love, John A.
    Univ Potsdam, Germany.
    Negi, Vikas
    Eindhoven Univ Technol, Netherlands.
    Liu, Feilong
    Eindhoven Univ Technol, Netherlands.
    Bobbert, Peter
    Eindhoven Univ Technol, Netherlands.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering. Stanford Univ, CA 94305 USA.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
    Hofacker, Andreas
    Tech Univ Dresden, Germany.
    Neher, Dieter
    Univ Potsdam, Germany.
    Equilibrated Charge Carrier Populations Govern Steady-State Nongeminate Recombination in Disordered Organic Solar Cells2019In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 10, no 6, p. 1374-1381Article in journal (Refereed)
    Abstract [en]

    We employed bias-assisted charge extraction techniques to investigate the transient and steady-state recombination of photogenerated charge carriers in complete devices of a disordered polymer-fullerene blend. Charge recombination is shown to be dispersive, with a significant slowdown of the recombination rate over time, consistent with the results from kinetic Monte Carlo simulations. Surprisingly, our experiments reveal little to no contributions from early time recombination of nonequilibrated charge carriers to the steady-state recombination properties. We conclude that energetic relaxation of photogenerated carriers outpaces any significant nongeminate recombination under application-relevant illumination conditions. With equilibrated charges dominating the steady-state recombination, quasi-equilibrium concepts appear suited for describing the open-circuit voltage of organic solar cells despite pronounced energetic disorder.

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    fulltext
  • 22.
    Tang, Zheng
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Elfwing, Anders
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Bergqvist, Jonas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Bao, Qinye
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, Faculty of Science & Engineering.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fully-solution-processed organic solar cells with a highly efficient paper-based light trapping element2015In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 3, no 48, p. 24289-24296Article in journal (Refereed)
    Abstract [en]

    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 approximate to 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.

  • 23.
    Tang, Zheng
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Liu, Bo
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Bergqvist, Jonas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Tress, Wolfgang
    Ecole Polytech Federal Lausanne, Switzerland.
    Bao, Qinye
    Linköping University, Department of Physics, Chemistry and Biology, Surface Physics and Chemistry. Linköping University, The Institute of Technology.
    Qian, Deping
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    Zhang, Fengling
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, The Institute of Technology.
    A New Fullerene-Free Bulk-Heterojunction System for Efficient High-Voltage and High-Fill Factor Solution-Processed Organic Photovoltaics2015In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 27, no 11, p. 1900-+Article in journal (Refereed)
    Abstract [en]

    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.

  • 24.
    Tang, Zheng
    et al.
    Linköping University, Department of Physics, Chemistry and Biology. Linköping University, Faculty of Science & Engineering. Donghua Univ, Peoples R China.
    Wang, Jing
    Donghua Univ, Peoples R China.
    Melianas, Armantas
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Wu, Yang
    Xi An Jiao Tong Univ, Peoples R China.
    Kroon, Renee
    Chalmers Univ Technol, Sweden.
    Li, Weiwei
    Chinese Acad Sci, Peoples R China.
    Ma, Wei
    Xi An Jiao Tong Univ, Peoples R China.
    Andersson, Mats R.
    Flinders Univ S Australia, Australia.
    Ma, Zaifei
    Donghua Univ, Peoples R China.
    Wanzhu, Cai
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tress, Wolfgang
    Ecole Polytech Fed Lausanne, Switzerland.
    Inganäs, Olle
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Relating open-circuit voltage losses to the active layer morphology and contact selectivity in organic solar cells2018In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 6, no 26, p. 12574-12581Article in journal (Refereed)
    Abstract [en]

    We demonstrate that voltage losses due to both radiative and non-radiative recombination of charge carriers are strongly dependent on D/A phase separation. By processing the active layer with various solvent additives, we create distinct morphologies that lead to significantly different device open-circuit voltages (V-OC), even though the charge transfer state energy (E-CT) of the D/A blend remains rather constant. We find that radiative recombination losses are significantly increased for a finely intermixed morphology, due to the large D/A interface area. This leads to a total recombination loss of E-CT - qV(OC) approximate to 0.7 eV. However, considerably smaller losses (0.5 eV), due to suppressed non-radiative recombination, are possible in solar cells where the D/A materials are organized to only allow for selective charge carrier extraction. Using a drift diffusion model, we show that the origin of the reduced non-radiative recombination losses is related to an effect which has not been considered for optimized solar cells - the suppression of minority carrier diffusion to the wrong contact. Our results suggest that the built-in field is not sufficiently strong even in optimized organic solar cells and that selective carrier extraction is critical for further improvements in V-OC.

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