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  • Journal article
    Cui J, Daboczi M, Regue M, Chin Y, Pagano K, Zhang J, Isaacs MA, Kerherve G, Mornto A, West J, Gimenez S, Kim J, Eslava Set al., 2022,

    2D bismuthene as a functional interlayer between BiVO4 and NiFeOOH for enhanced oxygen-evolution photoanodes

    , Advanced Functional Materials, Vol: 32, Pages: 1-12, ISSN: 1616-301X

    BiVO4 has attracted wide attention for oxygen-evolution photoanodes in water-splitting photoelectrochemical devices. However, its performance is hampered by electron-hole recombination at surface states. Herein, partially oxidized two-dimensional (2D) bismuthene is developed as an effective, stable, functional interlayer between BiVO4 and the archetypal NiFeOOH co-catalyst. Comprehensive (photo)electrochemical and surface photovoltage characterizations show that NiFeOOH can effectively increase the lifetime of photogenerated holes by passivating hole trap states of BiVO4; however, it is limited in influencing electron trap states related to oxygen vacancies (VO). Loading bismuthene on BiVO4 photoanodes increases the density of VO that are beneficial for the oxygen evolution reaction via the formation of oxy/hydroxyl-based water oxidation intermediates at the surface. Moreover, bismuthene increases interfacial band bending and fills the VO-related electron traps, leading to more efficient charge extraction. With the synergistic interaction of bismuthene and NiFeOOH on BiVO4, this composite photoanode achieves a 5.8-fold increase in photocurrent compared to bare BiVO4 reaching a stable 3.4 (±0.2) mA cm–2 at a low bias of +0.8 VRHE or 4.7(±0.2) mA cm–2 at +1.23 VRHE. The use of 2D bismuthene as functional interlayer provides a new strategy to enhance the performance of photoanodes.

  • Journal article
    Tan E, Kim J, Stewart K, Pitsalidis C, Kwon S, Siemons N, Kim J, Jiang Y, Frost JM, Pearce D, Tyrrell JE, Nelson J, Owens RM, Kim Y-H, Kim J-Set al., 2022,

    The role of long-alkyl-group spacers in glycolated copolymers for high performance organic electrochemical transistors

    , Advanced Materials, Vol: 34, ISSN: 0935-9648

    Semiconducting polymers with oligoethylene glycol sidechains have attracted strong research interest for organic electrochemical transistor (OECT) applications. However, key molecular design rules for high-performance OECTs via efficient mixed electronic/ionic charge transport are still unclear. Herein, we synthesize and characterize new glycolated copolymers (gDPP-TTT and gDPP-TTVTT) with diketopyrrolopyrrole (DPP) acceptor and thiophene-based (TTT or TTVTT) donor units for accumulation mode OECTs, where a long-alkyl-group (C12 ) attached to DPP unit acts as a spacer distancing the oligoethylene glycol from the polymer backbone. gDPP-TTVTT shows the highest OECT transconductance (61.9 S cm-1 ) and high operational stability, compared to gDPP-TTT and their alkylated counterparts. Surprisingly, gDPP-TTVTT also shows high electronic charge mobility in field-effect transistor, suggesting efficient ion injection/diffusion without hindering its efficient electronic charge transport. The elongated donor unit (TTVTT) facilitates the hole polaron formation more localized to the donor unit, leading to faster and easier polaron formation with less impact on polymer structure during OECT operation, as opposed to the TTT unit. This is supported by molecular dynamics (MD) simulation. We conclude that these simultaneously high electronic and ionic charge transport properties are achieved due to the long-alkyl-group spacer in amphipathic sidechains, providing an important molecular design rule for glycolated copolymers. This article is protected by copyright. All rights reserved.

  • Journal article
    Labanti C, Wu J, Shin J, Limbu S, Yun S, Fang F, Park SY, Heo C-J, Lim Y, Choi T, Kim H-J, Hong H, Choi B, Park K-B, Durrant J, Kim J-Set al., 2022,

    Light-intensity dependent photoresponse time of organic photodetectors and its molecular origin

    , Nature Communications, Vol: 13, Pages: 1-10, ISSN: 2041-1723

    Organic photodetectors (OPDs) exhibit superior spectral responses but slower photoresponse times compared to inorganic counterparts. Herein, we study the light-intensity-dependent OPD photoresponse time with two small-molecule donors (planar MPTA or twisted NP-SA) co-evaporated with C 60 acceptors. MPTA:C60 exhibits the fastest response time at high-lightintensities (>0.5 mW/cm 2), attributed to its planar structure favoring strong intermolecular interactions. However, this blend exhibits the slowest response at low-light intensities, which is correlated with biphasic photocurrent transients indicative of the pr esence of a low density of deep trap states. Optical, structural and en ergetical analyses indicate that MPTA molecular packing is strongly disrupted by C 60, resulting in a larger (370 meV) HOMO level shift. This results in greater energetic inhomogeneity including possible MPTA-C 60 adduct formation, leading to deep trap states which limit the low-light photoresponse time. This work provides important insights into the small molecule design rules critical for low charge-trapping and high-speed OPD applications.

  • Journal article
    Luke J, Yang EJ, Chin Y-C, Che Y, Winkler L, Whatling D, Labanti C, Park SY, Kim J-Set al., 2022,

    Strong intermolecular interactions induced by high quadrupole moments enable excellent photostability of non-fullerene acceptors for organic photovoltaics

    , Advanced Energy Materials, Vol: 12, Pages: 1-11, ISSN: 1614-6832

    Understanding degradation mechanisms of organic photovoltaics (OPVs) is a critical prerequisite for improving device stability. Herein, the effect of molecular structure on the photostability of non-fullerene acceptors (NFAs) is studied by changing end-group substitution of ITIC derivatives: ITIC, ITIC-2F, and ITIC-DM. Using an assay of in situ spectroscopy techniques and molecular simulations, the photodegradation product of ITIC and the rate of product formation are identified, which correlates excellently to reported device stability, with ITIC-2F being the most stable and ITIC-DM the least. The choice of acceptor is found to affect both the donor polymer (PBDB-T) photostability and the morphological stability of the bulk heterojunction blend. Molecular simulations reveal that NFA end-group substitution strongly modulates the electron distribution within the molecule and thus its quadrupole moment. Compared to unsubstituted-ITIC, end-group fluorination results in a stronger, and demethylation a weaker, molecular quadrupole moment. This influences the intermolecular interactions between NFAs and between the NFA and the polymer, which in turn affects the photostability and morphological stability. This hypothesis is further tested on two other high quadrupole acceptors, Y6 and IEICO-4F, which both show impressive photostability. The strong correlation observed between NFA quadrupole moment and photostability opens a new synthetic direction for photostable organic photovoltaic materials.

  • Journal article
    Lee HKH, Stewart K, Hughes D, Barbe J, Pockett A, Kilbride RC, Heasman KC, Wei Z, Watson TM, Carnie MJ, Kim J-S, Tsoi WCet al., 2022,

    Proton radiation hardness of organic photovltaics: an in-depth study

    , Solar RRL, Vol: 6, Pages: 1-10, ISSN: 2367-198X

    Recent developments of solution-processed bulk-heterojunction organic photovoltaic (OPV) cells have demonstrated power conversion efficiencies (PCEs) as high as 18% for single-junction devices. Such a high PCE in addition to its desirable lightweight property and high mechanical flexibility can realize high specific power and small stowed volume, which are key considerations when choosing PV for space missions. To take one important step forward, their resilience to ionizing radiation should be well studied. Herein, the effect of proton irradiation at various fluences on the performance of benchmark OPV cells is explored under AM0 illumination. The remaining device performance is found to decrease with increasing proton fluence, which correlates to changes in electrical and chemical properties of the active layer. By redissolving the devices, the solubility of the active layer is found to decrease with increasing proton fluence, suggesting that the active materials are likely cross-linked. Additionally, Raman studies reveal conformational changes of the polymer leading to a higher degree of energetic disorder. Despite a drop in performance, the retaining percentage of the performance is indeed higher than the current market-dominating space PV technology—III–V semiconductor-based PV, demonstrating a high potential of the OPV cell as a candidate for space applications

  • Journal article
    Xu W, Du T, Sachs M, Macdonald TJ, Min G, Mohan L, Stewart K, Lin C-T, Wu J, Pacalaj R, Haque SA, McLachlan MA, Durrant JRet al., 2022,

    Asymmetric charge carrier transfer and transport in planar lead halide perovskite solar cells

    , Cell Reports Physical Science, Vol: 3, Pages: 1-17, ISSN: 2666-3864

    Understanding charge carrier extraction from the perovskite photoactive layer is critical to optimizing the design of perovskite solar cells. Herein, we demonstrate a simple time-resolved photoluminescence method to characterize the kinetics of charge transport across the bulk perovskite and charge transfer from the perovskite layer to the interlayers, elucidating the dependence of these dynamics on film thickness, grain boundaries (GBs), and interlayers. Using asymmetric laser excitation, we selectively probe charge transport by generating charges both close to and far from the heterojunction interface and correlate these results with device performance. We observe that both film thickness and GBs affect the asymmetry between electron and hole charge transport across the bulk perovskite and charge transfer from the bulk perovskite to the respective interlayers.

  • Journal article
    Wang B, Nam S, Limbu S, Kim J-S, Riede M, Bradley DDCet al., 2022,

    Properties and Applications of Copper(I) Thiocyanate Hole-Transport Interlayers Processed from Different Solvents

  • Journal article
    Yan H, Tseng T-W, Omagari S, Hamilton I, Nakamura T, Vacha M, Kim J-Set al., 2022,

    Dynamic molecular conformational change leading to energy transfer in F8-5% BSP copolymer revealed by single-molecule spectroscopy

    , JOURNAL OF CHEMICAL PHYSICS, Vol: 156, ISSN: 0021-9606
  • Journal article
    Marin-Beloqui J, Zhang G, Guo J, Shaikh J, Wohrer T, Hosseini SM, Sun B, Shipp J, Auty AJ, Chekulaev D, Ye J, Chin Y-C, Sullivan MB, Mozer AJ, Kim J-S, Shoaee S, Clarke TMet al., 2022,

    Insight into the origin of trapping in polymer/fullerene blends with a systematic alteration of the fullerene to higher adducts

    , The Journal of Physical Chemistry C: Energy Conversion and Storage, Optical and Electronic Devices, Interfaces, Nanomaterials, and Hard Matter, Vol: 126, Pages: 2708-2719, ISSN: 1932-7447

    The bimolecular recombination characteristics of conjugated polymer poly[(4,4′-bis(2-ethylhexyl)dithieno[3,2-b:2′,3′-d]silole)-2,6-diyl-alt-(2,5-bis 3-tetradecylthiophen-2-yl thiazolo 5,4-d thiazole)-2,5diyl] (PDTSiTTz) blended with the fullerene series PC60BM, ICMA, ICBA, and ICTA have been investigated using microsecond and femtosecond transient absorption spectroscopy, in conjunction with electroluminescence measurements and ambient photoemission spectroscopy. The non-Langevin polymer PDTSiTTz allows an inspection of intrinsic bimolecular recombination rates uninhibited by diffusion, while the low oscillator strengths of fullerenes allow polymer features to dominate, and we compare our results to those of the well-known polymer Si-PCPDTBT. Using μs-TAS, we have shown that the trap-limited decay dynamics of the PDTSiTTz polaron becomes progressively slower across the fullerene series, while those of Si-PCPDTBT are invariant. Electroluminescence measurements showed an unusual double peak in pristine PDTSiTTz, attributed to a low energy intragap charge transfer state, likely interchain in nature. Furthermore, while the pristine PDTSiTTz showed a broad, low-intensity density of states, the ICBA and ICTA blends presented a virtually identical DOS to Si-PCPDTBT and its blends. This has been attributed to a shift from a delocalized, interchain highest occupied molecular orbital (HOMO) in the pristine material to a dithienosilole-centered HOMO in the blends, likely a result of the bulky fullerenes increasing interchain separation. This HOMO localization had a side effect of progressively shifting the polymer HOMO to shallower energies, which was correlated with the observed decrease in bimolecular recombination rate and increased “trap” depth. However, since the density of tail states remained the same, this suggests that the traditional viewpoint of “trapping” being dominated by tail states may not encompass the full picture

  • Journal article
    Park SY, Labanti C, Luke J, Chin YC, Kim JSet al., 2022,

    Organic bilayer photovoltaics for efficient indoor light harvesting

    , Advanced Energy Materials, Vol: 12, Pages: 1-10, ISSN: 1614-6832

    Indoor organic photovoltaics (OPVs) are a potential niche application for organic semiconductors due to their strong and well-matched absorption with the emission of indoor lighting. However, due to extremely low photocurrent generation, the device parameters critical for efficient indoor OPVs differ from those under 1 Sun conditions. Herein, these critical device parameters—recombination loss and shunt resistance (Rsh)—are identified and it is demonstrated that bilayer OPVs are suitable for indoor PV applications. Compared to bulk-heterojunction (BHJ), the open-circuit voltage loss of bilayer devices under low light intensities is much smaller, consistent with a larger surface photovoltage response, indicating suppressed recombination losses. The bilayer devices show a higher fill factor at low light intensities, resulting from high Rsh afforded by the ideal interfacial contacts between the photoactive and the charge transport layers. The high Rsh enables bilayer devices to perform well without a light-soaking process. Finally, the charge carriers are extracted rapidly in bilayers, which are attributed to strongly suppressed trap states possibly induced by isolated domains and non-ideal interfacial contacts in BHJs. This study highlights the excellent suitability of bilayer OPVs for indoor applications and demonstrates the importance of device architecture and interfacial structures for efficient indoor OPVs.

  • Journal article
    Chin Y-C, Daboczi M, Henderson C, Luke J, Kim J-Set al., 2022,

    Suppressing PEDOT:PSS doping-induced interfacial recombination loss in perovskite solar cells

    , ACS Energy Letters, Vol: 7, Pages: 560-568, ISSN: 2380-8195

    PEDOT:PSS is widely used as a hole transport layer (HTL) in perovskite solar cells (PSCs) due to its facile processability, industrial scalability, and commercialization potential. However, PSCs utilizing PEDOT:PSS suffer from strong recombination losses compared to other organic HTLs. This results in lower open-circuit voltage (VOC) and power conversion efficiency (PCE). Most studies focus on doping PEDOT:PSS to improve charge extraction, but it has been suggested that a high doping level can cause strong recombination losses. Herein, we systematically dedope PEDOT:PSS with aqueous NaOH, raising its Fermi level by up to 500 meV, and optimize its layer thickness in p-i-n devices. A significant reduction of recombination losses at the dedoped PEDOT:PSS/perovskite interface is evidenced by a longer photoluminescence lifetime and higher magnitude of surface photovoltage, leading to an increased device VOC, fill factor, and PCE. These results provide insights into the relationship between doping level of HTLs and interfacial charge carrier recombination losses.

  • Journal article
    Daboczi M, Ratnasingham SR, Mohan L, Pu C, Hamilton I, Chin Y-C, McLachlan MA, Kim J-Set al., 2021,

    Optimal Interfacial Band Bending Achieved by Fine Energy Level Tuning in Mixed-Halide Perovskite Solar Cells

    , ACS ENERGY LETTERS, Vol: 6, Pages: 3970-3981, ISSN: 2380-8195
  • Journal article
    Mohan L, Ratnasingham SR, Panidi J, Daboczi M, Kim J-S, Anthopoulos TD, Briscoe J, McLachlan MA, Kreouzis Tet al., 2021,

    Determining out-of-plane hole mobility in CuSCN via the time-of-flight technique to elucidate its function in perovskite solar cells

    , ACS Applied Materials and Interfaces, Vol: 13, Pages: 38499-38507, ISSN: 1944-8244

    Copper(I) thiocyanate (CuSCN) is a stable, low-cost, solution-processable p-type inorganic semiconductor used in numerous optoelectronic applications. Here, for the first time, we employ the time-of-flight (ToF) technique to measure the out-of-plane hole mobility of CuSCN films, enabled by the deposition of 4 μm-thick films using aerosol-assisted chemical vapor deposition (AACVD). A hole mobility of ∼10–3 cm2/V s was measured with a weak electric field dependence of 0.005 cm/V1/2. Additionally, by measuring several 1.5 μm CuSCN films, we show that the mobility is independent of thickness. To further validate the suitability of our AACVD-prepared 1.5 μm-thick CuSCN film in device applications, we demonstrate its incorporation as a hole transport layer (HTL) in methylammonium lead iodide (MAPbI3) perovskite solar cells (PSCs). Our AACVD films result in devices with measured power conversion efficiencies of 10.4%, which compares favorably with devices prepared using spin-coated CuSCN HTLs (12.6%), despite the AACVD HTLs being an order of magnitude thicker than their spin-coated analogues. Improved reproducibility and decreased hysteresis were observed, owing to a combination of excellent film quality, high charge-carrier mobility, and favorable interface energetics. In addition to providing a fundamental insight into charge-carrier mobility in CuSCN, our work highlights the AACVD methodology as a scalable, versatile tool suitable for film deposition for use in optoelectronic devices.

  • Journal article
    Tyrrell JE, Petkos K, Drakakis EM, Boutelle MG, Campbell AJet al., 2021,

    Organic electrochemical transistor common‐source amplifier for electrophysiological measurements

    , Advanced Functional Materials, Vol: 31, Pages: 1-13, ISSN: 1616-301X

    The portability of physiological monitoring has necessitated the biocompatibility of components used in circuitry local to biological environments. A key component in processing circuitry is the linear amplifier. Amplifier circuit topologies utilize transistors, and recent advances in bioelectronics have focused on organic electrochemical transistors (OECTs). OECTs have shown the capability to transduce physiological signals at high signal-to-noise ratios. In this study high-performance interdigitated electrode OECTs are implemented in a common source linear amplifier topology. Under the constraints of OECT operation, stable circuit component parameters are found, and OECT geometries are varied to determine the best amplifier performance. An equation is formulated which approximates transistor behavior in the linear, nonlinear, and saturation regimes. This equation is used to simulate the amplifier response of the circuits with the best performing OECT geometries. The amplifier figures of merit, including distortion characterizations, are then calculated using physical and simulation measurements. Based on the figures of merit, prerecorded electrophysiological signals from spreading depolarizations, electrocorticography, and electromyography fasciculations are inputted into an OECT linear amplifier. Using frequency filtering, the primary features of events in the bioelectric signals are resolved and amplified, demonstrating the capability of OECT amplifiers in bioelectronics.

  • Journal article
    Vasilopoulou M, Mohd Yusoff ARB, Daboczi M, Conforto J, Gavim AEX, da Silva WJ, Macedo AG, Soultati A, Pistolis G, Schneider FK, Dong Y, Jacoutot P, Rotas G, Jang J, Vougioukalakis GC, Chochos CL, Kim J-S, Gasparini Net al., 2021,

    High efficiency blue organic light-emitting diodes with below-bandgap electroluminescence

    , Nature Communications, Vol: 12, ISSN: 2041-1723

    Blue organic light-emitting diodes require high triplet interlayer materials, which induce large energetic barriers at the interfaces resulting in high device voltages and reduced efficiencies. Here, we alleviate this issue by designing a low triplet energy hole transporting interlayer with high mobility, combined with an interface exciplex that confines excitons at the emissive layer/electron transporting material interface. As a result, blue thermally activated delay fluorescent organic light emitting diodes with a below-bandgap turn-on voltage of 2.5 V and an external quantum efficiency of 41.2% were successfully fabricated. These devices also showed suppressed efficiency roll-off maintaining an EQE of 34.8% at 1000 cd m-2. Our approach paves the way for further progress through exploring alternative device engineering approaches instead of only focusing on the demanding synthesis of organic compounds with complex structures.

  • Journal article
    Clarke AJ, Luke J, Meitzner R, Wu J, Wang Y, Lee HKH, Speller EM, Bristow H, Cha H, Newman MJ, Hooper K, Evans A, Gao F, Hoppe H, McCulloch I, Schubert US, Watson TM, Durrant JR, Tsoi WC, Kim J-S, Li Zet al., 2021,

    Non-fullerene acceptor photostability and its impact on organic solar cell lifetime

  • Journal article
    Marin-Beloqui JM, Toolan DTW, Panjwani NA, Limbu S, Kim J-S, Clarke TMet al., 2021,

    Triplet-Charge Annihilation in a Small Molecule Donor: Acceptor Blend as a Major Loss Mechanism in Organic Photovoltaics

    , ADVANCED ENERGY MATERIALS, Vol: 11, ISSN: 1614-6832
  • Journal article
    Limbu S, Stewart K, Nightingale J, Yan H, Balamurugan C, Hong S, Kim J, Lee K, Kwon S, Kim J-Set al., 2021,

    Solid-State Ionic Liquid: Key to Efficient Detection and Discrimination in Organic Semiconductor Gas Sensors

    , ACS APPLIED ELECTRONIC MATERIALS, Vol: 3, Pages: 2152-2163
  • Journal article
    Kyeong M, Lee J, Daboczi M, Stewart K, Yao H, Cha H, Luke J, Lee K, Durrant JR, Kim J-S, Hong Set al., 2021,

    Organic cathode interfacial materials for non-fullerene organic solar cells

    , JOURNAL OF MATERIALS CHEMISTRY A, Vol: 9, Pages: 13506-13514, ISSN: 2050-7488
  • Journal article
    Yun D-J, Lee S, Kim SH, Jung C, Kim YS, Chung JG, Heo S, Kwon Y-N, Lee E, Kim J-S, Ko D-S, Kim SYet al., 2021,

    Bevel Structure Based XPS Analysis as a Non-Destructive Chemical Probe for Complex Interfacial Structures of Organic Semiconductors

    , SMALL METHODS, Vol: 5, ISSN: 2366-9608
  • Journal article
    Labanti C, Sung MJ, Luke J, Kwon S, Kumar R, Hong J, Kim J, Bakulin AA, Kwon S-K, Kim Y-H, Kim J-Set al., 2021,

    Selenium-substituted non-fullerene acceptors: a route to superior Operational stability for organic bulk heterojunction solar cells.

    , ACS Nano, Vol: 15, Pages: 7700-7712, ISSN: 1936-0851

    Non-fullerene acceptors (NFAs) for organic solar cells (OSCs) have significantly developed over the past five years with continuous improvements in efficiency now over 18%. However, a key challenge still remains in order to fully realize their commercialization potential: the need to extend device lifetime and to control degradation mechanisms. Herein, we investigate the effect of two different molecular engineering routes on the widely utilized ITIC NFA, to tune its optoelectronic properties and interactions with the donor polymer in photoactive blends. Heavier selenium (Se) atoms substitute sulfur (S) atoms in the NFA core in either outer or inner positions, and methyl chains are attached to the end groups. By investigating the effects of these structural modifications on the long-term operational stability of bulk-heterojunction OSC devices, we identify outer selenation as a powerful strategy to significantly increase device lifetime compared to ITIC. Combining outer selenation and methylation results in an impressive 95% of the initial OSC efficiency being retained after 450 h under operating conditions, with an exceptionally long projected half-lifetime of 5600 h compared to 400 h for ITIC. We find that the heavier and larger Se atoms at outer-core positions rigidify the molecular structure to form highly crystalline films with low conformational energetic disorder. It further enhances charge delocalization over the molecule, promoting strong intermolecular interactions among acceptor molecules. Upon methylation, this strong intermolecular interaction stabilizes acceptor domains in blends to be resilient to light-induced morphological changes, thereby leading to superior device stability. Our results highlight the crucial role of NFA molecular structure for OSC operational stability and provide important NFA design rules via heteroatom position and end-group control.

  • Journal article
    Kafourou P, Park B, Luke J, Tan L, Panidi J, Glöcklhofer F, Kim J, Anthopoulos TD, Kim J, Lee K, Kwon S, Heeney Met al., 2021,

    One‐step sixfold cyanation of benzothiadiazole acceptor units for air‐stable high‐performance n‐type organic field‐effect transistors

    , Angewandte Chemie, Vol: 133, Pages: 6035-6042, ISSN: 0044-8249

    Reported here is a new high electron affinity acceptor end group for organic semiconductors, 2,1,3‐benzothiadiazole‐4,5,6‐tricarbonitrile (TCNBT). An n‐type organic semiconductor with an indacenodithiophene (IDT) core and TCNBT end groups was synthesized by a sixfold nucleophilic substitution with cyanide on a fluorinated precursor, itself prepared by a direct arylation approach. This one‐step chemical modification significantly impacted the molecular properties: the fluorinated precursor, TFBT IDT, a poor ambipolar semiconductor, was converted into TCNBT IDT, a good n‐type semiconductor. The electron‐deficient end group TCNBT dramatically decreased the energy of the highest occupied and lowest unoccupied molecular orbitals (HOMO/LUMO) compared to the fluorinated analogue and improved the molecular orientation when utilized in n‐type organic field‐effect transistors (OFETs). Solution‐processed OFETs based on TCNBT IDT exhibited a charge‐carrier mobility of up to μe≈0.15 cm2 V−1 s−1 with excellent ambient stability for 100 hours, highlighting the benefits of the cyanated end group and the synthetic approach.

  • Journal article
    Heeney M, Kafourou P, Park B, Luke J, Luxi T, Panidi J, Glöcklhofer F, Kim J, Anthopoulos TD, Kim J-S, Lee K, Kwon Set al., 2021,

    One-step six-fold cyanation of benzothiadiazole acceptor Units for air-stable high-performance n-type organic field-effect transistors

    , Angewandte Chemie International Edition, Vol: 60, Pages: 5970-5977, ISSN: 1433-7851

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

  • Journal article
    Ratnasingham SR, Mohan L, Daboczi M, Degousée T, Binions R, Fenwick O, Kim J-S, McLachlan MA, Briscoe Jet al., 2021,

    Novel scalable aerosol-assisted CVD route for perovskite solar cells

    , Materials Advances, Vol: 2, Pages: 1606-1612

    Organo-metal halide perovskite research has progressed rapidly, with photovoltaic (PV) devices achieving over 25% power conversion efficiency (PCE). However, scalable production of these devices is an ongoing challenge. We demonstrate the growth of methylammonium lead triiodide (MAPI) films via a novel two-step aerosol-assisted chemical vapour deposition (AACVD) method leading to the first ever perovskite-based PV devices using active layers deposited by AACVD. This is a scalable deposition process, requiring less complex equipment than conventional CVD. Furthermore, our method utilises methanol (MeOH) as the only solvent, as opposed to harmful solvents typically used in perovskite processing. Structural and optical characterization confirms successful formation of MAPI with no secondary phases and an optical bandgap of ∼1.58 eV. The final film had large grains (order of μm), with thickness ranging from 500–1100 nm. These films were used to fabricate working PV devices resulting in a champion PCE of 5.4%. While films demonstrated high structural and compositonal quality, we identified large film roughness as a limiting factor in device PCE, and elucidate the origin of this via detailed study of the film growth, which reveals a unique multi-step film formation process.

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

    Recent progress and Challenges toward highly stable nonfullerene acceptor‐based organic solar cells

    , Advanced Energy Materials, Vol: 11, ISSN: 1614-6832

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

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

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

    , ACS NANO, Vol: 15, Pages: 1217-1228, ISSN: 1936-0851
  • Journal article
    Luke J, Correa L, Rodrigues J, Martins J, Daboczi M, Bagnis D, Kim J-Set al., 2021,

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

    , ADVANCED ENERGY MATERIALS, Vol: 11, ISSN: 1614-6832
  • Journal article
    Tyrrell J, Boutelle M, Campbell A, 2021,

    Measurement of electrophysiological signals in vitro using high-performance organic electrochemical transistors

    , Advanced Functional Materials, Vol: 31, Pages: 1-12, ISSN: 1616-301X

    Biological environments use ions in charge transport for information transmission. The properties of mixed electronic and ionic conductivity in organic materials make them ideal candidates to transduce physiological information into electronically processable signals. A device proven to be highly successful in measuring such information is the organic electrochemical transistor (OECT). Previous electrophysiological measurements performed using OECTs show superior signal‐to‐noise ratios than electrodes at low frequencies. Subsequent development has significantly improved critical performance parameters such as transconductance and response time. Here, interdigitated‐electrode OECTs are fabricated on flexible substrates, with one such state‐of‐the‐art device achieving a peak transconductance of 139 mS with a 138 µs response time. The devices are implemented into an array with interconnects suitable for micro‐electrocorticographic application and eight architecture variations are compared. The two best‐performing arrays are subject to the full electrophysiological spectrum using prerecorded signals. With frequency filtering, kHz‐scale frequencies with 10 µV‐scale voltages are resolved. This is supported by a novel quantification of the noise, which compares the gate voltage input and drain current output. These results demonstrate that high‐performance OECTs can resolve the full electrophysiological spectrum and suggest that superior signal‐to‐noise ratios could be achieved in high frequency measurements of multiunit activity.

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

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

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

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

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

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

    , JOURNAL OF MATERIALS CHEMISTRY C, Vol: 8, Pages: 15268-15276, ISSN: 2050-7526

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