Imperial College London

ProfessorThomasAnthopoulos

Faculty of Natural SciencesDepartment of Physics

Visiting Professor
 
 
 
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Contact

 

+44 (0)20 7594 6669thomas.anthopoulos Website

 
 
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Assistant

 

Mrs Carolyn Dale +44 (0)20 7594 7579

 
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Location

 

1111Blackett LaboratorySouth Kensington Campus

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Summary

 

Publications

Publication Type
Year
to

315 results found

Paterson AF, Tsetseris L, Li R, Basu A, Faber H, Emwas A-H, Panidi J, Fei Z, Niazi MR, Anjum DH, Heeney M, Anthopoulos TDet al., 2019, Addition of the Lewis Acid Zn(C6 F5 )2 Enables Organic Transistors with a Maximum Hole Mobility in Excess of 20 cm2 V-1 s-1., Adv Mater

Incorporating the molecular organic Lewis acid tris(pentafluorophenyl)borane [B(C6 F5 )3 ] into organic semiconductors has shown remarkable promise in recent years for controlling the operating characteristics and performance of various opto/electronic devices, including, light-emitting diodes, solar cells, and organic thin-film transistors (OTFTs). Despite the demonstrated potential, however, to date most of the work has been limited to B(C6 F5 )3 with the latter serving as the prototypical air-stable molecular Lewis acid system. Herein, the use of bis(pentafluorophenyl)zinc [Zn(C6 F5 )2 ] is reported as an alternative Lewis acid additive in high-hole-mobility OTFTs based on small-molecule:polymer blends comprising 2,7-dioctyl[1]benzothieno [3,2-b][1]benzothiophene and indacenodithiophene-benzothiadiazole. Systematic analysis of the materials and device characteristics supports the hypothesis that Zn(C6 F5 )2 acts simultaneously as a p-dopant and a microstructure modifier. It is proposed that it is the combination of these synergistic effects that leads to OTFTs with a maximum hole mobility value of 21.5 cm2 V-1 s-1 . The work not only highlights Zn(C6 F5 )2 as a promising new additive for next-generation optoelectronic devices, but also opens up new avenues in the search for high-mobility organic semiconductors.

Journal article

Firdaus Y, Le Corre VM, Khan JI, Kan Z, Laquai F, Beaujuge PM, Anthopoulos TDet al., 2019, Key Parameters Requirements for Non-Fullerene-Based Organic Solar Cells with Power Conversion Efficiency > 20%, ADVANCED SCIENCE, Vol: 6, ISSN: 2198-3844

Journal article

Sun G, Shahid M, Fei Z, Xu S, Eisner FD, Anthopoulos TD, McLachlan MA, Heeney Met al., 2019, Highly-efficient semi-transparent organic solar cells utilising non-fullerene acceptors with optimised multilayer MoO3/Ag/MoO3 electrodes (vol 3, pg 450, 2019), MATERIALS CHEMISTRY FRONTIERS, Vol: 3, Pages: 955-955

Journal article

Eisner F, Azzouzi M, Fei Z, Hou X, Anthopoulos T, Dennis TJ, Heeney M, Nelson Jet al., 2019, Hybridization of local exciton and charge-transfer states reduces non-radiative voltage losses in organic solar cells, Journal of the American Chemical Society, Vol: 141, Pages: 6362-6374, ISSN: 1520-5126

A number of recent studies have shown that the nonradiative voltage losses in organic solar cells can be suppressed in systems with low energetic offsets between donor and acceptor molecular states, but the physical reasons underpinning this remain unclear. Here, we present a systematic study of 18 different donor/acceptor blends to determine the effect that energetic offset has on both radiative and nonradiative recombination of the charge-transfer (CT) state. We find that, for certain blends, low offsets result in hybridization between charge-transfer and lowest donor or acceptor exciton states, which leads to a strong suppression in the nonradiative voltage loss to values as low as 0.23 V associated with an increase in the luminescence of the CT state. Further, we extend a two-state CT-state recombination model to include the interaction between CT and first excited states, which allows us to explain the low nonradiative voltage losses as an increase in the effective CT to ground state oscillator strength due to the intensity borrowing mechanism. We show that low nonradiative voltage losses can be achieved in material combinations with a strong electronic coupling between CT and first excited states and where the lower band gap material has a high oscillator strength for transitions from the excited state to the ground state. Finally, from our model we propose that achieving very low nonradiative voltage losses may come at a cost of higher overall recombination rates, which may help to explain the generally lower FF and EQE of highly hybridized systems.

Journal article

Eisner FD, Azzouzi M, Fei Z, Hou X, Anthopoulos TD, Dennis TJS, Heeney M, Nelson Jet al., 2019, Hybridization of Local Exciton and Charge-Transfer States Reduces Nonradiative Voltage Losses in Organic Solar Cells., J Am Chem Soc

A number of recent studies have shown that the nonradiative voltage losses in organic solar cells can be suppressed in systems with low energetic offsets between donor and acceptor molecular states, but the physical reasons underpinning this remain unclear. Here, we present a systematic study of 18 different donor/acceptor blends to determine the effect that energetic offset has on both radiative and nonradiative recombination of the charge-transfer (CT) state. We find that, for certain blends, low offsets result in hybridization between charge-transfer and lowest donor or acceptor exciton states, which leads to a strong suppression in the nonradiative voltage loss to values as low as 0.23 V associated with an increase in the luminescence of the CT state. Further, we extend a two-state CT-state recombination model to include the interaction between CT and first excited states, which allows us to explain the low nonradiative voltage losses as an increase in the effective CT to ground state oscillator strength due to the intensity borrowing mechanism. We show that low nonradiative voltage losses can be achieved in material combinations with a strong electronic coupling between CT and first excited states and where the lower band gap material has a high oscillator strength for transitions from the excited state to the ground state. Finally, from our model we propose that achieving very low nonradiative voltage losses may come at a cost of higher overall recombination rates, which may help to explain the generally lower FF and EQE of highly hybridized systems.

Journal article

Chen M, Yengel E, Zhang J, Zhu C, He X, Zhang C, Huang JK, Hedhili MN, Anthopoulos T, Zhang Xet al., 2019, One-step growth of reduced graphene oxide on arbitrary substrates, Carbon, Vol: 144, Pages: 457-463, ISSN: 0008-6223

© 2018 Elsevier Ltd Reduced graphene oxide (rGO) has inherited the outstanding electronic, optical, thermal and mechanical properties of graphene to a large extent, while maintaining sufficient chemically active sites. Therefore, it has attracted a great deal of research attention in the fields of energy storage, electronics, photonics, catalysis, environmental engineering, etc. Currently, the most popular way to prepare rGO is to reduce graphene oxide, which is obtained by modified Hummer methods using tedious treatments in a harsh environment, to rGO flakes. Industrial applications demand advanced preparation methods that can mass produce highly uniform rGO sheets on arbitrary substrates. In this work, a one-step growth process is introduced that utilizes cellulose acetate as a precursor, without any catalysts, to produce uniform ultrathin rGO films on various substrates and free-standing rGO powders. Systematic spectroscopic and microscopic studies on the resulting rGO are performed. Prototypes of electronic and optoelectronic devices, such as field effect transistors (FETs), photodetectors, and humidity sensors, are fabricated and tested, demonstrating the intriguing applications of our rGO materials across a wide range of fields.

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, 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

Paterson AF, Mottram AD, Faber H, Niazi MR, Fei Z, Heeney M, Anthopoulos TDet al., 2019, Impact of the gate dielectric on contact resistance in high-mobility organic transistors, Advanced Electronic Materials, ISSN: 2199-160X

The impact of the gate dielectric on contact resistance in organic thin-film transistors (OTFTs) is investigated using electrical characterization, bias-stress stability measurements, and bandgap density of states (DOS) analysis. Two similar dielectric materials, namely Cytop and poly[4,5-difluoro-2,2-bis(trifluoromethyl)-1,3-dioxole-co-tetrafluoroethylene] (Teflon AF2400), are tested in top-gate bottom-contact OTFTs. The contact resistance of Cytop-based OTFTs is found to be greater than that of the AF2400-based devices, even though the metal/OSC interface remains identical in both systems. The Cytop devices are also found to perform worse in bias-stress stability tests which, along with the DOS calculations, suggests that charge trapping at the OSC/dielectric interface is more prevalent with Cytop than AF2400. This increased charge trapping at the Cytop OSC/dielectric interface appears to be associated with the higher contact resistance in Cytop OTFTs. Differences in the molecular structure between Cytop and AF2400 and the large difference in the glass transition temperature of the two polymers may be responsible for the observed difference in the transistor performance. Overall, this study highlights the importance of the gate dielectric material in the quest for better performing OTFTs and integrated circuits.

Journal article

Sun G, Shahid M, Fei Z, Xu S, Eisner FD, Anthopolous TD, McLachlan MA, Heeney Met al., 2019, Highly-efficient semi-transparent organic solar cells utilising non-fullerene acceptors with optimised multilayer MoO3/Ag/MoO3 electrodes, Materials Chemistry Frontiers, Vol: 3, Pages: 450-455, ISSN: 2052-1537

We report the optimisation of a semi-transparent solar cell based on a blend of a recently reported high performance donor polymer (PFBDB-T) with a non-fullerene acceptor derivative (C8-ITIC). The performance is shown to strongly depend on the nature of the semi-transparent electrode, and we report the optimal fabrication conditions for a multilayer MoO3/Ag/MoO3 electrode. The effect of deposition rate and layer thickness of both the Ag and the outer MoO3 on transparency and sheet resistance is investigated, and is shown to have a significant impact on the overall device performance. The optimised PFBDB-T:C8-ITIC based devices exhibit an average power conversion efficiency (PCE) of 9.2% with an average visible transmittance (AVT) of 22%.

Journal article

Twyman N, Tetzner K, Anthopoulos T, Payne D, Regoutz Aet al., Rapid photonic curing of solution-processed In2O3 layers on flexible substrates, Applied Surface Science, ISSN: 0169-4332

In2O3 is one of the most important semiconducting metal oxides primarily because of its wide band gap, high electron mobility and processing versatility. To this end, high-quality thin films of In2O3 can be prepared using scalable and inexpensive solution-based deposition methods, hence making it attractive for application in a number of emerging electronic applications. However, traditional solution processing often requires high temperature and lengthy annealing steps, making it impossible to use in combination with temperature-sensitive plastic substrates, which would be desired for numerous emerging flexible device applications. Here, rapid photonic curing of In2O3 layers is explored as an alternative to thermal annealing. Oxide thin films are successfully prepared on a range of substrates, including glass, polyimide, and polyethylene naphthalate. The effect of substrate and post-processing treatment on the morphology, surface chemistry, and electronic properties is investigated by atomic force microscopy and X-ray photoelectron spectroscopy. Systematic trends are identified, particularly in the degree of conversion of the precursor and its influence on the electronic structure.

Journal article

Karuthedath S, Gorenflot J, Firdaus Y, Sit W-Y, Eisner F, Seitkhan A, Ravva MK, Anthopoulos TD, Laquai Fet al., 2019, Charge and Triplet Exciton Generation in Neat PC70BM Films and Hybrid CuSCN:PC70BM Solar Cells, ADVANCED ENERGY MATERIALS, Vol: 9, ISSN: 1614-6832

Journal article

Barrit D, Cheng P, Tang MC, Wang K, Dang H, Smilgies DM, Liu S, Anthopoulos TD, Zhao K, Amassian Aet al., 2019, Impact of the Solvation State of Lead Iodide on Its Two-Step Conversion to MAPbI <inf>3</inf> : An In Situ Investigation, Advanced Functional Materials, ISSN: 1616-301X

© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Producing high efficiency solar cells without high-temperature processing or use of additives still remains a challenge with the two-step process. Here, the solution processing of MAPbI 3 from PbI 2 films in N,N-dimethylformamide (DMF) is investigated. In-situ grazing incidence wide-angle X-ray scattering (GIWAXS) measurements reveal a sol–gel process involving three PbI 2 -DMF solvate complexes—disordered (P 0 ) and ordered (P 1 , P 2 )—prior to PbI 2 formation. When the appropriate solvated state of PbI 2 is exposed to MAI (methylammonium Iodide), it can lead to rapid and complete room temperature conversion into MAPbI 3 with higher quality films and improved solar cell performance. Complementary in-situ optical reflectance, absorbance, and quartz crystal microbalance with dissipation (QCM-D) measurements show that dry PbI 2 can take up only one third of the MAI taken up by the solvated-crystalline P 2 phase of PbI 2 , requiring additional annealing and yet still underperforming. The perovskite solar cells fabricated from the ordered P 2 precursor show higher power conversion efficiency (PCE) and reproducibility than devices fabricated from other cases. The average PCE of the solar cells is greatly improved from 13.2(±0.53)% (from annealed PbI 2 ) to 15.7(±0.35)% (from P 2 ) reaching up to 16.2%. This work demonstrates the importance of controlling the solvation of PbI 2 as an effective strategy for the growth of high-quality perovskite films and their application in high efficiency and reproducible solar cells.

Journal article

Georgiadou DG, Lin YH, Lim J, Ratnasingham S, McLachlan MA, Snaith HJ, Anthopoulos TDet al., 2019, High Responsivity and Response Speed Single-Layer Mixed-Cation Lead Mixed-Halide Perovskite Photodetectors Based on Nanogap Electrodes Manufactured on Large-Area Rigid and Flexible Substrates, Advanced Functional Materials, ISSN: 1616-301X

© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Mixed-cation lead mixed-halide perovskites are employed as the photoactive material in single-layer solution-processed photodetectors fabricated with coplanar asymmetric nanogap Al–Au and indium tin oxide–Al electrodes. The nanogap electrodes, bearing an interelectrode distance of ≈10 nm, are patterned via adhesion lithography, a simple, low-cost, and high-throughput technique. Different electrode shapes and sizes are demonstrated on glass and flexible plastic substrates, effectively engineering the device architecture, and, along with perovskite film and material optimization, paving the way toward devices with tunable operational characteristics. The optimized coplanar nanogap junction perovskite photodetectors show responsivities up to 33 A W −1 , specific detectivity on the order of 10 11 Jones, and response times below 260 ns, while retaining a low dark current (0.3 nA) under −2 V reverse bias. These values outperform the vast majority of perovskite photodetectors reported so far, while avoiding the complicated fabrication steps involved in conventional multilayer device structures. This work highlights the promising potential of the proposed asymmetric nanogap electrode architecture for application in the field of flexible optoelectronics.

Journal article

Chaudhry MU, Wang N, Tetzner K, Seitkhan A, Miao Y, Sun Y, Petty MC, Anthopoulos TD, Wang J, Bradley DDCet al., 2019, Light-Emitting Transistors Based on Solution-Processed Heterostructures of Self-Organized Multiple-Quantum-Well Perovskite and Metal-Oxide Semiconductors, Advanced Electronic Materials

© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Solution-processed hybrid organic–inorganic perovskite semiconductors have demonstrated remarkable performance for both photovoltaic and light-emitting-diode applications in recent years, launching a new field of condensed matter physics. However, their use in other emerging optoelectronic applications, such as light-emitting field-effect transistors (LEFETs) has been surprisingly limited, wth only a few low-performance devices reported. The development of hybrid LEFETs consisting of a solution-processed self-organized multiple-quantum-well lead iodide perovskite layer grown onto an electron-transporting In 2 O 3 /ZnO heterojunction channel is reported. The multilayer transistors offer bifunctional characteristics, namely, transistor function with high electron mobility (>20 cm 2 V −1 s −1 ) and a large current on/off ratio (>10 6 ), combined with near infrared light emission (λ max = 783 nm) and a promising external quantum efficiency (≈0.2% at 18 cd m −2 ). A further interesting feature of these hybrid LEFETs, in comparison to previously reported structures, is their highly uniform and stable emission characteristics, which make them attractive for smart-pixel-format display applications.

Journal article

Wang K, Neophytou M, Aydin E, Wang M, Laurent T, Harrison GT, Liu J, Liu W, De Bastiani M, Khan JI, Anthopoulos TD, Laquai F, De Wolf Set al., 2019, Triarylphosphine Oxide as Cathode Interfacial Material for Inverted Perovskite Solar Cells, Advanced Materials Interfaces

© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Metal halide perovskite solar cells (PSCs) in the inverted planar p-i-n configuration often employ phenyl-C61-butyric acid methyl ester (PC 61 BM) as electron transport layer, onto which Ag is deposited as outer electrode. However, the energy offset between PC 61 BM and Ag imposes an energy barrier for electron extraction. In this work, to improve the contact quality of this stack, a small organic molecule (2-(1,10-phenanthrolin-3-yl)naphth-6-yl)diphenylphosphine oxide (DPO) as a cathode interfacial material (CIM), inserted between PC 61 BM and Ag, is introduced. In devices with the indium tin oxide (ITO)/NiO x /methylammonium lead iodide (MAPbI 3 )/PC 61 BM/CIM/Ag configuration, it is found that this results in fill factor (FF) and short-circuit current density values (J SC ) that are up to ≈34% and ≈1 mA cm −2 higher, respectively, compared to DPO-free devices. Inserting additional thin ZnO nanoparticle layers further improves the contact quality, leading to a power conversion efficiency of 18.2%. Semitransparent PSCs, utilizing DPO as an interlayer buffer layer are also realised. Resultant devices exhibit improved performance compared to DPO-free devices. This proves that DPO withstands the sputtering of ITO, and may thus find application in perovskite-based tandem devices. It is concluded that DPO acts as an excellent cathode modifier, opening new device-engineering opportunities for p-i-n PSCs, especially in their semitransparent implementation.

Journal article

Panidi J, Kainth J, Paterson AF, Wang S, Tsetseris L, Emwas AH, McLachlan MA, Heeney M, Anthopoulos TDet al., 2019, Introducing a Nonvolatile N-Type Dopant Drastically Improves Electron Transport in Polymer and Small-Molecule Organic Transistors, Advanced Functional Materials, ISSN: 1616-301X

© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Molecular doping is a powerful yet challenging technique for enhancing charge transport in organic semiconductors (OSCs). While there is a wealth of research on p-type dopants, work on their n-type counterparts is comparatively limited. Here, reported is the previously unexplored n-dopant (12a,18a)-5,6,12,12a,13,18,18a,19-octahydro-5,6-dimethyl- 13,18[1′,2′]-benzenobisbenzimidazo [1,2-b:2′,1′-d]benzo[i][2.5]benzodiazo-cine potassium triflate adduct (DMBI-BDZC) and its application in organic thin-film transistors (OTFTs). Two different high electron mobility OSCs, namely, the polymer poly[[N,N′-bis(2-octyldodecyl)-naphthalene-1,4,5,8- bis(dicarboximide)-2,6-diyl]-alt-5,5′-(2′-bithiophene)] and a small-molecule naphthalene diimides fused with 2-(1,3-dithiol-2-ylidene)malononitrile groups (NDI-DTYM2) are used to study the effectiveness of DMBI-BDZC as a n-dopant. N-doping of both semiconductors results in OTFTs with improved electron mobility (up to 1.1 cm2 V−1 s−1), reduced threshold voltage and lower contact resistance. The impact of DMBI-BDZC incorporation is particularly evident in the temperature dependence of the electron transport, where a significant reduction in the activation energy due to trap deactivation is observed. Electron paramagnetic resonance measurements support the n-doping activity of DMBI-BDZC in both semiconductors. This finding is corroborated by density functional theory calculations, which highlights ground-state electron transfer as the main doping mechanism. The work highlights DMBI-BDZC as a promising n-type molecular dopant for OSCs and its application in OTFTs, solar cells, photodetectors, and thermoelectrics.

Journal article

Paterson AF, Anthopoulos TD, 2018, Enabling thin-film transistor technologies and the device metrics that matter, Nature Communications, Vol: 9, ISSN: 2041-1723

The field-effect transistor kickstarted the digital revolution that propelled our society into the information age. One member of the now large family of field-effect devices is the thin-film transistor (TFT), best known for its enabling role in modern flat-panel displays. TFTs can be used in all sorts of innovative applications because of the broad variety of materials they can be made from, which give them diverse electrical and mechanical characteristics. To successfully utilize TFT technologies in a variety of rapidly emerging applications, such as flexible, stretchable and transparent large-area microelectronics, there are a number of metrics that matter.

Journal article

Paterson AF, Lin Y-H, Mottram AD, Fei Z, Niazi MR, Kirmani AR, Amassian A, Solomeshch O, Tessler N, Heeney M, Anthopoulos TDet al., 2018, The Impact of Molecular p-Doping on Charge Transport in High-Mobility Small-Molecule/Polymer Blend Organic Transistors, ADVANCED ELECTRONIC MATERIALS, Vol: 4, ISSN: 2199-160X

Journal article

Costa JC, Pouryazdan A, Panidi J, Anthopoulos T, Liedke MO, Schneider C, Wagner A, Munzenrieder Net al., 2018, Low temperature and radiation stability of flexible IGZO TFTs and their suitability for space applications, Pages: 98-101, ISSN: 1930-8876

© 2018 IEEE. In this paper, Low Earth Orbit radiation and temperature conditions are mimicked to investigate the suitability of flexible Indium-Gallium-Zinc-Oxide transistors for lightweight space-wearables. Such wearable devices could be incorporated into spacesuits as unobtrusive sensors such as radiation detectors or physiological monitors. Due to the harsh environment to which these space-wearables would be exposed, they have to be able to withstand high radiation doses and low temperatures. For this reason, the impacts of high energetic electron irradiation with fluences up to 10 12 e - /cm 2 and low operating temperatures down to 78 K, are investigated. This simulates 278 h in a Low Earth Orbit. The threshold voltage and mobility of transistors that were exposed to e-irradiation are found to shift by +0.09 0.05 V and-0.6 0.5 cm 2 V -1 s -1 . Subsequent low temperature exposure resulted in additional shifts of +0.38V and-5.95 cm 2 V -1 s -1 for the same parameters. These values are larger than the ones obtained from non-irradiated reference samples. If this is considered during the systems' design, these devices can be used to unobtrusively integrate sensor systems into space-suits.

Conference paper

Boufflet P, Bovo G, Occhi L, Fei Z, Han Y, Anthopoulos T, Yuan H, Heeney MJet al., 2018, The influence of backbone fluorination on the dielectric constant of conjugated polythiophenes, Advanced Electronic Materials, Vol: 4, ISSN: 2199-160X

The ability to modify or enhance the dielectric constant of semiconducting polymers can prove valuable for a range of optoelectronic and microelectronic applications. In the case of organic photovoltaics, increasing the dielectric constant of the active layer has often been suggested as a method to control charge generation, recombination dynamics, and ultimately, the power conversion efficiencies. In this contribution, the impact that the degree and pattern of fluorination has on the dielectric constant of poly(3-octylthiophene) (P3OT), a more soluble analogue of the widely studied conjugated material poly(3-hexylthiophene), is explored. P3OT and its backbone-fluorinated analogue, F-P3OT, are compared along with a block and alternating copolymer version of these materials. It is found that the dielectric constant of the polymer thin films increases as the degree of backbone fluorination increases, in a trend consistent with density functional theory calculations of the dipole moment.

Journal article

Wyatt-Moon G, Georgiadou DG, Zoladek-Lemanczyk A, Castro FA, Anthopoulos TDet al., 2018, Flexible nanogap polymer light-emitting diodes fabricated via adhesion lithography (a-Lith), Journal of Physics: Materials, Vol: 1, ISSN: 2515-7639

We report the development of coplanar green colour organic light-emitting diodes (OLEDs) based on asymmetric nanogap electrodes fabricated on different substrates including glass and plastic. Using adhesion lithography (a-Lith) we pattern Al and Au layers acting as the cathode and anode electrodes, respectively, separated by an inter-electrode distance of <15 nm with an aspect ratio of up to 106. Spin-coating the organic light-emitting polymer poly(9,9-dioctylfluorene-alt-bithiophene) (F8T2) on top of the asymmetric Al–Au nanogap electrodes results in green light-emitting nanogap OLEDs with promising operating characteristics. We show that the scaling of the OLED's width from 4 to 200 mm can substantially improve the light output of the device without any adverse effects on the manufacturing yield. Furthermore, it is found that the light-emitting properties in the nanogap area differ from the bulk organic film, an effect attributed to confinement of the conjugated polymer chains in the nanogap channel. These results render a-Lith particularly attractive for low cost facile fabrication of nanoscale light-emitting sources and arrays on different substrates of arbitrary size.

Journal article

Xu Y, Ji D, Song H, Zhang N, Hu Y, Anthopoulos TD, Di Fabrizio EM, Xiao S, Gan Qet al., 2018, Light-Matter Interaction within Extreme Dimensions: From Nanomanufacturing to Applications, ADVANCED OPTICAL MATERIALS, Vol: 6, ISSN: 2195-1071

Journal article

Paterson AF, Singh S, Fallon KJ, Hodsden T, Han Y, Schroeder BC, Bronstein H, Heeney M, McCulloch I, Anthopoulos TDet al., 2018, Recent progress in high-mobility organic transistors: a reality check, Advanced Materials, Vol: 30, ISSN: 0935-9648

Over the past three decades, significant research efforts have focused on improving the charge carrier mobility of organic thin‐film transistors (OTFTs). In recent years, a commonly observed nonlinearity in OTFT current–voltage characteristics, known as the “kink” or “double slope,” has led to widespread mobility overestimations, contaminating the relevant literature. Here, published data from the past 30 years is reviewed to uncover the extent of the field‐effect mobility hype and identify the progress that has actually been achieved in the field of OTFTs. Present carrier‐mobility‐related challenges are identified, finding that reliable hole and electron mobility values of 20 and 10 cm2 V−1 s−1, respectively, have yet to be achieved. Based on the analysis, the literature is then reviewed to summarize the concepts behind the success of high‐performance p‐type polymers, along with the latest understanding of the design criteria that will enable further mobility enhancement in n‐type polymers and small molecules, and the reasons why high carrier mobility values have been consistently produced from small molecule/polymer blend semiconductors. Overall, this review brings together important information that aids reliable OTFT data analysis, while providing guidelines for the development of next‐generation organic semiconductors.

Journal article

Wahyudi W, Cao Z, Kumar P, Li M, Wu Y, Hedhili MN, Anthopoulos TD, Cavallo L, Li L-J, Ming Jet al., 2018, Phase Inversion Strategy to Flexible Freestanding Electrode: Critical Coupling of Binders and Electrolytes for High Performance Li-S Battery, ADVANCED FUNCTIONAL MATERIALS, Vol: 28, ISSN: 1616-301X

Journal article

Heeney MJ, Creamer A, Wood C, Howes P, Casey A, Cong S, Marsh A, Godin R, Panidi J, Anthopoulos T, Burgess C, Wu T, Fei Z, McLachlan M, Stevens Met al., 2018, Post-polymerisation functionalisation of conjugated polymer backbones and its application in multi-functional emissive nanoparticles, Nature Communications, Vol: 9, ISSN: 2041-1723

Backbone functionalisation of conjugated polymers is crucial to their performance in many applications, from electronic displays to nanoparticle biosensors, yet there are limited approaches to introduce functionality. To address this challenge we have developed a method for the direct modification of the aromatic backbone of a conjugated polymer, post-polymerisation. This is achieved via a quantitative nucleophilic aromatic substitution (SNAr) reaction on a range of fluorinated electron deficient comonomers. The method allows for facile tuning of the physical and optoelectronic properties within a batch of consistent molecular weight and dispersity. It also enables the introduction of multiple different functional groups onto the polymer backbone in a controlled manner. To demonstrate the versatility of this reaction, we designed and synthesised a range of emissive poly(9,9-dioctylfluorene-alt-benzothiadiazole) (F8BT) based polymers for the creation of mono and multifunctional semiconducting polymer nanoparticles (SPNs) capable of two orthogonal bioconjugation reactions on the same surface.

Journal article

Firdaus Y, Seitkhan A, Eisner F, Sit W-Y, Kan Z, Wehbe N, Balawi AH, Yengel E, Karuthedath S, Laquai F, Anthopoulos TDet al., 2018, Charge Photogeneration and Recombination in Mesostructured CuSCN-Nanowire/PC70BM Solar Cells, SOLAR RRL, Vol: 2, ISSN: 2367-198X

Journal article

Wijeyasinghe N, Eisner F, Tsetseris L, Lin Y-H, Seitkhan A, Li J, Yan F, Solomeshch O, Tessler N, Patsalas P, Anthopoulos TDet al., 2018, p-Doping of Copper(I) Thiocyanate (CuSCN) Hole-Transport Layers for High-Performance Transistors and Organic Solar Cells, ADVANCED FUNCTIONAL MATERIALS, Vol: 28, ISSN: 1616-301X

Journal article

Eisner F, Seitkhan A, Han Y, Khim D, Yengel E, Kirmani AR, Xu J, de Arquer FPG, Sargent EH, Amassian A, Fei Z, Heeney M, Anthopoulos TDet al., 2018, Solution-processed In2O3/ZnO heterojunction electron transport layers for efficient organic bulk heterojunction and inorganic colloidal quantum-dot solar cells, Solar RRL, Vol: 2, ISSN: 2367-198X

We report the development of a solution‐processed In2O3/ZnO heterojunction electron transport layer (ETL) and its application in high efficiency organic bulk‐heterojunction (BHJ) and inorganic colloidal quantum dot (CQD) solar cells. Study of the electrical properties of this low‐dimensional oxide heterostructure via field‐effect measurements reveals that electron transport along the heterointerface is enhanced by more than a tenfold when compared to the individual single‐layer oxides. Use of the heterojunction as the ETL in organic BHJ photovoltaics is found to consistently improve the cell's performance due to the smoothening of the ZnO surface, increased electron mobility and a noticeable reduction in the cathode's work function, leading to a decrease in the cells’ series resistance and a higher fill factor (FF). Specifically, non‐fullerene based organic BHJ solar cells based on In2O3/ZnO ETLs exhibit very high power conversion efficiencies (PCE) of up to 12.8%, and high FFs of over 70%. The bilayer ETL concept is further extended to inorganic lead‐sulphide CQD solar cells. Resulting devices exhibit excellent performance with a maximum PCE of 8.2% and a FF of 56.8%. The present results highlight the potential of multilayer oxides as novel ETL systems and lay the foundation for future developments.

Journal article

Choi HH, Rodionov YI, Paterson AF, Panidi J, Saranin D, Kharlamov N, Didenko SI, Anthopoulos TD, Cho K, Podzorov Vet al., 2018, Accurate Extraction of Charge Carrier Mobility in 4-Probe Field-Effect Transistors, ADVANCED FUNCTIONAL MATERIALS, Vol: 28, ISSN: 1616-301X

Journal article

Semple J, Georgiadou DG, Wyatt-Moon G, Yoon M, Seitkhan A, Yengel E, Rossbauer S, Bottacchi F, McLachlan MA, Bradley DDC, Anthopoulos TDet al., 2018, Large-area plastic nanogap electronics enabled by adhesion lithography, npj Flexible Electronics, Vol: 2, ISSN: 2397-4621

Large-area manufacturing of flexible nanoscale electronics has long been sought by the printed electronics industry. However, the lack of a robust, reliable, high throughput and low-cost technique that is capable of delivering high-performance functional devices has hitherto hindered commercial exploitation. Herein we report on the extensive range of capabilities presented by adhesion lithography (a-Lith), an innovative patterning technique for the fabrication of coplanar nanogap electrodes with arbitrarily large aspect ratio. We use this technique to fabricate a plethora of nanoscale electronic devices based on symmetric and asymmetric coplanar electrodes separated by a nanogap < 15 nm. We show that functional devices including self-aligned-gate transistors, radio frequency diodes and rectifying circuits, multi-colour organic light-emitting nanodiodes and multilevel non-volatile memory devices, can be fabricated in a facile manner with minimum process complexity on a range of substrates. The compatibility of the formed nanogap electrodes with a wide range of solution processable semiconductors and substrate materials renders a-Lith highly attractive for the manufacturing of large-area nanoscale opto/electronics on arbitrary size and shape substrates.

Journal article

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