Imperial College London

ProfessorIainMcCulloch

Faculty of Natural SciencesDepartment of Chemistry

Chair in Polymer Materials
 
 
 
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Contact

 

+44 (0)20 7594 5669i.mcculloch

 
 
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Location

 

RCS 1 M229ChemistrySouth Kensington Campus

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Summary

 

Publications

Publication Type
Year
to

407 results found

McCulloch I, 2019, New synthetic methodology paves the way to prepare electron deficient semiconducting mesopolymers with very high performance, Science China Chemistry, Vol: 62, Pages: 885-886, ISSN: 1674-7291

Journal article

Thomas TH, Harkin DJ, Gillett AJ, Lemaur V, Nikolka M, Sadhanala A, Richter JM, Armitage J, Chen H, McCulloch I, Menke SM, Olivier Y, Beljonne D, Sirringhaus Het al., 2019, Short contacts between chains enhancing luminescence quantum yields and carrier mobilities in conjugated copolymers, NATURE COMMUNICATIONS, Vol: 10, ISSN: 2041-1723

Journal article

Hu H, Deng W, Qin M, Yin H, Lau TK, Fong PWK, Ren Z, Liang Q, Cui L, Wu H, Lu X, Zhang W, McCulloch I, Li Get al., 2019, Charge carrier transport and nanomorphology control for efficient non-fullerene organic solar cells, Materials Today Energy, Vol: 12, Pages: 398-407

© 2019 Elsevier Ltd Single junction organic photovoltaic devices (OPVs) have exceeded 15% power conversion efficiency (PCE) with the help of fused ring based low-bandgap non-fullerene acceptors (NFAs). As a major type of NFA, the indacenodithiophene derivative NFA (IDTBR) has been shown to have superior OPV stability with outstanding V OC , but the efficiency is relatively lower compared to the reported OPV champion devices. Further improvements towards high efficiencies in this OPV system remains challenging due to the relatively poor charge carrier transport properties in the bulk heterojunction film, particularly the electron transport in small molecule non-fullerene acceptor network. Here we conducted detailed study on the dependence of carrier transport on BHJ donor–acceptor (D–A) composition. Our results show that the nano-morphology or phase aggregation of non-fullerene acceptor (NFA) molecules can be tuned via D–A composition in bulk heterojunction layer, and the improvement of electron mobility was shown to be enhanced by almost one order – from 1.23 × 10 −6 cm 2 /V (D:A = 1:1 by weight) to 1.02 × 10 −5 cm 2 /V (D:A = 1:2) – due to the improved connectivity of electron transport pathways. Further increase of NFA component content, however, has led to over-sized phase segregation, deteriorating the photovoltaic performance of organic soar cells. The optimized BHJ cell shows more balanced charge carrier transport and phase segregation, which yields a PCE of 10.79%. Furthermore, it shows a V OC as high as 1.03 V, which is ascribed to the significantly suppressed radiative and non-radiative recombination losses with bandgap-V OC offset E g /q-V OC of only 0.55 V.

Journal article

Ghasemi M, Hu H, Peng Z, Rech JJ, Angunawela I, Carpenter JH, Stuard SJ, Wadsworth A, McCulloch I, You W, Ade Het al., 2019, Delineation of Thermodynamic and Kinetic Factors that Control Stability in Non-fullerene Organic Solar Cells, JOULE, Vol: 3, Pages: 1328-1348, ISSN: 2542-4351

Journal article

Nikolka M, Broch K, Armitage J, Hanifi D, Nowack PJ, Venkateshvaran D, Sadhanala A, Saska J, Mascal M, Jung S-H, Lee J-K, McCulloch I, Salleo A, Sirringhaus Het al., 2019, High-mobility, trap-free charge transport in conjugated polymer diodes, Nature Communications, Vol: 10, ISSN: 2041-1723

Charge transport in conjugated polymer semiconductors has traditionally been thought to be limited to a low-mobility regime by pronounced energetic disorder. Much progress has recently been made in advancing carrier mobilities in field-effect transistors through developing low-disorder conjugated polymers. However, in diodes these polymers have to date not shown much improved mobilities, presumably reflecting the fact that in diodes lower carrier concentrations are available to fill up residual tail states in the density of states. Here, we show that the bulk charge transport in low-disorder polymers is limited by water-induced trap states and that their concentration can be dramatically reduced through incorporating small molecular additives into the polymer film. Upon incorporation of the additives we achieve space-charge limited current characteristics that resemble molecular single crystals such as rubrene with high, trap-free SCLC mobilities up to 0.2 cm2/Vs and a width of the residual tail state distribution comparable to kBT.

Journal article

Speller EM, Clarke AJ, Aristidou N, Wyatt MF, Francàs L, Fish G, Cha H, Lee HKH, Luke J, Wadsworth A, Evans AD, McCulloch I, Kim JS, Haque SA, Durrant JR, Dimitrov SD, Tsoi WC, Li Zet al., 2019, Toward improved environmental stability of polymer:fullerene and polymer:non-fullerene organic solar cells: a common energetic origin of light and oxygen induced degradation, ACS Energy Letters, Vol: 4, Pages: 846-852, ISSN: 2380-8195

With the emergence of nonfullerene electron acceptors resulting in further breakthroughs in the performance of organic solar cells, there is now an urgent need to understand their degradation mechanisms in order to improve their intrinsic stability through better material design. In this study, we present quantitative evidence for a common root cause of light-induced degradation of polymer:nonfullerene and polymer:fullerene organic solar cells in air, namely, a fast photo-oxidation process of the photoactive materials mediated by the formation of superoxide radical ions, whose yield is found to be strongly controlled by the lowest unoccupied molecular orbital (LUMO) levels of the electron acceptors used. Our results elucidate the general relevance of this degradation mechanism to both polymer:fullerene and polymer:nonfullerene blends and highlight the necessity of designing electron acceptor materials with sufficient electron affinities to overcome this challenge, thereby paving the way toward achieving long-term solar cell stability with minimal device encapsulation.

Journal article

Babics M, Duan T, Balawi AH, Liang R-Z, Cruciani F, Carja I-D, Gottlieb D, McCulloch I, Vandewal K, Laquai F, Beaujuge PMet al., 2019, Negligible Energy Loss During Charge Generation in Small-Molecule/Fullerene Bulk-Heterojunction Solar Cells Leads to Open-Circuit Voltage over 1.10 V, ACS APPLIED ENERGY MATERIALS, Vol: 2, Pages: 2717-2722, ISSN: 2574-0962

Journal article

Dimitrov SD, Azzouzi M, Wu J, Yao J, Dong Y, Tuladhar PS, Schroeder BC, Bittner ER, McCulloch I, Nelson J, Durrant JRet al., 2019, Spectroscopic Investigation of the Effect of Microstructure and Energetic Offset on the Nature of Interfacial Charge Transfer States in Polymer: Fullerene Blends., J Am Chem Soc, Vol: 141, Pages: 4634-4643

Despite performance improvements of organic photovoltaics, the mechanism of photoinduced electron-hole separation at organic donor-acceptor interfaces remains poorly understood. Inconclusive experimental and theoretical results have produced contradictory models for electron-hole separation in which the role of interfacial charge-transfer (CT) states is unclear, with one model identifying them as limiting separation and another as readily dissociating. Here, polymer-fullerene blends with contrasting photocurrent properties and enthalpic offsets driving separation were studied. By modifying composition, film structures were varied from consisting of molecularly mixed polymer-fullerene domains to consisting of both molecularly mixed and fullerene domains. Transient absorption spectroscopy revealed that CT state dissociation generating separated electron-hole pairs is only efficient in the high energy offset blend with fullerene domains. In all other blends (with low offset or predominantly molecularly mixed domains), nanosecond geminate electron-hole recombination is observed revealing the importance of spatially localized electron-hole pairs (bound CT states) in the electron-hole dynamics. A two-dimensional lattice exciton model was used to simulate the excited state spectrum of a model system as a function of microstructure and energy offset. The results could reproduce the main features of experimental electroluminescence spectra indicating that electron-hole pairs become less bound and more spatially separated upon increasing energy offset and fullerene domain density. Differences between electroluminescence and photoluminescence spectra could be explained by CT photoluminescence being dominated by more-bound states, reflecting geminate recombination processes, while CT electroluminescence preferentially probes less-bound CT states that escape geminate recombination. These results suggest that apparently contradictory studies on electron-hole separation can be exp

Journal article

Wang SJ, Venkateshvaran D, Mahani MR, Chopra U, McNellis ER, Di Pietro R, Schott S, Wittmann A, Schweicher G, Cubukcu M, Kang K, Carey R, Wagner TJ, Siebrecht JNM, Wong DPGH, Jacobs IE, Aboljadayel RO, Ionescu A, Egorov SA, Mueller S, Zadvorna O, Skalski P, Jellett C, Little M, Marks A, McCulloch I, Wunderlich J, Sinova J, Sirringhaus Het al., 2019, Long spin diffusion lengths in doped conjugated polymers due to enhanced exchange coupling, Nature Electronics, Vol: 2, Pages: 98-107

© 2019, The Author(s), under exclusive licence to Springer Nature Limited. Carbon-based semiconductors such as conjugated organic polymers are of potential use in the development of spintronic devices and spin-based information processing. In particular, these materials offer a low spin–orbit coupling strength due to their relatively light constituent chemical elements, which should, in principle, favour long spin diffusion lengths. However, organic polymers are relatively disordered materials and typically have a carrier mobility that is orders of magnitude lower than crystalline inorganic materials. As a result, small spin diffusion lengths of around 50 nm have typically been measured using vertical organic spin valves. Here, we report measuring spin diffusion lengths in doped conjugated polymers using a lateral spin transport device architecture, which is based on spin pumping injection and inverse spin Hall detection. The approach suggests that long spin diffusion lengths of more than 1 μm and fast spin transit times of around 10 ns are possible in conjugated polymer systems when they have a sufficiently high spin density (around 10 20 cm −3 ). We explain these results in terms of an exchange-based spin diffusion regime in which the exchange interactions decouple spin and charge transport.

Journal article

Moia D, Giovannitti A, Szumska AA, Maria IP, Rezasoltani E, Sachs M, Schnurr M, Barnes PRF, McCulloch I, Nelson Jet al., Design and evaluation of conjugated polymers with polar side chains as electrode materials for electrochemical energy storage in aqueous electrolytes, Energy & Environmental Science, ISSN: 1754-5692

<p>Solution processable p-type and n-type conjugated polymers with polar side chains enable fast charging in aqueous electrolytes and 1.4 V cell voltage.</p>

Journal article

Tan CH, Wadsworth A, Gasparini N, Wheeler S, Holliday S, Ashraf RS, Dimitrov SD, Baran D, McCulloch I, Durrant JRet al., 2019, Excitation Wavelength-Dependent Internal Quantum Efficiencies in a P3HT/Nonfullerene Acceptor Solar Cell, Journal of Physical Chemistry C, Vol: 123, Pages: 5826-5832, ISSN: 1932-7447

© 2018 American Chemical Society. Solar cells based on blends of the donor polymer, P3HT, with the nonfullerene acceptor, O-IDTBR, have been shown to exhibit promising efficiencies and stabilities for low-cost organic photovoltaic devices. We focus herein on the charge separation and recombination dynamics in such devices. By employing selective wavelength excitations of P3HT and O-IDTBR, we show that photoexcitation of P3HT results in lower internal quantum efficiency (IQE) for photocurrent generation than that observed for photoexcitation of O-IDTBR. Transient absorption and photoluminescence quenching studies indicate that this lower IQE results primarily from higher geminate recombination losses of photogenerated charges following P3HT excitation compared with O-IDTBR excitation, rather than from differences in exciton separation efficiency. These higher geminate recombination losses result in lower photocurrent generation efficiency at short circuit upon selective excitation of the P3HT donor, when compared with O-IDTBR excitation.

Journal article

Dong Y, Cha H, Zhang J, Pastor E, Tuladhar PS, McCulloch I, Durrant JR, Bakulin AAet al., 2019, The binding energy and dynamics of charge-transfer states in organic photovoltaics with low driving force for charge separation, Journal of Chemical Physics, Vol: 150, ISSN: 0021-9606

Recent progress in organic photovoltaics (OPVs) has been enabled by optimization of the energetic driving force for charge separation, and thus maximization of open-circuit voltage, using non-fullerene acceptor (NFA) materials. In spite of this, the carrier dynamics and relative energies of the key states controlling the photophysics of these systems are still under debate. Herein, we report an in-depth ultrafast spectroscopic study of a representative OPV system based on a polymer donor PffBT4T-2OD and a small-molecule NFA EH-IDTBR. Global analysis of the transient absorption data reveals efficient energy transfer between donor and acceptor molecules. The extracted kinetics suggest that slow (∼15 ps) generation of charge carriers is followed by significant geminate recombination. This contrasts with the "reference" PffBT4T-2OD:PC71BM system where bimolecular recombination dominates. Using temperature-dependent pump-push-photocurrent spectroscopy, we estimate the activation energy for the dissociation of bound charge-transfer states in PffBT4T-2OD:EH-IDTBR to be 100 ± 6 meV. We also observe an additional activation energy of 14 ± 7 meV, which we assign to the de-trapping of mobile carriers. This work provides a comprehensive picture of photophysics in a system representing new generation of OPV blends with a small driving force for charge separation.

Journal article

Gasparini N, Salleo A, McCulloch I, Baran Det al., 2019, The role of the third component in ternary organic solar cells, Nature Reviews Materials

© 2019, Springer Nature Limited. Ternary organic solar cells (TSCs) contain a single three-component photoactive layer with a wide absorption window, which is obtained without the need for multiple stacks. Subsequently, TSCs have attracted great interest in the photovoltaics field. Through careful selection of the three (or more) active components that form the photoactive layer, all photovoltaic parameters can be simultaneously enhanced within a TSC — a strategy that has resulted in record efficiencies for single-junction solar cells. In this Review, we outline key developments in TSCs, with a focus on the central role of the third component in achieving record efficiencies. We analyse the effects of the third component on the nanomorphology of the bulk heterojunction and the photovoltaic parameters of TSCs. Moreover, we discuss the charge-transfer and/or energy-transfer mechanisms and nanomorphology models that govern the operation of TSCs. We consider both polymer and small-molecule donors as well as fullerenes and recently developed non-fullerene acceptors. In addition, we summarize the recent success of TSCs in mitigating the stability issues of binary solar cells. Finally, we provide a perspective on the advantages of ternary blends and suggest design strategies for highly efficient and stable devices for commercial photovoltaics.

Journal article

Kang K, Schott S, Venkateshvaran D, Broch K, Schweicher G, Harkin D, Jellett C, Nielsen CB, McCulloch I, Sirringhaus Het al., 2019, Investigation of the thermoelectric response in conducting polymers doped by solid-state diffusion, MATERIALS TODAY PHYSICS, Vol: 8, Pages: 112-122, ISSN: 2542-5293

Journal article

Luke J, Speller EM, Wadsworth A, Wyatt MF, Dmiitrov S, Lee HKH, Li Z, Tsoi WC, McCulloch I, Bagnis D, Durrant JR, Kim J-Set al., 2019, Twist and degrade – Impact of molecular structure on the photostability of non-fullerene acceptors and their photovoltaic blends, Advanced Energy Materials, ISSN: 1614-6832

Non-fullerene acceptors (NFAs) dominate organic photovoltaic (OPV) research due to their promising efficiencies and stabilities. However, there is very little investigation into the molecular processes of degradation, which is critical to guiding design of novel NFAs for long-lived, commercially viable OPVs. Here we investigate the important role of molecular structure and conformation on NFA photostability in air by comparing structurally similar but conformationally different promising NFAs; planar O-IDTBR and non-planar O-IDFBR. We identify a three-phase degradation process: (i) initial photo-induced conformational change (i.e. torsion about the Core-BT dihedral), induced by non-covalent interactions with environmental molecules, (ii) followed by photo-oxidation and fragmentation, leading to chromophore bleaching and degradation product formation, and (iii) finally complete chromophore bleaching.Initial conformational change is a critical prerequisite for further degradation, providing fundamental understanding of the relative stability of IDTBR and IDFBR, where the alreadytwisted IDFBR is more prone to degradation. When blended with the donor polymer P3HT, both NFAs exhibit improved photostability whilst the photostability of the polymer itself is significantly reduced by the more miscible twisted NFA. Our findings elucidate the important role of NFA molecular structure on photostability of OPV systems, and provide vital insights into molecular design rules for intrinsically photostable NFAs.

Journal article

Savva A, Cendra C, Giugni A, Torre B, Surgailis J, Ohayon D, Giovannitti A, McCulloch I, Di Fabrizio E, Salleo A, Rivnay J, Inal Set al., 2019, Influence of Water on the Performance of Organic Electrochemical Transistors, CHEMISTRY OF MATERIALS, Vol: 31, Pages: 927-937, ISSN: 0897-4756

Journal article

Thiburce Q, Giovannitti A, McCulloch I, Campbell AJet al., 2019, Nanoscale ion-doped polymer transistors, Nano Letters, ISSN: 1530-6984

Organic transistors with submicron dimensions have been shown to deviate from the expected behaviour due to a variety of so-called 'short-channel' effects, resulting in nonlinear output characteristics and a lack of current saturation, considerably limiting their use. Here, using an electrochemically-doped polymer in which ions are dynamically injected and removed from the bulk of the semiconductor, we show that devices with nanoscale channel lengths, down to 50 nm, exhibit output curves with well-defined linear and saturation regimes. Additionally, they show very large on-currents on par with their microscale counterparts, large on-to-off ratios of 108, and record-high width-normalised transconductances above 10 S m-1. We believe this work paves the way for the fabrication of high-gain, high-current polymer integrated circuits such as sensor arrays operating at voltages below |1 V| and prepared using simple solution processing methods.

Journal article

Kiefer D, Kroon R, Hofmann AI, Sun H, Liu X, Giovannitti A, Stegerer D, Cano A, Hynynen J, Yu L, Zhang Y, Nai D, Harrelson TF, Sommer M, Moule AJ, Kemerink M, Marder SR, McCulloch I, Fahlman M, Fabiano S, Muller Cet al., 2019, Double doping of conjugated polymers with monomer molecular dopants, NATURE MATERIALS, Vol: 18, Pages: 149-+, ISSN: 1476-1122

Journal article

Cendra C, Giovannitti A, Savva A, Venkatraman V, McCulloch I, Salleo A, Inal S, Rivnay Jet al., 2019, Role of the Anion on the Transport and Structure of Organic Mixed Conductors, ADVANCED FUNCTIONAL MATERIALS, Vol: 29, ISSN: 1616-301X

Journal article

Cha H, Fish G, Luke J, Alraddadi A, Lee HH, Zhang W, Dong Y, Limbu S, Wadsworth A, Maria IP, Francàs L, Sou HL, Du T, Kim JS, 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, ISSN: 1614-6832

© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Here, it is investigated whether an energetic cascade between mixed and pure regions assists in suppressing recombination losses in non-fullerene acceptor (NFA)-based organic solar cells. The impact of polymer-NFA blend composition upon morphology, energetics, charge carrier recombination kinetics, and photocurrent properties are studied. By changing film composition, morphological structures are varied from consisting of highly intermixed polymer-NFA phases to consisting of both intermixed and pure phase. Cyclic voltammetry is employed to investigate the impact of blend morphology upon NFA lowest unoccupied molecular orbital (LUMO) level energetics. Transient absorption spectroscopy reveals the importance of an energetic cascade between mixed and pure phases in the electron–hole dynamics in order to well separate spatially localized electron–hole pairs. Raman spectroscopy is used to investigate the origin of energetic shift of NFA LUMO levels. It appears that the increase in NFA electron affinity in pure phases relative to mixed phases is correlated with a transition from a relatively planar backbone structure of NFA in pure, aggregated phases, to a more twisted structure in molecularly mixed phases. The studies focus on addressing whether aggregation-dependent acceptor LUMO level energetics are a general design requirement for both fullerene and NFAs, and quantifying the magnitude, origin, and impact of such energetic shifts upon device performance.

Journal article

Schott S, Chopra U, Lemaur V, Melnyk A, Olivier Y, Di Pietro R, Romanov I, Carey RL, Jiao X, Jellett C, Little M, Marks A, McNeill CR, McCulloch I, McNellis ER, Andrienko D, Beljonne D, Sinova J, Sirringhaus Het al., 2019, Polaron spin dynamics in high-mobility polymeric semiconductors, Nature Physics, ISSN: 1745-2473

© 2019, The Author(s), under exclusive licence to Springer Nature Limited. Polymeric semiconductors exhibit exceptionally long spin lifetimes, and recently observed micrometre spin diffusion lengths in conjugated polymers demonstrate the potential for organic spintronics devices. Weak spin–orbit and hyperfine interactions lie at the origin of their long spin lifetimes, but the coupling mechanism of a spin to its environment remains elusive. Here, we present a systematic study of polaron spin lifetimes in field-effect transistors with high-mobility conjugated polymers as an active layer. We demonstrate how spin relaxation is governed by the charges’ hopping motion at low temperatures, whereas an Elliott–Yafet-like relaxation due to a transient localization of the carrier wavefunctions is responsible for spin relaxation at high temperatures. In this regime, charge, spin and structural dynamics are intimately related and depend sensitively on the local conformation of polymer backbones and the crystalline packing of the polymer chains.

Journal article

Wadsworth A, Bristow H, Hamid Z, Babics M, Gasparini N, Boyle CW, Zhang W, Dong Y, Thorley KJ, Neophytou M, Ashraf RS, Durrant JR, Baran D, McCulloch Iet al., 2019, End Group Tuning in Acceptor–Donor–Acceptor Nonfullerene Small Molecules for High Fill Factor Organic Solar Cells, Advanced Functional Materials, ISSN: 1616-301X

© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim High fill factors have only recently become commonplace in nonfullerene-based organic solar cells, with the balance of charge carrier mobilities often cited as the contributing factor. Here an end-group modification to a commonly used nonfullerene acceptor (O-IDTBR) is reported, in which the rhodanine end groups are replaced with dicyano moieties, resulting in the acceptor O-IDTBCN. This new acceptor affords significant improvement in the fill factor (73%) and photocurrent (19.8 mA cm−2) in organic solar cells with the low bandgap polymer PTB7-Th. A narrowing of the bandgap, as a result of greater push–pull hybridization, allows complementary absorption to the donor and thus improved photon harvesting. Additionally, the measurement of charge carrier mobilities and lifetimes in both systems reveal that the PTB7-Th:O-IDTBCN blend possesses more balanced charge carrier mobilities, and longer lifetimes. Morphology studies reveal a slightly greater degree of molecular mixing of the O-IDTBCN when blended with PTB7-Th, despite the greater and more balanced charge carrier mobilities in this blend.

Journal article

Savva A, Ohayon D, Surgailis J, Paterson AF, Hidalgo TC, Chen X, Maria IP, Paulsen BD, Petty AJ, Rivnay J, McCulloch I, Inal Set al., 2019, Solvent Engineering for High-Performance n-Type Organic Electrochemical Transistors, Advanced Electronic Materials

© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Organic electrochemical transistors (OECTs) exhibit strong potential for various applications in bioelectronics, especially as miniaturized, point-of-care biosensors, because of their efficient transducing ability. To date, however, the majority of reported OECTs have relied on p-type (hole transporting) polymer mixed conductors, due to the limited number of n-type (electron transporting) materials suitable for operation in aqueous electrolytes, and the low performance of those which exist. It is shown that a simple solvent-engineering approach boosts the performance of OECTs comprising an n-type, naphthalenediimide-based copolymer in the channel. The addition of acetone, a rather bad solvent for the copolymer, in the chloroform-based polymer solution leads to a three-fold increase in OECT transconductance, as a result of the simultaneous increase in volumetric capacitance and electron mobility in the channel. The enhanced electrochemical activity of the polymer film allows high-performance glucose sensors with a detection limit of 10 × 10−6 m of glucose and a dynamic range of more than eight orders of magnitude. The approach proposed introduces a new tool for concurrently improving the conduction of ionic and electronic charge carriers in polymer mixed conductors, which can be utilized for a number of bioelectronic applications relying on efficient OECT operation.

Journal article

Moser M, Thorley KJ, Moruzzi F, Ponder JF, Maria IP, Giovannitti A, Inal S, McCulloch Iet al., 2019, Highly selective chromoionophores for ratiometric Na <sup>+</sup> sensing based on an oligoethyleneglycol bridged bithiophene detection unit, Journal of Materials Chemistry C, Vol: 7, Pages: 5359-5365, ISSN: 2050-7534

© 2019 The Royal Society of Chemistry. Rapid and efficient measurement of sodium ion concentrations will benefit future studies and healthcare due to the importance of sodium to many biological processes. Ratiometric optical probes, where light absorption wavelengths shift according to ion concentration, can be used as a quick measurement method. In contrast to the currently available UV absorbing probes, we have synthesised a series of sensors which absorb in different regions of the visible spectrum. In addition to measurement by conventional UV-Vis spectroscopy, this also enables analysis of sodium ion concentration from colorimetry, opening the door to faster and cheaper analysis. Finally, the optical properties of the dyes were well reproduced by computational methods, with and without the presence of sodium, enabling acceleration of design of future materials.

Journal article

Wadsworth A, Moser M, Marks A, Little M, Gasparini N, Brabec C, Baran D, McCulloch Iet al., Critical review of the molecular design progress in non-fullerene electron acceptors towards commercially viable organic solar cells, Chemical Society Reviews, ISSN: 1460-4744

Fullerenes have formed an integral part of high performance organic solar cells over the last 20 years, however their inherent limitations in terms of synthetic flexibility, cost and stability have acted as a motivation to develop replacements; the so-called non-fullerene electron acceptors. A rapid evolution of such materials has taken place over the last few years, yielding a number of promising candidates that can exceed the device performance of fullerenes and provide opportunities to improve upon the stability and processability of organic solar cells. In this review we explore the structure-property relationships of a library of non-fullerene acceptors, highlighting the important chemical modifications that have led to progress in the field and provide an outlook for future innovations in electron acceptors for use in organic photovoltaics.

Journal article

Hallani RK, Fallah Hamidabadi V, Huckaba AJ, Galliani G, Babaei A, La-Placa M-G, Bahari A, McCulloch I, Nazeeruddin MK, Sessolo M, Bolink HJet al., 2018, A new cross-linkable 9,10-diphenylanthracene derivative as a wide bandgap host for solution-processed organic light-emitting diodes, JOURNAL OF MATERIALS CHEMISTRY C, Vol: 6, Pages: 12948-12954, ISSN: 2050-7526

Journal article

Xie C, Heumueller T, Gruber W, Tang X, Classen A, Schuldes I, Bidwell M, Spaeth A, Fink RH, Unruh T, McCulloch I, Li N, Brabec CJet al., 2018, Overcoming efficiency and stability limits in water-processing nanoparticular organic photovoltaics by minimizing microstructure defects, NATURE COMMUNICATIONS, Vol: 9, ISSN: 2041-1723

Journal article

Moser M, Ponder JF, Wadsworth A, Giovannitti A, McCulloch Iet al., 2018, Materials in Organic Electrochemical Transistors for Bioelectronic Applications: Past, Present, and Future, Advanced Functional Materials, ISSN: 1616-301X

© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Organic electrochemical transistors are bioelectronic devices that exploit the coupled nature of ionic and electronic fluxes to achieve superior transducing abilities compared to conventional organic field effect transistors. In particular, the operation of organic electrochemical transistors relies on a channel material capable of conducting both ionic and electronic charge carriers to ensure bulk electrochemical doping. This review explores the various types of organic semiconductors that are employed as channel materials, with a particular focus on the past 5 years, during which the transducing abilities of organic electrochemical transistors have witnessed an almost tenfold increase. Specifically, the structure–property relationships of the various channel materials employed are investigated, highlighting how device performance can be related to functionality at the molecular level. Finally, an outlook on the field is provided, in particular toward the design guidelines of future materials and the challenges ahead in the field.

Journal article

Thorley KJ, McCulloch I, 2018, Why are S-F and S-O non-covalent interactions stabilising?, JOURNAL OF MATERIALS CHEMISTRY C, Vol: 6, Pages: 12413-12421, ISSN: 2050-7526

Journal article

Kosco J, Sachs M, Godin R, Kirkus M, Francas L, Bidwell M, Qureshi M, Anjum D, Durrant JR, McCulloch Iet al., 2018, The effect of residual palladium catalyst contamination on the photocatalytic hydrogen evolution activity of conjugated polymers, Advanced Energy Materials, Vol: 8, ISSN: 1614-6832

The effect of residual Pd on hydrogen evolution activity in conjugated polymer photocatalytic systems is systematically investigated using colloidal poly(9,9-dioctylfluorene-alt-benzothiadiazole) (F8BT) nanoparticles as a model system. Residual Pd, originating from the synthesis of F8BT via Pd catalyzed polycondensation polymerization, is observed in the form of homogeneously distributed Pd nanoparticles within the polymer. Residual Pd is essential for any hydrogen evolution to be observed from this polymer, and very low Pd concentrations (<40 ppm) are sufficient to have a significant effect on the hydrogen evolution reaction (HER) rate. The HER rate increases linearly with increasing Pd concentration from <1 ppm to approximately 100 ppm, at which point the rate begins to saturate. Transient absorption spectroscopy experiments support these conclusions, and suggest that residual Pd mediates electron transfer from the F8BT nanoparticles to protons in the aqueous medium.

Journal article

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