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  • Journal article
    Limbu S, Park K-B, Wu J, Cha H, Yun S, Lim S-J, Yan H, Luke J, Ryu G, Heo C-J, Kim S, Jin YW, Durrant JR, Kim J-Set al., 2021,

    Identifying the Molecular Origins of High-Performance in Organic Photodetectors Based on Highly Intermixed Bulk Heterojunction Blends.

    , ACS Nano, Vol: 15, Pages: 1217-1228

    A bulk-heterojunction (BHJ) structure of organic semiconductor blend is widely used in photon-to-electron converting devices such as organic photodetectors (OPD) and photovoltaics (OPV). However, the impact of the molecular structure on the interfacial electronic states and optoelectronic properties of the constituent organic semiconductors is still unclear, limiting further development of these devices for commercialization. Herein, the critical role of donor molecular structure on OPD performance is identified in highly intermixed BHJ blends containing a small-molecule donor and C60 acceptor. Blending introduces a twisted structure in the donor molecule and a strong coupling between donor and acceptor molecules. This results in ultrafast exciton separation (<1 ps), producing bound (binding energy ∼135 meV), localized (∼0.9 nm), and highly emissive interfacial charge transfer (CT) states. These interfacial CT states undergo efficient dissociation under an applied electric field, leading to highly efficient OPDs in reverse bias but poor OPVs. Further structural twisting and molecular-scale aggregation of the donor molecules occur in blends upon thermal annealing just above the transition temperature of 150 °C at which donor molecules start to reorganize themselves without any apparent macroscopic phase-segregation. These subtle structural changes lead to significant improvements in charge transport and OPD performance, yielding ultralow dark currents (∼10-10 A cm-2), 2-fold faster charge extraction (in μs), and nearly an order of magnitude increase in effective carrier mobility. Our results provide molecular insights into high-performance OPDs by identifying the role of subtle molecular structural changes on device performance and highlight key differences in the design of BHJ blends for OPD and OPV devices.

  • Journal article
    Luke J, Correa L, Rodrigues J, Martins J, Daboczi M, Bagnis D, Kim J-Set al., 2021,

    A Commercial Benchmark: Light-Soaking Free, Fully Scalable, Large-Area Organic Solar Cells for Low-Light Applications

  • Journal article
    Yiwen W, Jinho L, Xueyan H, Chiara L, Yan J, Eva M, Amber P, Jenny N, Ji-Seon K, Zhe Let al., 2021,

    Recent Progress and Challenges Towards Highly Stable Nonfullerene Acceptor-Based Organic Solar Cells

    , Advanced Energy Materials, ISSN: 1614-6832

    Organic solar cells (OSCs) based on nonfullerene acceptors (NFAs) have made significant breakthrough in their device performance, now achieving a power conversion efficiency of ≈18% for single junction devices, driven by the rapid development in their molecular design and device engineering in recent years. However, achieving long‐term stability remains a major challenge to overcome for their commercialization, due in large part to the current lack of understanding of their degradation mechanisms as well as the design rules for enhancing their stability. In this review, the recent progress in understanding the degradation mechanisms and enhancing the stability of high performance NFA‐based OSCs is a specific focus. First, an overview of the recent advances in the molecular design and device engineering of several classes of high performance NFA‐based OSCs for various targeted applications is provided, before presenting a critical review of the different degradation mechanisms identified through photochemical‐, photo‐, and morphological degradation pathways. Potential strategies to address these degradation mechanisms for further stability enhancement, from molecular design, interfacial engineering, and morphology control perspectives, are also discussed. Finally, an outlook is given highlighting the remaining key challenges toward achieving the long‐term stability of NFA‐OSCs.

  • Journal article
    Heeney M, Kafourou P, Park B, Luke J, Luxi T, Panidi J, Glöcklhofer F, Kim J, Anthopoulos TD, Kim J-S, Lee K, Kwon Set al., 2020,

    One-step Six-fold Cyanation of Benzothiadiazole Acceptor Units for Air-Stable High-Performance n-Type Organic Field-Effect Transistors

    , Angewandte Chemie International Edition, ISSN: 1433-7851

    We report a new high electron affinity acceptor end group for organic semiconductors, 2,1,3-benzothiadiazole-4,5,6-tricarbonitrile (TCNBT). An n-type organic semiconductor with an indacenodithiophene (IDT) core and TCNBT end groups was synthesized by a six-fold nucleophilic substitution with cyanides on a fluorinated precursor, itself prepared by a direct arylation approach. This one-step chemical modification was found to significantly impact the molecular properties: the fluorinated precursor, TFBT IDT, a poor ambipolar semiconductor, was converted into TCNBT IDT, a good n-type semiconductor. The highly electron-deficient end group TCNBT dramatically decreased the energy of the highest occupied and lowest unoccupied molecular orbitals (HOMO/LUMO) compared to the fluorinated analogue and improved the molecular orientation when utilized in n-type organic field-effect transistors (OFETs). Solution-processed OFETs based on TCNBT IDT exhibited a charge carrier mobility of up to µ e ≈ 0.15 cm 2 V -1 s -1 with excellent ambient stability for 100 hours, highlighting the benefits of the cyanated end group and the synthetic approach.

  • Journal article
    Tseng T-W, Yan H, Nakamura T, Omagari S, Kim J-S, Vacha Met al., 2020,

    Real-time monitoring of formation and dynamics of intra- and interchain phases in single molecules of polyfluorene

    , ACS Nano, Vol: 14, Pages: 16096-16104, ISSN: 1936-0851

    Poly(9,9-dioctylfluorene) (PFO) is one of the most important conjugated polymer materials, exhibiting outstanding photophysical and electrical properties. PFO is also known for a diversity of morphological phases determined by conformational states of the main chain. Our goal in this work is to address some of the key questions on formation and dynamics of one such conformation, the β-phase, by following in real time the evolution of fluorescence spectra of single PFO chains. The PFO is dispersed in a thin polystyrene film, and the spectra are monitored during the process of solvent vapor annealing with toluene. We confirm unambiguously that the PFO β-phase segments are formed on a true single-chain level at room temperature in the solvent-softened polystyrene. We further find that the formation of the β-phase is a dynamic and reversible process occurring on the order of seconds, leading to repeated spontaneous transitions between the glassy and β-phase segments during the annealing. Comparison of PFO with two largely different molecular weights (Mw) shows that chains with lower Mw form the β-phase segments much faster. For the high Mw PFO chains, a detailed Franck-Condon analysis of the β-phase spectra shows a large distribution of the Huang-Rhys factor, S, and even dynamic changes of this factor occurring on a single chain. Such dynamics are likely a manifestation of changing coherence length of the exciton. Further, for the high Mw PFO chains we observe an additional conformational state, a crystalline γ-phase. The γ-phase formation is also a spontaneous reversible process in the solvent-softened matrix. The phase can form from both the β-phase and the glassy phase, and the formation requires high Mw to enable intersegment interactions in a self-folded chain.

  • Journal article
    Stewart K, Limbu S, Nightingale J, Pagano K, Park B, Hong S, Lee K, Kwon S, Kim J-Set al., 2020,

    Molecular understanding of a pi-conjugated polymer/solid-state ionic liquid complex as a highly sensitive and selective gas sensor

    , JOURNAL OF MATERIALS CHEMISTRY C, Vol: 8, Pages: 15268-15276, ISSN: 2050-7526
  • Journal article
    Dong Y, Nikolis VC, Talnack F, Chin Y-C, Benduhn J, Londi G, Kublitski J, Zheng X, Mannsfeld SCB, Spoltore D, Muccioli L, Li J, Blase X, Beljonne D, Kim J-S, Bakulin AA, D'Avino G, Durrant JR, Vandewal Ket al., 2020,

    Orientation dependent molecular electrostatics drives efficient charge generation in homojunction organic sol

    , Nature Communications, Vol: 11, ISSN: 2041-1723

    Organic solar cells usually utilise a heterojunction between electron-donating (D) and electron-accepting (A) materials to split excitons into charges. However, the use of D-A blends intrinsically limits the photovoltage and introduces morphological instability. Here, we demonstrate that polycrystalline films of chemically identical molecules offer a promising alternative and show that photoexcitation of α-sexithiophene (α-6T) films results in efficient charge generation. This leads to α-6T based homojunction organic solar cells with an external quantum efficiency reaching up to 44% and an open-circuit voltage of 1.61 V. Morphological, photoemission, and modelling studies show that boundaries between α-6T crystalline domains with different orientations generate an electrostatic landscape with an interfacial energy offset of 0.4 eV, which promotes the formation of hybridised exciton/charge-transfer states at the interface, dissociating efficiently into free charges. Our findings open new avenues for organic solar cell design where material energetics are tuned through molecular electrostatic engineering and mesoscale structural control.

  • Journal article
    Kwon S, Pak Y, Kim B, Park B, Kim J, Kim G, Jo Y-R, Limbu S, Stewart K, Kim H, Kim B-J, Jang S-Y, Kang H, Min J-W, Kim J-S, Jung GY, Lee Ket al., 2020,

    Molecular-level electrochemical doping for fine discrimination of volatile organic compounds in organic chemiresistors

    , JOURNAL OF MATERIALS CHEMISTRY A, Vol: 8, Pages: 16884-16891, ISSN: 2050-7488
  • Journal article
    Jayaram AK, Pitsalidis C, Tan E, Moysidou C-M, De Volder MFL, Kim J-S, Owens RMet al., 2020,

    3D Hybrid Scaffolds Based on PEDOT:PSS/MWCNT Composites (vol 7, 363, 2019)

    , FRONTIERS IN CHEMISTRY, Vol: 8, ISSN: 2296-2646
  • Journal article
    Wu J, Lee J, Chin Y-C, Yao H, Cha H, Luke J, Hou J, Kim J-S, Durrant Jet al., 2020,

    Exceptionally low charge trapping enables highly efficient organic bulk heterojunction solar cells

    , Energy & Environmental Science, Vol: 13, Pages: 2422-2430, ISSN: 1754-5692

    In this study, we investigate the underlying origin of the high performance of PM6:Y6 organic solar cells. Employing transient optoelectronic and photoemission spectroscopies, we find that this blend exhibits greatly suppressed charge trapping into electronic intra-bandgap tail states compared to other polymer/non-fullerene acceptor solar cells, attributed to lower energetic disorder. The presence of tail states is a key source of energetic loss in most organic solar cells, as charge carriers relax into these states, reducing the quasi-Fermi level splitting and therefore device VOC. DFT and Raman analyses indicate this suppression of tail state energetics disorder could be associated with a higher degree of conformational rigidity and uniformity for the Y6 acceptor. We attribute the origin of such conformational rigidity and uniformity of Y6 to the presence of the two alkyl side chains on the outer core that restricts end-group rotation by acting as a conformation locker. The resultant enhanced carrier dynamics and suppressed charge carrier trapping are proposed to be a key factor behind the high performance of this blend. Low energetic disorder is suggested to be a key factor enabling reasonably efficient charge generation in this low energy offset system. In the absence of either energetic disorder or a significant electronic energy offset, it is argued that charge separation in this system is primarily entropy driven. Nevertheless, photocurrent generation is still limited by slow hole transfer from Y6 to PM6, suggesting pathways for further efficiency improvement.

  • Journal article
    Daboczi M, Kim J, Lee J, Kang H, Hamilton I, Lin C-T, Dimitrov SD, McLachlan MA, Lee K, Durrant JR, Kim J-Set al., 2020,

    Towards efficient integrated perovskite/organic bulk heterojunction solar cells: interfacial energetic requirement to reduce charge carrier recombination losses

    , Advanced Functional Materials, Vol: 30, Pages: 1-8, ISSN: 1616-301X

    Integrated perovskite/organic bulk heterojunction (BHJ) solar cells have the potential to enhance the efficiency of perovskite solar cells by a simple one‐step deposition of an organic BHJ blend photoactive layer on top of the perovskite absorber. It is found that inverted structure integrated solar cells show significantly increased short‐circuit current (J sc) gained from the complementary absorption of the organic BHJ layer compared to the reference perovskite‐only devices. However, this increase in J sc is not directly reflected as an increase in power conversion efficiency of the devices due to a loss of fill factor. Herein, the origin of this efficiency loss is investigated. It is found that a significant energetic barrier (≈250 meV) exists at the perovskite/organic BHJ interface. This interfacial barrier prevents efficient transport of photogenerated charge carriers (holes) from the BHJ layer to the perovskite layer, leading to charge accumulation at the perovskite/BHJ interface. Such accumulation is found to cause undesirable recombination of charge carriers, lowering surface photovoltage of the photoactive layers and device efficiency via fill factor loss. The results highlight a critical role of the interfacial energetics in such integrated cells and provide useful guidelines for photoactive materials (both perovskite and organic semiconductors) required for high‐performance devices.

  • Journal article
    Nightingale J, Pitsalidis C, Pappa A-M, Tan E, Stewart K, Owens RM, Kim J-Set al., 2020,

    Small molecule additive for low-power accumulation mode organic electrochemical transistors

    , Journal of Materials Chemistry C, Vol: 8, Pages: 8846-8855, ISSN: 2050-7526

    A small molecule additive, dodecylbenzenesulfonate (DBSA), is added to the electrolyte in OECTs to improve the device performance.

  • Journal article
    Luo H, Dimitrov S, Daboczi M, Kim J-S, Guo Q, Fang Y, Stoeckel M-A, Samori P, Fenwick O, Sobrido ABJ, Wang X, Titirici M-Met al., 2020,

    Nitrogen-Doped Carbon Dots/TiO2 Nanoparticle Composites for Photoelectrochemical Water Oxidation

    , ACS APPLIED NANO MATERIALS, Vol: 3, Pages: 3371-3381, ISSN: 2574-0970
  • Journal article
    Iandolo D, Sheard J, Levy GK, Pitsalidis C, Tan E, Dennis A, Kim J-S, Markaki AE, Widera D, Owens RMet al., 2020,

    Biomimetic and electroactive 3D scaffolds for human neural crest-derived stem cell expansion and osteogenic differentiation

    , MRS COMMUNICATIONS, Vol: 10, Pages: 179-187, ISSN: 2159-6859
  • Journal article
    Lin C-T, Lee J, Kim J, Macdonald TJ, Ngiam J, Xu B, Daboczi M, Xu W, Pont S, Park B, Kang H, Kim J-S, Payne DJ, Lee K, Durrant JR, McLachlan MAet al., 2020,

    Origin of open-circuit voltage enhancements in planar Perovskite solar cells induced by addition of bulky organic cations

    , Advanced Functional Materials, Vol: 30, ISSN: 1616-301X

    The origin of performance enhancements in p‐i‐n perovskite solar cells (PSCs) when incorporating low concentrations of the bulky cation 1‐naphthylmethylamine (NMA) are discussed. A 0.25 vol % addition of NMA increases the open circuit voltage (Voc) of methylammonium lead iodide (MAPbI3) PSCs from 1.06 to 1.16 V and their power conversion efficiency (PCE) from 18.7% to 20.1%. X‐ray photoelectron spectroscopy and low energy ion scattering data show NMA is located at grain surfaces, not the bulk. Scanning electron microscopy shows combining NMA addition with solvent assisted annealing creates large grains that span the active layer. Steady state and transient photoluminescence data show NMA suppresses non‐radiative recombination resulting from charge trapping, consistent with passivation of grain surfaces. Increasing the NMA concentration reduces device short‐circuit current density and PCE, also suppressing photoluminescence quenching at charge transport layers. Both Voc and PCE enhancements are observed when bulky cations (phenyl(ethyl/methyl)ammonium) are incorporated, but not smaller cations (Cs/MA)—indicating size is a key parameter. Finally, it demonstrates that NMA also enhances mixed iodide/bromide wide bandgap PSCs (Voc of 1.22 V with a 1.68 eV bandgap). The results demonstrate a facile approach to maximizing Voc and provide insights into morphological control and charge carrier dynamics induced by bulky cations in PSCs.

  • Journal article
    Hamilton I, Suh M, Kim K, Jeon DY, Bradley DDC, Kim J-Set al., 2020,

    Organic-inorganic hybrid composites as an electron injection layer in highly efficient inverted green-emitting polymer LEDs

    , Organic Electronics, Vol: 77, Pages: 1-8, ISSN: 1566-1199

    Organic-inorganic hybrid light emitting diodes (HyLEDs) consist of an organic emission layer in combination with at least one metal oxide charge injection layer in an inverted structure. Low temperature, solution processing of metal oxide charge injection layers is one of the key factors in reducing the manufacture cost of HyLEDs. Herein, we report the use of composite materials, comprising conjugated polyelectrolytes (CPE) and zinc oxide nanoparticles (ZnO NPs), as the electron injection layer (EIL) in highly-efficient, green-light-emitting poly (9,9-dioctylfluorene-co-benzothiadiazole) (F8BT) polymer LEDs that are carefully optimised for use in an inverted HyLED architecture for the first time. The composite CPE:ZnO EILs are processed via a room temperature, one-step, solution deposition and enable superior device performance relative to ZnO NPs on their own. We find that specifically, they (i) improve EIL morphology, reducing surface roughness as well as pin-hole size and density, (ii) induce a favourable vacuum level shift for electron injection by coordinate bonding between the CPE and ZnO constituents, and (iii) reduce interfacial quenching by passivation of ZnO chemical defects caused by oxygen vacancies. This work is also the first demonstration that blending ZnO NPs and CPE supports much faster electroluminescence turn-on times (∼7.12 μs) than for traditional ZnO/CPE bilayer devices (∼0.4 s) via ‘locking’ of the CPE mobile ions, as well as higher device performance. This demonstrates good suitability for display applications. After optimisation of the EIL composition and the thickness of the F8BT emissive layer, we achieve promising device efficiencies of 16.5 cd/A and 5.41 lm/W for devices with a 1.1 μm thick F8BT layer, which is particularly relevant for potential roll-to-roll fabrication. These results clearly demonstrate the potential that this organic-inorganic composite EIL material has for the realisation of cheap, scalable

  • Journal article
    Tan E, Pappa A-M, Pitsalidis C, Nightingale J, Wood S, Castro FA, Owens RM, Kim J-Set al., 2020,

    A highly sensitive molecular structural probe applied to in-situ biosensing of metabolites using PEDOT:PSS

    , Biotechnology and Bioengineering, Vol: 117, Pages: 291-299, ISSN: 0006-3592

    A large amount of research within organic biosensors is dominated by organic electrochemical transistors (OECTs) that use conducting polymers such as poly(3,4-ethylene dioxythiophene doped with poly(styrenesulfonate) (PEDOT:PSS). Despite the recent advances in OECT-based biosensors, the sensing is solely reliant on the amperometric detection of the bioanalytes. This is typically accompanied by large undesirable parasitic electrical signals from the electroactive components in the electrolyte. Herein, we present the use of in-situ resonance Raman spectroscopy to probe subtle molecular structural changes of PEDOT:PSS associated with its doping level. We demonstrate how such doping level changes of PEDOT:PSS can be used, for the first time, on operational OECTs for sensitive and selective metabolite sensing whilst simultaneously performing amperometric detection of the analyte. We test the sensitivity by molecularly sensing a lowest glucose concentration of 0.02 mM in phosphate buffered saline (PBS) solution. By changing the electrolyte to cell culture media, the selectivity of in-situ resonance Raman spectroscopy is emphasized as it remains unaffected by other electroactive components in the electrolyte. The application of this molecular structural probe highlights the importance of developing biosensing probes that benefit from high sensitivity of the material's structural and electrical properties whilst being complimentary with the electronic methods of detection.

  • Journal article
    Daboczi M, Hamilton I, Xu S, Luke J, Limbu S, Lee J, McLachlan MA, Lee K, Durrant JR, Baikie ID, Kim J-Set al., 2019,

    Origin of Open-Circuit Voltage Losses in Perovskite Solar Cells Investigated by Surface Photovoltage Measurement

    , ACS Applied Materials & Interfaces, Vol: 11, Pages: 46808-46817, ISSN: 1944-8244
  • Journal article
    Kasimatis M, Nunez-Bajo E, Grell M, Cotur Y, Barandun G, Kim J-S, Guder Fet al., 2019,

    Monolithic solder-on nanoporous Si-Cu contacts for stretchable silicone composite sensors

    , ACS Applied Materials and Interfaces, Vol: 11, Pages: 47577-47586, ISSN: 1944-8244

    We report a method of creating solderable, mechanically robust, electrical contacts to interface (soft) silicone-based strain sensors with conventional (hard) solid-state electronics using a nanoporous Si-Cu composite. The Si-based solder-on electrical contact consists of a copper-plated nanoporous Si top surface formed through metal-assisted chemical etching and electroplating, and a smooth Si bottom surface which can be covalently bonded onto silicone-based strain sensors through plasma bonding. We investigated the mechanical and electrical properties of the contacts proposed under relevant ranges of mechanical stress for applications in physiological monitoring and rehabilitation. We also produced a series of proof-of-concept devices, including a wearable respiration monitor, leg band for exercise monitoring and Squeeze-ball for monitoring rehabilitation of patients with hand injuries or neurological disorders, to demonstrate the mechanical robustness and versatility of the technology developed, in real-world applications.

  • Journal article
    Decataldo F, Druet V, Pappa A-M, Tan E, Savva A, Pitsalidis C, Inal S, Kim J-S, Fraboni B, Owens RM, Iandolo Det al., 2019,

    BMP-2 functionalized PEDOT:PSS-based OECTs for stem cell osteogenic differentiation monitoring

  • Journal article
    Wu J, Luke J, Lee HKH, Tuladhar PS, Cha H, Jang S-Y, Tsoi WC, Heeney M, Kang H, Lee K, Kirchartz T, Kim J-S, Durrant JRet al., 2019,

    Tail state limited photocurrent collection of thick photoactive layers in organic solar cells

    , Nature Communications, Vol: 10, ISSN: 2041-1723

    Weanalyseorganic solar cells with four differentphotoactive blends exhibiting differing dependencies ofshort-circuit current upon photoactive layer thickness.These blends and devices are analysedbytransient optoelectronic techniques ofcarrier kinetics and densities, airphotoemission spectroscopyof material energetics, Kelvin probe measurements of work function, Mott-Schottky analyses of apparent doping density and by device modelling. We concludethat,for the device series studied, the photocurrent losswith thick active layersis primarilyassociatedwith the accumulation of photo-generated charge carriers in intra-bandgap tail states.This charge accumulation screens the device internal electricalfield, preventing efficient charge collection. Purification of one studied donor polymer is observed to reduce tail statedistribution anddensity and increase the maximal photoactive thickness forefficient operation. Ourwork suggests that selectingorganic photoactive layerswith a narrow distribution of tail states isa keyrequirement for the fabrication of efficient, high photocurrent, thick organic solar cells.

  • Journal article
    Yan H, Limbu S, Wang X, Nightingale J, Hamilton I, Wade J, Kwon S, Lee K, Kim J-Set al., 2019,

    Efficient charge carrier injection and balance achieved by low electrochemical doping in solution-processed polymer light-emitting diodes

    , Advanced Functional Materials, Vol: 29, Pages: 1-9, ISSN: 1616-301X

    Charge carrier injection and transport in polymer light‐emitting diodes (PLEDs) is strongly limited by the energy level offset at organic/(in)organic interfaces and the mismatch in electron and hole mobilities. Herein, these limitations are overcome via electrochemical doping of a light‐emitting polymer. Less than 1 wt% of doping agent is enough to effectively tune charge injection and balance and hence significantly improve PLED performance. For thick single‐layer (1.2 µm) PLEDs, dramatic reductions in current and luminance turn‐on voltages (VJ = 11.6 V from 20.0 V and VL = 12.7 V from 19.8 V with/without doping) accompanied by reduced efficiency roll‐off are observed. For thinner (<100 nm) PLEDs, electrochemical doping removes a thickness dependence on VJ and VL, enabling homogeneous electroluminescence emission in large‐area doped devices. Such efficient charge injection and balance properties achieved in doped PLEDs are attributed to a strong electrochemical interaction between the polymer and the doping agents, which is probed by in situ electric‐field‐dependent Raman spectroscopy combined with further electrical and energetic analysis. This approach to control charge injection and balance in solution‐processed PLEDs by low electrochemical doping provides a simple yet feasible strategy for developing high‐quality and efficient lighting applications that are fully compatible with printing technologies.

  • Journal article
    Wade J, Pugh H, Nightingale J, Kim J, Williams STet al., 2019,

    Colour in bivalve shells: Using resonance Raman spectroscopy to compare pigments at different phylogenetic levels

    , Journal of Raman Spectroscopy, Vol: 50, Pages: 1527-1536, ISSN: 0377-0486

    Several studies have suggested that shell colour may be phylogenetically distributed within the phylum Mollusca, but this pattern is confounded by our ignorance of the homology of colour and lack of understanding about the identity of most molluscan pigments. We use resonance Raman spectroscopy to address this problem by examining bivalve pigments producing a range of colours and compare spectra from taxa at different phylogenetic levels. The spectra of most shell pigments exhibited a skeletal signature typical of partially methylated polyenes, possibly modified carotenoids, with the strongest peaks occurring between 1,501–1,540 cm−1 and 1,117–1,144 cm−1 due to the C═C (ν1) and C–C (ν2) stretching modes, respectively. Neither pigment class nor mineral structure differentiated Imparidentia and Pteriomorphia. Spectral acquisitions for purple pigments for two species of Asaphis suggest that identical or nearly identical pigments are shared within this genus, and some red pigments from distantly related species have similar spectra. Conversely, two species with brown shells have distinctly different pigments, highlighting the difficulty in determining the homology of colour even within a single class of pigments. Curiously, we were unable to detect any Raman activity for green‐coloured shell or pigment peaks for the yellow area of Codakia paytenorum, suggesting that these colours are due to structural elements or a pigment that is quite different from those observed in other taxa examined to date. Our results are consistent with the idea that classes of pigments are evolutionarily ancient but heritable modifications may be specific to clades.

  • Journal article
    Way A, Luke J, Evans AD, Li Z, Kim J-S, Durrant JR, Hin Lee HK, Tsoi WCet al., 2019,

    Fluorine doped tin oxide as an alternative of indium tin oxide for bottom electrode of semi-transparent organic photovoltaic devices

    , AIP Advances, Vol: 9, Pages: 085220-1-085220-5, ISSN: 2158-3226

    Indium tin oxide (ITO) is commonly used as the transparent bottom electrode for organic solar cells. However, it is known that the cost ofthe ITO is quite high due to the indium element, and in some studies ITO coated glass substrate is found to be the most expensive componentof device fabrication. Moreover, indium migration from ITO can cause stability issues in organic solar cells. Nevertheless, the use of ITO asthe bottom electrode is still dominating in the field. Here, we explore the possibility of using fluorine doped tin oxide (FTO) as an alternativeto ITO for the bottom electrode of organic solar cells particularly on semi-transparent cells. We present side-by-side comparisons on theiroptical, morphological and device properties and suggest that FTO could be more suitable than ITO as the bottom electrode for glass substratebased organic photovoltaic devices.

  • Journal article
    Speller EM, Clarke AJ, Luke J, Lee HKH, Durrant JR, Li N, Wang T, Wong HC, Kim J-S, Tsoi WC, Li Zet al., 2019,

    From fullerene acceptors to non-fullerene acceptors: prospects and challenges in the stability of organic solar cells

    , Journal of Materials Chemistry A, ISSN: 2050-7488

    <p>This review highlights the opportunities and challenges in stability of organic solar cells arising from the emergence of non-fullerene acceptors.</p>

  • Journal article
    Cha H, Fish G, Luke J, Alraddadi A, Lee HH, Zhang W, Dong Y, Limbu S, Wadsworth A, Maria IP, Francas L, Sou HL, Du T, Kim J-S, McLachlan MA, McCulloch I, Durrant JRet al., 2019,

    Suppression of Recombination Losses in Polymer:Nonfullerene Acceptor Organic Solar Cells due to Aggregation Dependence of Acceptor Electron Affinity

    , ADVANCED ENERGY MATERIALS, Vol: 9, ISSN: 1614-6832
  • Journal article
    Du T, Xu W, Daboczi M, Kim J, Xu S, Lin C-T, Kang H, Lee K, Heeney MJ, Kim J-S, Durrant JR, McLachlan MAet al., 2019,

    p-Doping of organic hole transport layers in p–i–n perovskite solar cells: correlating open-circuit voltage and photoluminescence quenching

    , Journal of Materials Chemistry A, Vol: 7, Pages: 18971-18979, ISSN: 2050-7488

    Doping is a widely implemented strategy for enhancing the inherent electronic properties of charge transport layers in photovoltaic (PV) devices. Here, in direct contrast to existing understanding, we find that a reduction in p-doping of the organic hole transport layer (HTL) leads to substantial improvements in PV performance in planar p–i–n perovskite solar cells (PSCs), driven by improvements in open circuit voltage (VOC). Employing a range of transient and steady state characterisation tools, we find that the improvements of VOC correlate with reduced surface recombination losses in less p-doped HTLs. A simple device model including screening of bulk electric fields in the perovskite layer is used to explain this observation. In particular, photoluminescence (PL) emission of complete solar cells shows that efficient performance is correlated to a high PL intensity at open circuit and a low PL intensity at short circuit. We conclude that desirable transport layers for p–i–n PSCs should be charge selective contacts with low doping densities.

  • Journal article
    He Q, Shahid M, Panidi J, Marsh AV, Huang W, Daboczi M, Kim J-S, Fei Z, Anthopoulos TD, Heeney Met al., 2019,

    A versatile star-shaped organic semiconductor based on benzodithiophene and diketopyrrolopyrrole

    , Journal of Materials Chemistry C, Vol: 7, Pages: 6622-6629, ISSN: 2050-7526

    We report the synthesis of a new star-shaped π-conjugated oligomer, BDT(DPP)4, containing a benzodithiophene core and four diketopyrrolopyrrole arms. The thermal, electrochemical and optical properties are characterized and the results complemented by computational studies. The utility of the molecule is demonstrated in both solar cell and field-effect transistor devices. In the former, BDT(DPP)4 displays low efficiency when used as an acceptor in blends with poly(3-hexylthiophene) but exhibits promising performance as a donor, in blends with either a fullerene or a non-fullerene acceptor. In field-effect transistors BDT(DPP)4 exhibits typical p-type transistor behavior, which is in accordance with its better donor performance in solar cell devices.

  • Journal article
    Jayaram AK, Pitsalidis C, Tan E, Moysidou C-M, De Voider MFL, Kim J-S, Owens RMet al., 2019,

    3D hybrid scaffolds based on PEDOT:PSS/MWCNT composites

    , Frontiers in Chemistry, Vol: 7, Pages: 1-9, ISSN: 2296-2646

    Conducting polymer scaffolds combine the soft-porous structures of scaffolds with the electrical properties of conducting polymers. In most cases, such functional systems are developed by combining an insulating scaffold matrix with electrically conducting materials in a 3D hybrid network. However, issues arising from the poor electronic properties of such hybrid systems, hinder their application in many areas. This work reports on the design of a 3D electroactive scaffold, which is free of an insulating matrix. These 3D polymer constructs comprise of a water soluble conducting polymer (PEDOT:PSS) and multi-walled carbon nanotubes (MWCNTs). The insertion of the MWCNTs in the 3D polymer matrix directly contributes to the electron transport efficiency, resulting in a 7-fold decrease in resistivity values. The distribution of CNTs, as characterized by SEM and Raman spectroscopy, further define the micro- and nano-structural topography while providing active sites for protein attachment, thereby rendering the system suitable for biological/sensing applications. The resulting scaffolds, combine high porosity, mechanical stability and excellent conducting properties, thus can be suitable for a variety of applications ranging from tissue engineering and biomedical devices to (bio-) energy storage.

  • Journal article
    Wang Y, Daboczi M, Mesa CA, Ratnasingham SR, Kim JS, Durrant JR, Dunn S, Yan H, Briscoe J, Wang Y, Daboczi M, Mesa CA, Ratnasingham SR, Kim J-S, Durrant JR, Dunn S, Yan H, Briscoe Jet al., 2019,

    Bi₂Fe₄O₉ thin films as novel visible-light-active photoanodes for solar water splitting

    , Journal of Materials Chemistry A, Vol: 7, Pages: 9537-9541, ISSN: 2050-7496

    We report the chemical solution deposition (CSD) of a phase-pure Bi2Fe4O9 thin film for use as a photoanode in photoelectrochemical (PEC) water splitting. The energy levels of Bi2Fe4O9 films have been measured and n-type characteristics have been confirmed. With band gaps determined as 2.05 eV (indirect) and 2.80 eV (direct) and valence and conduction bands straddling the water oxidation and reduction potentials, this material is highly promising as a photocatalyst for solar water splitting. The photocurrent of a planar photoanode reached 0.1 mA cm−2 at 1.23 VNHE under AM1.5G illumination. The addition of H2O2 as a hole scavenger increased the photocurrent to 0.25 mA cm−2, indicating hole injection is one limiting factor to the performance. The performance was enhanced by nearly 5-fold when the Bi2Fe4O9 photoanode is coupled to a Co–Pi surface co-catalyst. The photoanode also shows excellent stability with no change in photocurrent over three hours of continuous illumination. These results indicate that this material represents a promising addition to the growing selection of low-cost, stable photocatalysts for use in solar water splitting.

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