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  • 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

    , CELL REPORTS PHYSICAL SCIENCE, Vol: 2
  • 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
    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
    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
    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
    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
    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 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
    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 π-conjugated polymer/solid-state ionic liquid complex as a highly sensitive and selective gas sensor

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

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

    Nitrogen-Doped Carbon Dots/TiO<sub>2</sub> Nanoparticle Composites for Photoelectrochemical Water Oxidation

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

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

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

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

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

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

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