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  • Journal article
    Chen H, Hurhangee M, Nikolka M, Zhang W, Kirkus M, Neophytou M, Cryer SJ, Harkin D, Hayoz P, Abdi-Jalebi M, McNeill CR, Sirringhaus H, McCulloch Iet al., 2017,

    Dithiopheneindenofluorene (<bold>TIF</bold>) Semiconducting Polymers with Very High Mobility in Field-Effect Transistors

    , ADVANCED MATERIALS, Vol: 29, ISSN: 0935-9648
  • Journal article
    Utzat H, Dimitroy SD, Wheeler S, Collado-Fregoso E, Tuladhar PS, Schroeder BC, McCulloch I, Durrant JRet al., 2017,

    Charge-Separation in Intermixed Polymer:PC70BM Photovoltaic Blends: Correlating Structural and Photophysical Length Scales as a Function of Blend Composition

    , JOURNAL OF PHYSICAL CHEMISTRY C, Vol: 121, Pages: 9790-9801, ISSN: 1932-7447

    A key challenge in achieving control over photocurrent generation by bulk-heterojunction organic solar cells is understanding how the morphology of the active layer impacts charge separation and in particular the separation dynamics within molecularly intermixed donor–acceptor domains versus the dynamics between phase-segregated domains. This paper addresses this issue by studying blends and devices of the amorphous silicon–indacenodithiophene polymer SiIDT-DTBT and the acceptor PC70BM. By changing the blend composition, we modulate the size and density of the pure and intermixed domains on the nanometer length scale. Laser spectroscopic studies show that these changes in morphology correlate quantitatively with the changes in charge separation dynamics on the nanosecond time scale and with device photocurrent densities. At low fullerene compositions, where only a single, molecularly intermixed polymer–fullerene phase is observed, photoexcitation results in a ∼ 30% charge loss from geminate polaron pair recombination, which is further studied via light intensity experiments showing that the radius of the polaron pairs in the intermixed phase is 3–5 nm. At high fullerene compositions (≥67%), where the intermixed domains are 1–3 nm and the pure fullerene phases reach ∼4 nm, the geminate recombination is suppressed by the reduction of the intermixed phase, making the fullerene domains accessible for electron escape.

  • Journal article
    Barbe J, Tietze ML, Neophytou M, Murali B, Alarousu E, El Labban A, Abulikemu M, Yue W, Mohammed OF, McCulloch I, Amassian A, Del Gobbo Set al., 2017,

    Amorphous Tin Oxide as a Low-Temperature -Processed Electron Transport Layer for Organic and Hybrid Perovskite Solar Cells

    , ACS APPLIED MATERIALS & INTERFACES, Vol: 9, Pages: 11828-11836, ISSN: 1944-8244
  • Journal article
    Kumar N, Zoladek-Lemanczyk A, Guilbert AAY, Su W, Tuladhar SM, Kirchartz T, Schroeder BC, McCulloch I, Nelson J, Roy D, Castro FAet al., 2017,

    Simultaneous topographical, electrical and optical microscopy of optoelectronic devices at the nanoscale

    , Nanoscale, Vol: 9, Pages: 2723-2731, ISSN: 2040-3364

    Novel optoelectronic devices rely on complex nanomaterial systems where the nanoscale morphology and local chemical composition are critical to performance. However, the lack of analytical techniques that can directly probe these structure–property relationships at the nanoscale presents a major obstacle to device development. In this work, we present a novel method for non-destructive, simultaneous mapping of the morphology, chemical composition and photoelectrical properties with <20 nm spatial resolution by combining plasmonic optical signal enhancement with electrical-mode scanning probe microscopy. We demonstrate that this combined approach offers subsurface sensitivity that can be exploited to provide molecular information with a nanoscale resolution in all three spatial dimensions. By applying the technique to an organic solar cell device, we show that the inferred surface and subsurface composition distribution correlates strongly with the local photocurrent generation and explains macroscopic device performance. For instance, the direct measurement of fullerene phase purity can distinguish between high purity aggregates that lead to poor performance and lower purity aggregates (fullerene intercalated with polymer) that result in strong photocurrent generation and collection. We show that the reliable determination of the structure–property relationship at the nanoscale can remove ambiguity from macroscopic device data and support the identification of the best routes for device optimisation. The multi-parameter measurement approach demonstrated herein is expected to play a significant role in guiding the rational design of nanomaterial-based optoelectronic devices, by opening a new realm of possibilities for advanced investigation via the combination of nanoscale optical spectroscopy with a whole range of scanning probe microscopy modes.

  • Journal article
    Baran D, Kirchartz T, Wheeler S, Dimitrov S, Abdelsamie M, Gorman J, Ashraf R, Holliday S, Wadsworth A, Gasparini N, Kaienburg P, Yan H, Amassian A, Brabec C, Durrant J, McCulloch Iet al., 2016,

    Reduced voltage losses yield 10% efficient fullerene free organic solar cells with >1 V open circuit voltages

    , Energy & Environmental Science, Vol: 9, Pages: 3783-3793, ISSN: 1754-5706

    Optimization of the energy levels at the donor–acceptor interface of organic solar cells has driven their efficiencies to above 10%. However, further improvements towards efficiencies comparable with inorganic solar cells remain challenging because of high recombination losses, which empirically limit the open-circuit voltage (Voc) to typically less than 1 V. Here we show that this empirical limit can be overcome using non-fullerene acceptors blended with the low band gap polymer PffBT4T-2DT leading to efficiencies approaching 10% (9.95%). We achieve Voc up to 1.12 V, which corresponds to a loss of only Eg/q − Voc = 0.5 ± 0.01 V between the optical bandgap Eg of the polymer and Voc. This high Voc is shown to be associated with the achievement of remarkably low non-geminate and non-radiative recombination losses in these devices. Suppression of non-radiative recombination implies high external electroluminescence quantum efficiencies which are orders of magnitude higher than those of equivalent devices employing fullerene acceptors. Using the balance between reduced recombination losses and good photocurrent generation efficiencies achieved experimentally as a baseline for simulations of the efficiency potential of organic solar cells, we estimate that efficiencies of up to 20% are achievable if band gaps and fill factors are further optimized.

  • Journal article
    Baran D, Ashraf RS, Hanifi DA, Abdelsamie M, Gasparini N, Röhr JA, Holliday S, Wadsworth A, Lockett S, Neophytou M, Emmott CJ, Nelson J, Brabec CJ, Amassian A, Salleo A, Kirchartz T, Durrant JR, McCulloch Iet al., 2016,

    Reducing the efficiency-stability-cost gap of organic photovoltaics with highly efficient and stable small molecule acceptor ternary solar cells

    , Nature Materials, Vol: 16, Pages: 363-369, ISSN: 1476-4660

    Technological deployment of organic photovoltaic modules requires improvements in device light-conversion efficiency and stability while keeping material costs low. Here we demonstrate highly efficient and stable solar cells using a ternary approach, wherein two non-fullerene acceptors are combined with both a scalable and affordable donor polymer, poly(3-hexylthiophene) (P3HT), and a high-efficiency, low-bandgap polymer in a single-layer bulk-heterojunction device. The addition of a strongly absorbing small molecule acceptor into a P3HT-based non-fullerene blend increases the device efficiency up to 7.7 ± 0.1% without any solvent additives. The improvement is assigned to changes in microstructure that reduce charge recombination and increase the photovoltage, and to improved light harvesting across the visible region. The stability of P3HT-based devices in ambient conditions is also significantly improved relative to polymer:fullerene devices. Combined with a low-bandgap donor polymer (PBDTTT-EFT, also known as PCE10), the two mixed acceptors also lead to solar cells with 11.0 ± 0.4% efficiency and a high open-circuit voltage of 1.03 ± 0.01 V.

  • Journal article
    Fallon KJ, Wijeyasinghe N, Manley EF, Dimitrov SD, Yousaf SA, Ashraf RS, Duffy W, Guilbert AAY, Freeman DME, Al-Hashimi M, Nelson J, Durrant JR, Chen LX, McCulloch I, Marks TJ, Clarke TM, Anthopoulos TD, Bronstein Het al., 2016,

    Indolo-naphthyridine-6,13-dione Thiophene Building Block for Conjugated Polymer Electronics: Molecular Origin of Ultrahigh n-Type Mobility

    , CHEMISTRY OF MATERIALS, Vol: 28, Pages: 8366-8378, ISSN: 0897-4756
  • Journal article
    Nam S, Han H, Seo J, Song M, Kim H, Anthopoulos TD, McCulloch I, Bradley DDC, Kim Yet al., 2016,

    Ambipolar Organic Phototransistors with p-Type/n-Type Conjugated Polymer Bulk Heterojunction Light-Sensing Layers

  • Journal article
    Giovannitti A, nielsen CN, Sbircea DTS, Inal SI, Donahue MD, Niazi MN, Hanifi DH, Amassian AA, Malliaras GGM, Rivnay JR, McCulloch IMet al., 2016,

    N-type organic electrochemical transistors with stability in water

    , Nature Communications, Vol: 7, Pages: 1-10, ISSN: 2041-1723

    Organic electrochemical transistors (OECTs) are receiving significant attention due to their ability to efficiently transduce biological signals. A major limitation of this technology is that only p-type materials have been reported, which precludes the development of complementary circuits, and limits sensor technologies. Here, we report the first ever n-type OECT, with relatively balanced ambipolar charge transport characteristics based on a polymer that supports both hole and electron transport along its backbone when doped through an aqueous electrolyte and in the presence of oxygen. This new semiconducting polymer is designed specifically to facilitate ion transport and promote electrochemical doping. Stability measurements in water show no degradation when tested for 2 h under continuous cycling. This demonstration opens the possibility to develop complementary circuits based on OECTs and to improve the sophistication of bioelectronic devices.

  • Journal article
    Yue W, Nikolka M, Xiao M, Sadhanala A, Nielsen CB, White AJP, Chen H-Y, Onwubiko A, Sirringhaus H, McCulloch Iet al., 2016,

    Azaisoindigo conjugated polymers for high performance n-type and ambipolar thin film transistor applications

    , JOURNAL OF MATERIALS CHEMISTRY C, Vol: 4, Pages: 9704-9710, ISSN: 2050-7526
  • Journal article
    Vezie M, Few S, Meager I, Pieridou G, Dörling B, Ashraf RA, Goñi AR, Bronstein H, McCulloch I, Hayes SC, Campoy-Quiles M, Nelson Jet al., 2016,

    Exploring the origin of high optical absorption in conjugated polymers

    , Nature Materials, Vol: 15, Pages: 746-753, ISSN: 1476-4660

    The specific optical absorption of an organic semiconductor is critical to the performance of organic optoelectronic devices. For example, higher light-harvesting efficiency can lead to higher photocurrent in solar cells that are limited by sub-optimal electrical transport. Here, we compare over 40 conjugated polymers, and find that many different chemical structures share an apparent maximum in their extinction coefficients. However, a diketopyrrolopyrrole-thienothiophene copolymer shows remarkably high optical absorption at relatively low photon energies. By investigating its backbone structure and conformation with measurements and quantum chemical calculations, we find that the high optical absorption can be explained by the high persistence length of the polymer. Accordingly, we demonstrate high absorption in other polymers with high theoretical persistence length. Visible light harvesting may be enhanced in other conjugated polymers through judicious design of the structure.

  • Journal article
    Holliday S, Ashraf RS, Wadsworth A, Baran D, Yousaf A, Nielsen CB, Tan C, Dimitrov S, Shang Z, Gasparini N, Alamoudi M, Laquai F, Brabec C, Salleo A, Durrant J, Mcculloch Iet al., 2016,

    High-efficiency and air-stable P3HT-based polymer solar cells with a new non-fullerene acceptor

    , Nature Communications, Vol: 7, Pages: 1-11, ISSN: 2041-1723

    Solution-processed organic photovoltaics (OPV) offer the attractive prospect of low-cost, light-weight and environmentally benign solar energy production. The highest efficiency OPV at present use low-bandgap donor polymers, many of which suffer from problems with stability and synthetic scalability. They also rely on fullerene-based acceptors, which themselves have issues with cost, stability and limited spectral absorption. Here we present a new non-fullerene acceptor that has been specifically designed to give improved performance alongside the wide bandgap donor poly(3-hexylthiophene), a polymer with significantly better prospects for commercial OPV due to its relative scalability and stability. Thanks to the well-matched optoelectronic and morphological properties of these materials, efficiencies of 6.4% are achieved which is the highest reported for fullerene-free P3HT devices. In addition, dramatically improved air stability is demonstrated relative to other high-efficiency OPV, showing the excellent potential of this new material combination for future technological applications.

  • Journal article
    Harkin DJ, Broch K, Schreck M, Ceymann H, Stoy A, Yong CK, Nikolka M, McCulloch I, Stingelin N, Lambert C, Sirringhaus Het al., 2016,

    Decoupling Charge Transport and Electroluminescence in a High Mobility Polymer Semiconductor

    , Advanced Materials, Vol: 28, Pages: 6378-6385, ISSN: 1521-4095

    Fluorescence enhancement of a high mobility polymer semiconductor is achieved via energy transfer to a higher fluorescence quantum yield squaraine dye molecule on 50 ps timescales. In organic light emitting diodes an order of magnitude enhancement of the external quantum efficiency is observed without reduction in the charge carrier mobility resulting in radiances of up to 5 W str(-1) m(-2) at 800 nm.

  • Journal article
    Dimitrov SD, Schroeder BC, Nielsen CB, Bronstein H, Fei Z, McCulloch I, Heeney M, Durrant JRet al., 2016,

    Singlet Exciton Lifetimes in Conjugated Polymer Films for Organic Solar Cells

    , Polymers, Vol: 8, ISSN: 2073-4360

    The lifetime of singlet excitons in conjugated polymer films is a key factor taken into account during organic solar cell device optimization. It determines the singlet exciton diffusion lengths in polymer films and has a direct impact on the photocurrent generation by organic solar cell devices. However, very little is known about the material properties controlling the lifetimes of singlet excitons, with most of our knowledge originating from studies of small organic molecules. Herein, we provide a brief summary of the nature of the excited states in conjugated polymer films and then present an analysis of the singlet exciton lifetimes of 16 semiconducting polymers. The exciton lifetimes of seven of the studied polymers were measured using ultrafast transient absorption spectroscopy and compared to the lifetimes of seven of the most common photoactive polymers found in the literature. A plot of the logarithm of the rate of exciton decay vs. the polymer optical bandgap reveals a medium correlation between lifetime and bandgap, thus suggesting that the Energy Gap Law may be valid for these systems. This therefore suggests that small bandgap polymers can suffer from short exciton lifetimes, which may limit their performance in organic solar cell devices. In addition, the impact of film crystallinity on the exciton lifetime was assessed for a small bandgap diketopyrrolopyrrole co-polymer. It is observed that the increase of polymer film crystallinity leads to reduction in exciton lifetime and optical bandgap again in agreement with the Energy Gap Law.

  • Journal article
    Heeney MJ, Han Y, Fei Z, McCulloch I, Stingelin N, Treat N, Anthopoulos T, Faber H, Zhang W, Zhu X, Feng Yet al., 2015,

    A Novel Alkylated Indacenodithieno[3,2-b]thiophene-based Polymer for High-performance Field Effect Transistors

    , Advanced Materials, Vol: 28, Pages: 3922-3927, ISSN: 1521-4095

    A novel rigid donor monomer, indacenodithieno[3,2-b]thiophene (IDTT), containing linear alkyl chains is reported. Its copolymer with benzothiadiazole is an excellent p-type semiconductor, affording a mobility of 6.6 cm² V⁻¹ s⁻¹ in top-gated field-effect transistors with pentafluorobenzenethiol-modified Au electrodes. Electrode treatment with solution-deposited copper(I) thiocyanate (CuSCN) has a beneficial hole-injection/electron-blocking effect, further enhancing the mobility to 8.7 cm² V⁻¹ s⁻¹.

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