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307 results found
Wu J, Luke J, Lee HKH, et al., Tail state limited photocurrent collection of thick photoactive layers in organic solar cells, Nature Communications, 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.
Lami V, Weu A, Zhang J, et al., 2019, Visualizing the Vertical Energetic Landscape in Organic Photovoltaics, JOULE, Vol: 3, Pages: 2513-2534, ISSN: 2542-4351
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He Q, Shahid M, Wu J, et al., 2019, Fused Cyclopentadithienothiophene acceptor enables ultrahigh short‐circuit current and high efficiency >11% in as‐cast organic solar cells, Advanced Functional Materials, Vol: 29, Pages: 1-7, ISSN: 1616-301X
A new method to synthesize an electron‐rich building block cyclopentadithienothiophene (9H‐thieno‐[3,2‐b]thieno[2″,3″:4′,5′]thieno[2′,3′:3,4]cyclopenta[1,2‐d]thiophene, CDTT) via a facile aromatic extension strategy is reported. By combining CDTT with 1,1‐dicyanomethylene‐3‐indanone endgroups, a promising nonfullerene small molecule acceptor (CDTTIC) is prepared. As‐cast, single‐junction nonfullerene organic solar cells based on PFBDB‐T: CDTTIC blends exhibit very high short‐circuit currents up to 26.2 mA cm−2 in combination with power conversion efficiencies over 11% without any additional processing treatments. The high photocurrent results from the near‐infrared absorption of the CDTTIC acceptor and the well‐intermixed blend morphology of polymer donor PFBDB‐T and CDTTIC. This work demonstrates a useful fused ring extension strategy and promising solar cell results, indicating the great potential of the CDTT derivatives as electron‐rich building blocks for constructing high‐performance small molecule acceptors in organic solar cells.
Lin Y-H, Huang W, Pattanasattayavong P, et al., 2019, Deciphering photocarrier dynamics for tuneable high-performance perovskite-organic semiconductor heterojunction phototransistors, NATURE COMMUNICATIONS, Vol: 10, ISSN: 2041-1723
Jang S-Y, Kim I-B, Kang M, et al., 2019, Erratum: Diseleno[3,2-b:2',3'-d]selenophene-Containing High-Mobility Conjugated Polymer for Organic Field-Effect Transistors., Adv Sci (Weinh), Vol: 6, ISSN: 2198-3844
[This corrects the article DOI: 10.1002/advs.201900245.].
Panidi J, Kainth J, Paterson AF, et al., 2019, Introducing a nonvolatile N-type dopant drastically improves electron transport in polymer and small-molecule organic transistors, Advanced Functional Materials, Vol: 29, Pages: 1-10, ISSN: 1616-301X
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.
Musser AJ, Al-Hashimi M, Heeney M, et al., 2019, Heavy-atom effects on intramolecular singlet fission in a conjugated polymer, Journal of Chemical Physics, Vol: 151, ISSN: 0021-9606
A chief aim in singlet fission research is to develop new materials concepts for more efficient singlet fission. The typical approaches such as tuning π-overlap and charge-transfer interactions, enhancing delocalization, altering diradical character, or extending the conjugation length have profound effects simultaneously on the singlet and triplet energetics and the couplings between them. While these strategies have resulted in a handful of high-efficiency materials, the complex interplay of these factors makes systematic materials development challenging, and it would be useful to be able to selectively manipulate the properties and dynamics of just part of the singlet fission pathway. Here, we investigate the potential of heteroatom substitution as just such a selective tool. We explore the influence of heavy atoms within the main backbone of polythienylenevinylene and its selenophene and tellurophene derivatives. We find no significant effects on the prompt <300 fs intramolecular singlet fission dynamics but a clear heavy-atom effect on longer time scales.
Du T, Xu W, Daboczi M, et 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.
Choi HH, Paterson AF, Fusella MA, et al., Hall Effect in Polycrystalline Organic Semiconductors: The Effect of Grain Boundaries, ADVANCED FUNCTIONAL MATERIALS, ISSN: 1616-301X
Jang SY, Kim IB, Kang M, et al., 2019, Diseleno[3,2-b:2′,3′-d]selenophene-containing high-mobility conjugated polymer for organic field-effect transistors, Advanced Science, Vol: 6, ISSN: 2198-3844
KGaA, Weinheim The synthesis of a diseleno[3,2-b:2′,3′-d]selenophene (DSS) composed of three fused selenophenes is reported and it is used as a building block for the preparation of a high hole mobility conjugated polymer (PDSSTV). The polymer demonstrates strong intermolecular interactions even in solution, despite steric repulsion between the large Se atom in DSS and adjacent (C β )–H atoms which leads to a partially twisted confirmation PDSSTV. Nevertheless, 2D grazing incidence X-ray diffraction (2D-GIXD) analysis reveals that the polymer tends to align in a highly ordered edge-on orientation after thermal annealing. The polymer demonstrates promising performance in a field-effect transistor device with saturated hole mobility up to 2 cm 2 V −1 s −1 obtained under relatively low gate voltages of −30 V. The ultilization of a Se-containing fused aromatic system, therefore, appears to be a promising avenue for the development of high-performance conjugated polymers.
Green JP, Cha H, Shahid M, et al., 2019, Dithieno[3,2-b:2,3-d]arsole-containing conjugated polymers in organic photovoltaic devices, Dalton Transactions, Vol: 48, Pages: 6676-6679, ISSN: 1477-9234
Arsole-derived conjugated polymers are a relatively new class of materials in the field of organic electronics. Herein, we report the synthesis of two new donor polymers containing fused dithieno[3,2-b:2′,3′-d]arsole units and report their application in bulk heterojunction solar cells for the first time. Devices based upon blends with PC71BM display high open circuit voltages around 0.9 V and demonstrate power conversion efficiencies around 4%.
Paterson AF, Tsetseris L, Li R, et 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, Advanced Materials, Vol: 31, ISSN: 0935-9648
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.
Eisner F, Azzouzi M, Fei Z, et 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.
Eisner FD, Azzouzi M, Fei Z, et 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.
He Q, Shahid M, Panidi J, et 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.
Ye L, Xiong Y, Chen Z, et al., 2019, Sequential Deposition of Organic Films with Eco-Compatible Solvents Improves Performance and Enables Over 12%-Efficiency Nonfullerene Solar Cells., Adv Mater, Pages: e1808153-e1808153
Casting of a donor:acceptor bulk-heterojunction structure from a single ink has been the predominant fabrication method of organic photovoltaics (OPVs). Despite the success of such bulk heterojunctions, the task ofcontrolling the microstructure in a single casting process has been arduous and alternative approaches are desired. To achieve OPVs with a desirable microstructure, a facile and eco-compatible sequential deposition approach is demonstrated for polymer/small-molecule pairs. Using a nominally amorphous polymer as the model material, the profound influence of casting solvent is shown on the molecular ordering of the film, and thus the device performance and mesoscale morphology of sequentially deposited OPVs can be tuned. Static and in situ X-ray scattering indicate that applying (R)-(+)-limonene is able to greatly promote the molecular order of weakly crystalline polymers and form the largest domain spacing exclusively, which correlates well with the best efficiency of 12.5% in sequentially deposited devices. The sequentially cast device generally outperforms its control device based on traditional single-ink bulk-heterojunction structure. More crucially, a simple polymer:solvent interaction parameter χ is positively correlated with domain spacing in these sequentially deposited devices. These findings shed light on innovative approaches to rationally create environmentally friendly and highly efficient electronics.
Paterson AF, Mottram AD, Faber H, et 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.
Reichsöllner E, Creamer A, Cong S, et al., 2019, Fast and selective post-polymerization modification of conjugated polymers using dimethyldioxirane, Frontiers in Chemistry, Vol: 7, ISSN: 2296-2646
Modification of functional groups attached to conjugated polymer backbones can drastically alter the material properties. Oxidation of electron-donating thioalkyl substituents to electron-withdrawing sulfoxides or sulfones is a particularly effective modification. However, so far, this reaction has not been studied for the modification of conjugated polymers used in organic electronics. Crucial questions regarding selectivity and reaction time waited to be addressed. Here, we show that the reaction is highly selective and complete within just a few minutes when using dimethyldioxirane (DMDO) for the oxidation of thioalkyl substituents attached to the well-investigated conjugated polymers poly(9-(1-octylnonyl)carbazole-alt-4,7-dithienylbenzothiadiazole) (PCDTBT) and poly(9,9-dioctylfluorene-alt-benzothiadiazole) (F8BT). The selectivity was confirmed by comparison with polymers obtained from pre-oxidized monomers and by control experiments using related polymers without thioalkyl substituents. Using DMDO, the oxidation yields acetone as the only side-product, which reduces the work-up to mere evaporation of solvents and excessive reagent. Our results show that this oxidation is an exciting method for the preparation of electron-deficient conjugated polymers. It may even allow the preparation of electron acceptors for solar cells directly from the electron donors.
Sun G, Shahid M, Fei Z, et 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%.
Rimmele M, Ableidinger K, Marsh AV, et al., 2019, Thioalkyl- and Sulfone-Substituted Poly(p-Phenylene Vinylene)s, Polymer Chemistry, Vol: 10, Pages: 738-750, ISSN: 1759-9954
Poly(p-phenylene vinylene)s (PPVs) have been studied for decades, but research on this interesting class of conjugated polymers is far from being completed. New applications like in bioimaging keep emerging and even simple structural variations are still waiting to be explored. Surprisingly, not even dithioalkyl-substituted PPVs (S-PPVs) have been reported in the peer-reviewed literature, although the corresponding dialkoxy-substituted PPVs (O-PPVs) like MEH-PPV or MDMO-PPV are most frequently used and although thioalkyl substituents can improve the material properties significantly. We herein report the development of a highly efficient, scalable two-step synthesis of Gilch monomers for S-PPVs starting from low-cost 1,4-diiodobenzene. A low-temperature polymerization protocol has been developed for these monomers, affording high-molecular weight S-PPVs in excellent yields. The thermal, electrochemical, and photophysical properties of S-PPVs are reported to highlight the potential of these polymers. Furthermore, treatment with dimethyldioxirane is demonstrated to result in rapid conversion into sulfone-substituted PPVs (SO2-PPVs), introducing a route to high-molecular weight SO2-PPVs with exceptional stability and solid-state photoluminescence quantum yields of up to 0.46.
Reichsöllner E, Creamer A, Cong S, et al., 2019, Fast and selective post-polymerization modification of conjugated polymers using dimethyldioxirane.
Modification of functional groups attached to conjugated polymer backbones can drastically alter the material properties. Oxidation of electron-donating thioalkyl substituents to electron-withdrawing sulfoxides or sulfones is a particularly effective modification. However, so far, this reaction has not been studied for the modification of conjugated polymers used in organic electronics. Crucial questions regarding selectivity and reaction time waited to be addressed. Here, we show that the reaction is highly selective and complete within just a few minutes when using dimethyldioxirane (DMDO) for the oxidation of thioalkyl substituents attached to the well investigated conjugated polymers poly(9-(1-octylnonyl)carbazole-alt-4,7-dithienylbenzothiadiazole) (PCDTBT) and poly(9,9-dioctylfluorene-alt-benzothiadiazole) (F8BT). The selectivity was confirmed by comparison with polymers obtained from pre-oxidized monomers and by control experiments using related polymers without thioalkyl substituents. Using DMDO, the oxidation yields acetone as the only side-product, which reduces the work-up to mere evaporation of solvents and excessive reagent. Our results show that this oxidation is an exciting method for the preparation of electron-deficient conjugated polymers. It may even allow the preparation of electron acceptors for solar cells directly from the electron donors.
Krauspe P, Tsokkou D, Causa M, et al., 2018, Terahertz short-range mobilities in neat and intermixed regions of polymer: fullerene blends with controlled phase morphology, JOURNAL OF MATERIALS CHEMISTRY A, Vol: 6, Pages: 22301-22309, ISSN: 2050-7488
Rimmele M, Ableidinger K, Marsh A, et al., 2018, Thioalkyl- and Sulfone-Substituted Poly(p-Phenylene Vinylene)s, Publisher: Royal society of chemistry
Poly(p-phenylene vinylene)s (PPVs) have been studied for decades, but research on this interesting class of conjugated polymers is far from being completed. New applications like in bioimaging keep emerging and even simple structural variations are still waiting to be explored. Surprisingly, not even dithioalkyl-substituted PPVs (S-PPVs) have been reported in the peer-reviewed literature, although the corresponding dialkoxy-substituted PPVs (O-PPVs) like MEH-PPV or MDMO-PPV are most frequently used and although thioalkyl substituents can improve the material properties significantly. We herein report the development of a highly efficient, scalable two-step synthesis of Gilch monomers for S-PPVs starting from low-cost 1,4-diiodobenzene. A low-temperature polymerization protocol has been developed for these monomers, affording high-molecular weight S-PPVs in excellent yields. The thermal, electrochemical, and photophysical properties of S-PPVs are reported to highlight the potential of these polymers. Furthermore, treatment with dimethyldioxirane is demonstrated to result in rapid conversion into sulfone-substituted PPVs (SO<sub>2</sub>-PPVs), introducing a route to high-molecular weight SO<sub>2</sub>-PPVs with exceptional stability and solid-state photoluminescence quantum yields of up to 0.46.
Paterson AF, Lin Y-H, Mottram AD, et 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
Boufflet P, Bovo G, Occhi L, et 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.
Paterson AF, Singh S, Fallon KJ, et 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.
Rodriquez D, Kohl JG, Morel P, et al., 2018, Measurement of Cohesion and Adhesion of Semiconducting Polymers by Scratch Testing: Effect of Side-Chain Length and Degree of Polymerization, ACS MACRO LETTERS, Vol: 7, Pages: 1003-1009, ISSN: 2161-1653
Heeney MJ, Creamer A, Wood C, et 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.
Marsh AV, Cheetham NJ, Little M, et al., 2018, Carborane‐Induced Excimer Emission of Severely Twisted Bis‐ o ‐Carboranyl Chrysene, Angewandte Chemie, Vol: 130, Pages: 10800-10805, ISSN: 0044-8249
Heeney MJ, Stavrinou P, Anthony S, et al., 2018, Carborane induced excimer emission of severely twisted Bis-o-carboranyl chrysene, Angewandte Chemie, Vol: 57, Pages: 10640-10645, ISSN: 1521-3757
The synthesis of a highly twisted chrysene derivative incorporating two electron deficient o‐carboranyl groups is reported. The molecule exhibits a complex, excitation‐dependent photoluminescence, including aggregation‐induced emission (AIE) with good quantum efficiency and an exceptionally long singlet excited state lifetime. Through a combination of detailed optical studies and theoretical calculations, the excited state species are identified, including an unusual excimer induced by the presence of o‐carborane. This is the first time that o‐carborane has been shown to induce excimer formation ab initio, as well as the first observation of excimer emission by a chrysene‐based small molecule in solution. Bis‐o‐carboranyl chrysene is thus an initial member of a new family of o‐carboranyl phenacenes exhibiting a novel architecture for highly‐efficient multi‐luminescent fluorophores.
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