233 results on '"Thomas D. Anthopoulos"'
Search Results
2. 28.2%-efficient, outdoor-stable perovskite/silicon tandem solar cell
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Frédéric Laquai, Michele De Bastiani, Emre Yengel, Stefaan De Wolf, Omar F. Mohammed, Erkan Aydin, Michael Salvador, Thomas D. Anthopoulos, Maxime Babics, Osman M. Bakr, Wenbo Yan, Thomas Allen, Furkan Halis Isikgor, Kaichen Zhu, Atteq ur Rehman, Fuzong Xu, Xiaopeng Zheng, Jun Yin, Mingcong Wang, Yajun Gao, Jafar Iqbal Khan, George T. Harrison, Esma Ugur, Jiang Liu, Anand S. Subbiah, and Mario Lanza
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Materials science ,Silicon ,Tandem ,Passivation ,business.industry ,Stacking ,chemistry.chemical_element ,law.invention ,General Energy ,chemistry ,law ,Phase (matter) ,Solar cell ,Optoelectronics ,Crystalline silicon ,business ,Perovskite (structure) - Abstract
Summary Stacking perovskite solar cells onto crystalline silicon bottom cells in a monolithic tandem configuration enables power-conversion efficiencies (PCEs) well above those of their single-junction counterparts. However, state-of-the-art wide-band-gap perovskite films suffer from phase stability issues. Here, we show how carbazole as an additive to the perovskite precursor solution can not only reduce nonradiative recombination losses but, perhaps more importantly, also can suppress phase segregation under exposure to moisture and light illumination. This enables a stabilized PCE of 28.6% (independently certified at 28.2%) for a monolithic perovskite/silicon tandem solar cell over ∼1 cm2 and 27.1% over 3.8 cm2, built from a textured silicon heterojunction solar cell. The modified tandem devices retain ∼93% of their performance over 43 days in a hot and humid outdoor environment of almost 100% relative humidity over 250 h under continuous 1-sun illumination and about 87% during a 85/85 damp-heat test for 500 h, demonstrating the improved phase stability.
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- 2021
3. Using Two Compatible Donor Polymers Boosts the Efficiency of Ternary Organic Solar Cells to 17.7%
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Wenhong Peng, Han Young Woo, Zewdneh Genene, Ergang Wang, Yuanbao Lin, Leonidas Tsetseris, Yuliar Firdaus, Thomas D. Anthopoulos, Sang Young Jeong, Weiguo Zhu, and Aggelos Nikitaras
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Photocurrent ,chemistry.chemical_classification ,Materials science ,Organic solar cell ,business.industry ,General Chemical Engineering ,Stacking ,General Chemistry ,Polymer ,Polymer solar cell ,chemistry ,Materials Chemistry ,Optoelectronics ,Binary system ,business ,Ternary operation ,HOMO/LUMO - Abstract
The use of ternary organic semiconducting blends is recognized as an effective strategy to boost the performance of polymer solar cells (PSCs) by increasing the photocurrent while minimizing voltage losses. Yet, the scarcity of suitable donors with a deep highest occupied molecular orbital (HOMO) level poses a challenge in extending this strategy to ternary systems based on two polymers. Here, we address this challenge by the synthesis of a new donor polymer (PM7-Si), which is akin to the well-known PM6 but has a deeper HOMO level. PM7-Si is utilized as the third component to enhance the performance of the best-in-class binary system of PM6:BTP-eC9, leading to simultaneous improvements in the efficiency (17.7%), open-circuit voltage (0.864 V), and fill factor (77.6%). These decisively enhanced features are attributed to the efficient carrier transport, improved stacking order, and morphology. Our results highlight the use of two polymer donors as a promising strategy toward high-performance ternary PSCs.
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- 2021
4. Determining Out-of-Plane Hole Mobility in CuSCN via the Time-of-Flight Technique To Elucidate Its Function in Perovskite Solar Cells
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Julianna Panidi, Martyn A. McLachlan, Matyas Daboczi, Lokeshwari Mohan, Thomas D. Anthopoulos, Theo Kreouzis, Ji-Seon Kim, Joe Briscoe, and Sinclair R. Ratnasingham
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Technology ,Electron mobility ,Materials science ,time-of-flight technique ,Materials Science ,Materials Science, Multidisciplinary ,hole transport material ,Time of flight technique ,FILMS ,perovskite solar cells ,LAYERS ,09 Engineering ,out-of-plane hole mobility ,Out of plane ,HIGH-EFFICIENCY ,chemistry.chemical_compound ,TRANSPORT MATERIAL ,CHARGE-TRANSPORT ,General Materials Science ,Nanoscience & Nanotechnology ,copper(I) thiocyanate ,HYSTERESIS ,CONDUCTIVITY ,Perovskite (structure) ,Science & Technology ,Function (mathematics) ,PERFORMANCE ,Engineering physics ,Copper(I) thiocyanate ,chemistry ,Science & Technology - Other Topics ,03 Chemical Sciences ,Electronic materials - Abstract
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.
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- 2021
5. Concurrent cationic and anionic perovskite defect passivation enables 27.4% perovskite/silicon tandems with suppression of halide segregation
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Frédéric Laquai, Iain McCulloch, Thomas D. Anthopoulos, Emre Yengel, Mingcong Wang, Shynggys Zhumagali, Furkan Halis Isikgor, Esma Ugur, Mathan Kumar Eswaran, Atteq ur Rehman, George T. Harrison, Stefaan De Wolf, Nicola Gasparini, Thomas Allen, Michele De Bastiani, Emmanuel Van Kerschaver, Calvyn Travis Howells, Udo Schwingenschlögl, Erkan Aydin, Francesco Furlan, Derya Baran, Jiang Liu, and Anand S. Subbiah
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Materials science ,Passivation ,Silicon ,Tandem ,business.industry ,Wide-bandgap semiconductor ,chemistry.chemical_element ,Halide ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,General Energy ,chemistry ,Chemical engineering ,Photovoltaics ,Grain boundary ,0210 nano-technology ,business ,Perovskite (structure) - Abstract
Summary Stable and efficient perovskite/silicon tandem solar cells require defect passivation and suppression of light-induced phase segregation of the wide-band-gap perovskite. Here, we report how molecules containing both electron-rich and electron-poor moieties, such as phenformin hydrochloride (PhenHCl), can satisfy both requirements, independent of the perovskite’s surface chemical composition and its grain boundaries and interfaces. PhenHCl-passivated wide-band-gap (∼1.68 eV) perovskite p-i-n single-junction solar cells deliver an open-circuit voltage (VOC) ∼100 mV higher than control devices, resulting in power conversion efficiencies (PCEs) up to 20.5%. These devices do not show any VOC losses after more than 3,000 h of thermal stress at 85°C in a nitrogen ambient. Moreover, PhenHCl passivation improves the PCE of textured perovskite/silicon tandem solar cells from 25.4% to 27.4%. Our findings provide critical insights for improved passivation of metal halide perovskite surfaces and the fabrication of highly efficient and stable perovskite-based single-junction and tandem solar cells.
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- 2021
6. 18.4 % Organic Solar Cells Using a High Ionization Energy Self‐Assembled Monolayer as Hole‐Extraction Interlayer
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Osman M. Bakr, Xiaopeng Zheng, Dimitris Kaltsas, Leonidas Tsetseris, Hendrik Faber, Yuliar Firdaus, Artiom Magomedov, Yuanbao Lin, Neha Chaturvedi, Thomas D. Anthopoulos, Abdulrahman El-Labban, Kalaivanan Loganathan, Frédéric Laquai, Dipti R Naphade, Emre Yarali, Sanaa Hayel Nazil Alshammari, Despoina Gkeka, Emre Yengel, and Vytautas Getautis
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Materials science ,Organic solar cell ,General Chemical Engineering ,Energy conversion efficiency ,Self-assembled monolayer ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Styrene ,chemistry.chemical_compound ,General Energy ,Sulfonate ,PEDOT:PSS ,chemistry ,Monolayer ,Environmental Chemistry ,Physical chemistry ,General Materials Science ,0210 nano-technology ,HOMO/LUMO - Abstract
Self-assembled monolayers (SAMs) based on Br-2PACz ([2-(3,6-dibromo-9H-carbazol-9-yl)ethyl]phosphonic acid) 2PACz ([2-(9H-Carbazol-9-yl)ethyl]phosphonic acid) and MeO-2PACz ([2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl]phosphonic acid) molecules were investigated as hole-extracting interlayers in organic photovoltaics (OPVs). The highest occupied molecular orbital (HOMO) energies of these SAMs were measured at -6.01 and -5.30 eV for Br-2PACz and MeO-2PACz, respectively, and found to induce significant changes in the work function (WF) of indium-tin-oxide (ITO) electrodes upon chemical functionalization. OPV cells based on PM6 (poly[(2,6-(4,8-bis(5-(2-ethylhexyl-3-fluoro)thiophen-2-yl)-benzo[1,2-b:4,5-b']dithiophene))-alt-(5,5-(1',3'-di-2-thienyl-5',7'-bis(2-ethylhexyl)benzo[1',2'-c:4',5'-c']dithiophene-4,8-dione)]) : BTP-eC9 : PC71 BM ([6,6]-phenyl-C71-butyric acid methyl ester) using ITO/Br-2PACz anodes exhibited a maximum power conversion efficiency (PCE) of 18.4 %, outperforming devices with ITO/MeO-2PACz (14.5 %) and ITO/poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT : PSS) (17.5 %). The higher PCE was found to originate from the much higher WF of ITO/Br-2PACz (-5.81 eV) compared to ITO/MeO-2PACz (4.58 eV) and ITO/PEDOT : PSS (4.9 eV), resulting in lower interface resistance, improved hole transport/extraction, lower trap-assisted recombination, and longer carrier lifetimes. Importantly, the ITO/Br-2PACz electrode was chemically stable, and after removal of the SAM it could be recycled and reused to construct fresh OPVs with equally impressive performance.
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- 2021
7. Adduct-based p-doping of organic semiconductors
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Fengyu Zhang, Simantini Nayak, Antoine Kahn, Vytautas Getautis, Sameer Vajjala Kesava, Tadas Malinauskas, Junliang Liu, Aniruddha Basu, Nobuya Sakai, Ross Warren, Thomas D. Anthopoulos, Himansu S. Biswal, Chris R. M. Grovenor, Moritz Riede, Yen-Hung Lin, Xin Lin, Pabitra K. Nayak, and Henry J. Snaith
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Organic electronics ,chemistry.chemical_classification ,Materials science ,Dopant ,Mechanical Engineering ,Doping ,Halide ,Nanotechnology ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Condensed Matter Physics ,01 natural sciences ,0104 chemical sciences ,Organic semiconductor ,chemistry ,Mechanics of Materials ,General Materials Science ,Electronics ,Counterion ,0210 nano-technology ,Perovskite (structure) - Abstract
Electronic doping of organic semiconductors is essential for their usage in highly efficient optoelectronic devices. Although molecular and metal complex-based dopants have already enabled significant progress of devices based on organic semiconductors, there remains a need for clean, efficient and low-cost dopants if a widespread transition towards larger-area organic electronic devices is to occur. Here we report dimethyl sulfoxide adducts as p-dopants that fulfil these conditions for a range of organic semiconductors. These adduct-based dopants are compatible with both solution and vapour-phase processing. We explore the doping mechanism and use the knowledge we gain to 'decouple' the dopants from the choice of counterion. We demonstrate that asymmetric p-doping is possible using solution processing routes, and demonstrate its use in metal halide perovskite solar cells, organic thin-film transistors and organic light-emitting diodes, which showcases the versatility of this doping approach.
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- 2021
8. All-Solution-Processed Quantum Dot Electrical Double-Layer Transistors Enhanced by Surface Charges of Ti3C2Tx MXene Contacts
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Thomas D. Anthopoulos, Zhenwei Wang, Husam N. Alshareef, Hyunho Kim, Xinwei Guan, Mohamad Insan Nugraha, Xiangming Xu, Tao Wu, Derya Baran, and Mrinal K. Hota
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Materials science ,business.industry ,Transistor ,General Engineering ,General Physics and Astronomy ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,law.invention ,Solution processed ,chemistry.chemical_compound ,chemistry ,law ,Quantum dot ,Optoelectronics ,General Materials Science ,Lead sulfide ,Colloidal quantum dots ,Surface charge ,0210 nano-technology ,MXenes ,business - Abstract
Fully solution-processed, large-area, electrical double-layer transistors (EDLTs) are presented by employing lead sulfide (PbS) colloidal quantum dots (CQDs) as active channels and Ti3C2Tx MXene as...
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- 2021
9. One‐Step Sixfold Cyanation of Benzothiadiazole Acceptor Units for Air‐Stable High‐Performance n‐Type Organic Field‐Effect Transistors
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Martin Heeney, Byoungwook Park, Julianna Panidi, Thomas D. Anthopoulos, Joel Luke, Sooncheol Kwon, Kwanghee Lee, Panagiota Kafourou, Florian Glöcklhofer, Ji-Seon Kim, Luxi Tan, Jehan Kim, EPSRC, The Royal Society, Kaust, EPRSC, National Research Foundation of Korea (NRF), Engineering and Physical Sciences Research Council, and CSEM Brasil
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Materials science ,Chemistry, Multidisciplinary ,nucleophilic aromatic substitution ,Cyanation ,010402 general chemistry ,Photochemistry ,01 natural sciences ,Catalysis ,Nucleophilic aromatic substitution ,fluorine ,Nucleophilic substitution ,field effect transistors ,Molecular orbital ,HOMO/LUMO ,Research Articles ,Organic electronics ,Science & Technology ,010405 organic chemistry ,Organic Chemistry ,General Medicine ,General Chemistry ,Acceptor ,0104 chemical sciences ,organic electronics ,Organic semiconductor ,Chemistry ,Organic semiconductor Acceptor endgroup n-type material Nucleophillic aromatic substitution Field-effect transistor ,Semiconductors ,Physical Sciences ,03 Chemical Sciences ,Research Article - Abstract
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 μ e≈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., A new strongly electron‐accepting end group, 2,1,3‐benzothiadiazole‐4,5,6‐tricarbonitrile (TCNBT), has been prepared by a one‐step sixfold nucleophilic substitution reaction. Cyanation results in a significant enhancement of the electron affinity in comparison to the fluorinated analogue, and the material demonstrates promising n‐type performance in solution processed organic field‐effect transistors with excellent stability.
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- 2021
10. The influence of alkyl group regiochemistry and backbone fluorination on the packing and transistor performance of N-cyanoimine functionalised indacenodithiophenes
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Thomas D. Anthopoulos, Andrew J. P. White, Karl J. Thorley, Changsheng Wang, Aniruddha Basu, Florian Glöcklhofer, William Mitchell, Thomas Hodsden, Martin Heeney, and FWF Austrian Science Fund (FWF)
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Technology ,Electron mobility ,Materials science ,Materials Science ,SEMICONDUCTING POLYMERS ,Stacking ,Materials Science, Multidisciplinary ,02 engineering and technology ,010402 general chemistry ,01 natural sciences ,Electron transfer ,DCNQI ,CHARGE-TRANSPORT ,Structural isomer ,General Materials Science ,Alkyl ,chemistry.chemical_classification ,Science & Technology ,DESIGN STRATEGIES ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,Organic semiconductor ,Crystallography ,chemistry ,Chemistry (miscellaneous) ,Polar effect ,CHANNEL ORGANIC TRANSISTORS ,THIOPHENE ,FIELD-EFFECT TRANSISTORS ,0210 nano-technology ,Single crystal - Abstract
The synthesis of two novel n-type molecular organic semiconductors based on a fluorinated indacenodithiophene core in combination with an electron withdrawing N-cyanoimine group is reported, and the influence of the regiochemistry of the solubilizing sidechain is investigated. The N-cyanoimine is confirmed to be a strongly electron accepting group, which in combination with the core fluorination resulted in high electron affinities for both materials. Single crystal analysis demonstrated that whilst both materials arrange in ordered slipped stacks with close π–π stacking distances (∼3.40 Å), significant differences in electron transfer integrals for the two regioisomers were observed, relating to differences in relative molecular displacement along the π-stacking direction. Organic thin-film transistors fabricated via blade-coating displayed electron mobility up to 0.13 cm2 V−1 s−1 for the isomer with the larger transfer integral.
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- 2021
11. Unraveling the compositional heterogeneity and carrier dynamics of alkali cation doped 3D/2D perovskites with improved stability
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Thomas D. Anthopoulos, Timothy J. Magnanelli, Siyuan Zhang, Christina A. Hacker, Ming-Chun Tang, Edwin J. Heilweil, and Nhan V. Nguyen
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Materials science ,Photoemission spectroscopy ,business.industry ,Doping ,Analytical chemistry ,chemistry.chemical_element ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Rubidium ,chemistry ,X-ray photoelectron spectroscopy ,Chemistry (miscellaneous) ,Electrical resistivity and conductivity ,Photovoltaics ,General Materials Science ,Work function ,0210 nano-technology ,business ,Perovskite (structure) - Abstract
Preventing the degradation of hybrid perovskites by humid air remains a challenge for their future commercial utilization. 3D/2D perovskites with hierarchical architecture have attracted significant attention due to their promising power conversion efficiency (PCE) and device stability. Here, we report a novel 3D/2D planar bi-layer perovskite obtained by growing a 2D Ruddlesden–Popper layer on top of a 3D rubidium (Rb+)-doped triple-cation perovskite. Rb+ cation incorporation decreases the work function, and 3D/2D films show smaller work function values compared to classic 3D perovskites. X-ray photoemission spectroscopy (XPS) confirms the presence of a 2D perovskite capping layer and observes halide migration. Time-resolved terahertz spectroscopy (TRTS) shows that the average DC carrier mobility for the 3D/2D hierarchical structures and their 3D counterparts is one order of magnitude higher than that for the 2D perovskite. The resulting 3D/2D Rb+-incorporated perovskite solar cells show a peak PCE of >20%, which is slightly higher than their 3D counterparts (19.5%). Benefiting from moisture resistivity, the 3D/2D perovskite photovoltaics show significantly improved long-term stability by retaining 81% of the initial PCE after 60 days of exposure to ambient air (50 ± 10% relative humidity) without encapsulation, highlighting the potential of engineered stable 3D/2D perovskite solar cells for their commercial utilization.
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- 2021
12. Tyrian purple: an ancient natural dye for cross-conjugated n-type charge transport
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Tracey M. Clarke, Thomas D. Anthopoulos, Kealan J. Fallon, Hugo Bronstein, Daniel T. W. Toolan, Jose Manuel Marin-Beloqui, Mohammed Al-Hashimi, Nilushi Wijeyasinghe, and Anastasia Leventis
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Quantum chemical ,chemistry.chemical_classification ,Delocalized electron ,Materials science ,chemistry ,Materials Chemistry ,Charge (physics) ,General Chemistry ,Polymer ,Conjugated system ,Photochemistry ,Natural dye ,Visible spectrum - Abstract
Herein, we present two novel organic semiconducting polymers synthesised from an ancient dye. By employing cross-conjugation within the polymer backbone as a synthetic strategy, we are able to engineer optical gaps such that the novel materials absorb over the entire visible spectrum. The cross-conjugated polymers exhibited relatively high n-type charge transport performance in organic field-effect transistors, a rare characteristic for this type of polymer. Quantum chemical calculations provide insight into this behaviour, suggesting that, whilst conjugation along the HOMO is indeed inhibited via molecular design, these materials possess highly delocalized LUMOs, facilitating high n-type charge transport.
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- 2021
13. Molecular doping of near-infrared organic photodetectors for photoplethysmogram sensors
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Thomas D. Anthopoulos, Binghao Wang, Yuliar Firdaus, Mari Koizumi, Tomoyuki Yokota, Yuanbao Lin, Sunghoon Lee, Mohamad Insan Nugraha, Alberto D. Scaccabarozzi, Haoyang Wang, Yan Wang, and Takao Someya
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Materials science ,Dopant ,business.industry ,Near-infrared spectroscopy ,Doping ,Photodetector ,General Chemistry ,Borane ,chemistry.chemical_compound ,chemistry ,Materials Chemistry ,Pulse wave ,Optoelectronics ,business ,Dimethylamine ,Dark current - Abstract
Doping is a common strategy in the field of semiconductor technology but its employment in organic photodetectors (OPDs) has been limited due to the typical uncontrollable increase of the dark currents. This study introduces three different molecular dopants, including p-type tris(pentafluorophenyl)borane, n-type benzyl viologen, and (4-(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)-phenyl)dimethylamine, for near-infrared poly[[2,5-bis(2-hexyldecyl)-2,3,5,6-tetrahydro-3,6-dioxopyrrolo[3,4-c]pyrrole-1,4-diyl]-alt-[3′,3′′-dimethyl-2,2′:5′,2′′-terthiophene]-5,5′′-diyl]:[6,6]-phenyl C61 butyric acid methyl ester (PMDPP3T:PC61BM) bulk-heterojunction OPDs. The results show that OPDs with optimal 0.02 wt% dopants exhibit low dark current (3.18 × 10−8 A cm−2), high detectivity (5.56 × 1012 Jones), and good environmental stability for ∼2 months. These doped OPDs are further used for pulse wave monitoring, which exhibit stable waveforms and can distinguish slow and fast heartbeat rates.
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- 2021
14. Unraveling the New Role of an Ethylene Carbonate Solvation Shell in Rechargeable Metal Ion Batteries
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Wandi Wahyudi, Thomas D. Anthopoulos, Luigi Cavallo, Jun Ming, Gang Liu, Geon Tae Park, Yang-Kook Sun, Limin Wang, Zhen Cao, Qian Li, and Husam N. Alshareef
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Renewable Energy, Sustainability and the Environment ,Rare earth ,Energy Engineering and Power Technology ,Library science ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Chinese academy of sciences ,0104 chemical sciences ,chemistry.chemical_compound ,Fuel Technology ,Solvation shell ,chemistry ,Chemistry (miscellaneous) ,Materials Chemistry ,0210 nano-technology ,Ethylene carbonate ,Independent research - Abstract
This work is supported by the National Natural Science Foundation of China (21978281, 21975250) and the National Key R&D Program of China (SQ2017YFE9128100). The authors also thank the Independent Research Project of the State Key Laboratory of Rare Earth Resources Utilization (110005R086), Changchun Institute of Applied Chemistry, Chinese Academy of Sciences. The research was also supported by King Abdullah University of Science and Technology (KAUST) and Hanyang University.
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- 2020
15. N-type organic thermoelectrics: demonstration of ZT > 0.3
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Mohamad Insan Nugraha, Jingjin Dong, Mario Caironi, Siewert J. Marrink, Derya Baran, Thomas D. Anthopoulos, Bas van der Zee, Giuseppe Portale, Selim Sami, Ryan C. Chiechi, Remco W. A. Havenith, L. Jan Anton Koster, Riccardo Alessandri, Xinkai Qiu, Alex J. Barker, Jian Liu, Jan C. Hummelen, Li Qiu, Nathalie Klasen, Sylvia Rousseva, Photophysics and OptoElectronics, Molecular Dynamics, Theoretical Chemistry, Macromolecular Chemistry & New Polymeric Materials, and Molecular Energy Materials
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EFFICIENCY ,Science ,POWER ,THERMAL-CONDUCTIVITY ,General Physics and Astronomy ,02 engineering and technology ,HEAT ,010402 general chemistry ,01 natural sciences ,Article ,General Biochemistry, Genetics and Molecular Biology ,NANOSTRUCTURED THERMOELECTRICS ,Thermal conductivity ,DESIGN ,Electrical resistivity and conductivity ,DOPANT ,Thermoelectric effect ,Electronic devices ,Figure of merit ,lcsh:Science ,Thermoelectrics ,Multidisciplinary ,Dopant ,business.industry ,Thermoelectric devices and materials ,Doping ,POLYMER ,General Chemistry ,021001 nanoscience & nanotechnology ,Thermoelectric materials ,0104 chemical sciences ,Organic semiconductor ,Chemistry ,ELECTRONIC-STRUCTURE ,Physics and Astronomy ,MOBILITY ,Optoelectronics ,lcsh:Q ,0210 nano-technology ,business - Abstract
The ‘phonon-glass electron-crystal’ concept has triggered most of the progress that has been achieved in inorganic thermoelectrics in the past two decades. Organic thermoelectric materials, unlike their inorganic counterparts, exhibit molecular diversity, flexible mechanical properties and easy fabrication, and are mostly ‘phonon glasses’. However, the thermoelectric performances of these organic materials are largely limited by low molecular order and they are therefore far from being ‘electron crystals’. Here, we report a molecularly n-doped fullerene derivative with meticulous design of the side chain that approaches an organic ‘PGEC’ thermoelectric material. This thermoelectric material exhibits an excellent electrical conductivity of >10 S cm−1 and an ultralow thermal conductivity of, Achieved high thermoelectric figure of merit (ZT) in organic thermoelectric materials remains a challenge due to their low packing order and poor host/dopant miscibility. Here, the authors report side chain-engineered n-doped fullerene derivatives with record ZT >0.3 for organic thermoelectrics.
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- 2020
16. Infrared organic photodetectors employing ultralow bandgap polymer and non-fullerene acceptors for biometric monitoring
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Polina Jacoutot, Alberto D. Scaccabarozzi, Tianyi Zhang, Zhuoran Qiao, Filip Aniés, Marios Neophytou, Helen Bristow, Rhea Kumar, Maximilian Moser, Alkmini D. Nega, Andriana Schiza, Antonia Dimitrakopoulou‐Strauss, Vasilis G. Gregoriou, Thomas D. Anthopoulos, Martin Heeney, Iain McCulloch, Artem A. Bakulin, Christos L. Chochos, Nicola Gasparini, and The Royal Society
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Technology ,biometric sensors ,Infrared Rays ,Polymers ,Chemistry, Multidisciplinary ,Materials Science ,Materials Science, Multidisciplinary ,Physics, Applied ,Biomaterials ,CHARGE-TRANSFER ,NIR sensors ,Solar Energy ,General Materials Science ,Nanoscience & Nanotechnology ,Monitoring, Physiologic ,Science & Technology ,Chemistry, Physical ,Physics ,PHOTODIODES ,General Chemistry ,non-fullerene photodetectors ,organic photodetectors ,Chemistry ,Physics, Condensed Matter ,STATES ,very low bandgap polymers ,Physical Sciences ,Science & Technology - Other Topics ,Biotechnology - Abstract
Recent efforts in the field of organic photodetectors (OPD) have been focused on extending broadband detection into the near-infrared (NIR) region. Here, two blends of an ultralow bandgap push–pull polymer TQ-T combined with state-of-the-art non-fullerene acceptors, IEICO-4F and Y6, are compared to obtain OPDs for sensing in the NIR beyond 1100 nm, which is the cut off for benchmark Si photodiodes. It is observed that the TQ-T:IEICO-4F device has a superior IR responsivity (0.03 AW-1 at 1200 nm and −2 V bias) and can detect infrared light up to 1800 nm, while the TQ-T:Y6 blend shows a lower responsivity of 0.01 AW-1. Device physics analyses are tied with spectroscopic and morphological studies to link the superior performance of TQ-T:IEICO-4F OPD to its faster charge separation as well as more favorable donor–acceptor domains mixing. In the polymer blend with Y6, the formation of large agglomerates that exceed the exciton diffusion length, which leads to high charge recombination, is observed. An application of these devices as biometric sensors for real-time heart rate monitoring via photoplethysmography, utilizing infrared light, is demonstrated.
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- 2022
17. A Simple n-Dopant Derived from Diquat Boosts the Efficiency of Organic Solar Cells to 18.3%
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Abdul-Hamid M. Emwas, Osman M. Bakr, Thomas D. Anthopoulos, Leonidas Tsetseris, Emre Yengel, Mohamad Insan Nugraha, Jiakai Liu, Yuliar Firdaus, Xiaopeng Zheng, Martin Heeney, Filip Aniés, Hendrik Faber, Wandi Wahyudi, Emre Yarali, Yuanbao Lin, and Alberto D. Scaccabarozzi
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Materials science ,Organic solar cell ,Dopant ,Renewable Energy, Sustainability and the Environment ,Doping ,Energy Engineering and Power Technology ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Diquat ,0104 chemical sciences ,chemistry.chemical_compound ,Fuel Technology ,Chemical engineering ,chemistry ,Chemistry (miscellaneous) ,Materials Chemistry ,0210 nano-technology - Abstract
Molecular doping has recently been shown to improve the operating characteristics of organic photovoltaics (OPVs). Here, we prepare neutral Diquat (DQ) and use it as n-dopant to improve the perform...
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- 2020
18. Ledge-directed epitaxy of continuously self-aligned single-crystalline nanoribbons of transition metal dichalcogenides
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Thomas D. Anthopoulos, Wen-Hao Chang, Jui-Han Fu, Wei Ting Hsu, Vincent Tung, Dipti R Naphade, Rehab Albaridy, Lain-Jong Li, Mariam Hakami, Chen Tse-An, Jeehwan Kim, Zhen Cao, Emre Yengel, Steven Brems, Chien-Ju Lee, Chih-Piao Chuu, Chih-Chan Hsu, Areej Aljarb, Sang-Hoon Bae, Ming-Yang Li, Sergei Lopatin, and Yi Wan
- Subjects
Electron mobility ,Materials science ,Oxide ,02 engineering and technology ,Substrate (electronics) ,010402 general chemistry ,Epitaxy ,01 natural sciences ,law.invention ,chemistry.chemical_compound ,law ,Monolayer ,General Materials Science ,business.industry ,Mechanical Engineering ,Transistor ,Heterojunction ,General Chemistry ,021001 nanoscience & nanotechnology ,Condensed Matter Physics ,Exfoliation joint ,0104 chemical sciences ,chemistry ,Mechanics of Materials ,Optoelectronics ,0210 nano-technology ,business - Abstract
Two-dimensional transition metal dichalcogenide nanoribbons are touted as the future extreme device downscaling for advanced logic and memory devices but remain a formidable synthetic challenge. Here, we demonstrate a ledge-directed epitaxy (LDE) of dense arrays of continuous, self-aligned, monolayer and single-crystalline MoS2 nanoribbons on β-gallium (iii) oxide (β-Ga2O3) (100) substrates. LDE MoS2 nanoribbons have spatial uniformity over a long range and transport characteristics on par with those seen in exfoliated benchmarks. Prototype MoS2-nanoribbon-based field-effect transistors exhibit high on/off ratios of 108 and an averaged room temperature electron mobility of 65 cm2 V−1 s−1. The MoS2 nanoribbons can be readily transferred to arbitrary substrates while the underlying β-Ga2O3 can be reused after mechanical exfoliation. We further demonstrate LDE as a versatile epitaxy platform for the growth of p-type WSe2 nanoribbons and lateral heterostructures made of p-WSe2 and n-MoS2 nanoribbons for futuristic electronics applications. Aligned arrays of single-crystalline monolayer TMD nanoribbons with high aspect ratios, as well as their lateral heterostructures, are realized, with the growth directed by the ledges on the β-Ga2O3 substrate. This approach provides an epitaxy platform for advanced electronics applications of TMD nanoribbons.
- Published
- 2020
19. Colloidal Quantum Dot Photovoltaics Using Ultrathin, Solution-Processed Bilayer In2O3/ZnO Electron Transport Layers with Improved Stability
- Author
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Thomas D. Anthopoulos, Flurin Eisner, Ahmed M. Mansour, Edward H. Sargent, Aram Amassian, Mohamad Insan Nugraha, Yuliar Firdaus, Akmaral Seitkhan, Neha Chaturvedi, Ahmad R. Kirmani, F. Pelayo García de Arquer, and Emre Yarali
- Subjects
Materials science ,Ligand ,business.industry ,Bilayer ,Energy Engineering and Power Technology ,chemistry.chemical_element ,Nanotechnology ,Zinc ,Electron transport chain ,Solution processed ,Colloid ,chemistry ,Quantum dot ,Photovoltaics ,cardiovascular system ,Materials Chemistry ,Electrochemistry ,Chemical Engineering (miscellaneous) ,Electrical and Electronic Engineering ,business - Abstract
Solution-processed colloidal quantum dot (CQD) photovoltaics (PVs) continue to mature with improvements in device architectures and ligand exchange strategies. Carrier selective contacts extract ph...
- Published
- 2020
20. Thienyl Sidechain Substitution and Backbone Fluorination of Benzodithiophene-Based Donor Polymers Concertedly Minimize Carrier Losses in ITIC-Based Organic Solar Cells
- Author
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Thomas D. Anthopoulos, Shengjian Liu, Pierre M. Beaujuge, Yuliar Firdaus, Jafar Iqbal Khan, Federico Cruciani, and Frédéric Laquai
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chemistry.chemical_classification ,Quantitative Biology::Biomolecules ,Fullerene ,Organic solar cell ,Chemistry ,Substitution (logic) ,02 engineering and technology ,Polymer ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Photochemistry ,01 natural sciences ,Acceptor ,0104 chemical sciences ,Surfaces, Coatings and Films ,Electronic, Optical and Magnetic Materials ,Condensed Matter::Materials Science ,General Energy ,Physics::Atomic and Molecular Clusters ,Physics::Chemical Physics ,Physical and Theoretical Chemistry ,0210 nano-technology ,Computer Science::Formal Languages and Automata Theory - Abstract
Non-fullerene acceptor (NFA) based organic solar cells have outperformed fullerene-based devices, yet their photophysics is less well understood. Herein, changes in the donor polymer backbone side-...
- Published
- 2020
21. Solution-Processed Mixed-Dimensional Hybrid Perovskite/Carbon Nanotube Electronics
- Author
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Sarah Clark, Lain-Jong Li, Ran Tao, Thomas D. Anthopoulos, Zhixiong Liu, Tom Wu, Liangliang Liang, Xiaogang Liu, Chun Ma, Yuliar Firdaus, Mark C. Hersam, and Ali Han
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Materials science ,General Engineering ,General Physics and Astronomy ,Nanotechnology ,02 engineering and technology ,Carbon nanotube ,Methylammonium lead halide ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Solution processed ,law.invention ,chemistry.chemical_compound ,chemistry ,law ,Thin-film transistor ,General Materials Science ,Electronics ,0210 nano-technology ,Perovskite (structure) - Abstract
Benefiting from their extraordinary physical properties, methylammonium lead halide perovskites (PVKs) have attracted significant attention in optoelectronics. However, the PVK-based devices suffer from low carrier mobility and high operation voltage. Here, we utilize sorted semiconducting single-walled carbon nanotubes (95% s-SWCNTs) to enhance the performance of thin-film transistors (TFTs) based on the mixed-cation perovskite (MA
- Published
- 2020
22. Chlorine Vacancy Passivation in Mixed Halide Perovskite Quantum Dots by Organic Pseudohalides Enables Efficient Rec. 2020 Blue Light-Emitting Diodes
- Author
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Chun Zhou, Jun Yin, Thomas D. Anthopoulos, Xiaopeng Zheng, Yu Han, Mohamed N. Hedhili, Shuai Yuan, Liang-Sheng Liao, Kepeng Song, Jiakai Liu, Edward H. Sargent, Wan-Shan Shen, Zheng-Hong Lu, Hong-Tao Sun, Mingyang Wei, Fanglong Yuan, Yuanbao Lin, Omar F. Mohammed, Osman M. Bakr, Nimer Wehbe, Bin-Bin Zhang, and Ke Xin Yao
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Materials science ,Passivation ,Renewable Energy, Sustainability and the Environment ,Energy Engineering and Power Technology ,chemistry.chemical_element ,Halide ,Rec. 2020 ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Photochemistry ,01 natural sciences ,0104 chemical sciences ,Fuel Technology ,chemistry ,Chemistry (miscellaneous) ,Quantum dot ,Vacancy defect ,Materials Chemistry ,Chlorine ,0210 nano-technology ,Perovskite (structure) ,Diode - Abstract
Blue-emitting perovskites can be easily attained by precisely tuning the halide ratio of mixed halide (Br/Cl) perovskites (MHPs). However, the adjustable halide ratio hinders the passivation of Cl ...
- Published
- 2020
23. Electrolyte Engineering Enables High Stability and Capacity Alloying Anodes for Sodium and Potassium Ion Batteries
- Author
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Thomas D. Anthopoulos, Lin Zhou, Jun Ming, Husam N. Alshareef, Jang Yeon Hwang, Yang-Kook Sun, Wandi Wahyudi, Luigi Cavallo, Yong Cheng, Limin Wang, Jiao Zhang, and Zhen Cao
- Subjects
Materials science ,Renewable Energy, Sustainability and the Environment ,Sodium ,Potassium ,Energy Engineering and Power Technology ,chemistry.chemical_element ,02 engineering and technology ,Electrolyte ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Anode ,Fuel Technology ,chemistry ,Chemical engineering ,Chemistry (miscellaneous) ,Materials Chemistry ,Energy density ,0210 nano-technology - Abstract
Development of sodium and potassium ion batteries with greater energy density is gaining great attention. Although recently proposed alloying anodes (e.g., Sn and Bi) demonstrate much higher capaci...
- Published
- 2020
24. Impact of p-type doping on charge transport in blade-coated small-molecule:polymer blend transistors
- Author
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Alexandra F. Paterson, Aniruddha Basu, Alberto D. Scaccabarozzi, Olga V. Boltalina, Zuping Fei, Hendrik Faber, Muhammad Rizwan Niazi, Dalaver H. Anjum, Thomas D. Anthopoulos, and Martin Heeney
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Organic electronics ,chemistry.chemical_classification ,Electron mobility ,Fabrication ,Materials science ,business.industry ,Transistor ,Benzothiophene ,General Chemistry ,Polymer ,law.invention ,chemistry.chemical_compound ,chemistry ,law ,Compatibility (mechanics) ,Materials Chemistry ,Optoelectronics ,Polymer blend ,business - Abstract
Blade-coating is a roll-to-roll (R2R) compatible processing technique and has the potential to address the industry's needs for scalable manufacturing of future organic electronics. Here we investigate the applicability of blade-coating for the fabrication of organic thin-film transistors (OTFTs) based on best-in-class organic semiconducting blends comprised of the conjugated small-molecule 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene (C8-BTBT), and the conjugated polymer poly(indacenodithiophene-co-benzothiadiazole) (C16IDT-BT). We show that the operating characteristics of blade-coated transistors consistently outperform devices prepared via spin-coating, showcasing the compatibility of the technique. Introducing the molecular p-dopant C60F48 into the binary C8-BTBT:C16IDT-BT blend formulation, in combination with carefully optimized blade-coating conditions, helps to enhance the performance of the ensuing transistors further resulting in a maximum hole mobility of ≈14 cm2 V−1 s−1, and an all-around improvement of the device operating characteristics. Our results show that p-doped blend OTFTs can be manufactured using industry relevant processing techniques without sacrificing their state-of-the-art performance.
- Published
- 2020
25. Liquid phase exfoliation of MoS2 and WS2 in aqueous ammonia and their application in highly efficient organic solar cells
- Author
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Begimai Adilbekova, Abdulrahman El-Labban, Yuanbao Lin, Yuliar Firdaus, Emre Yengel, Hendrik Faber, Thomas D. Anthopoulos, Vincent Tung, Dalaver H. Anjum, and George T. Harrison
- Subjects
Aqueous solution ,Materials science ,Organic solar cell ,Tungsten disulfide ,Energy conversion efficiency ,General Chemistry ,Environmentally friendly ,Exfoliation joint ,chemistry.chemical_compound ,chemistry ,Transition metal ,Chemical engineering ,Materials Chemistry ,Molybdenum disulfide - Abstract
Simple, scalable and cost-effective synthesis of quality two-dimensional (2D) transition metal dichalcogenides (TMDs) is critical for fundamental investigations but also for the widespread adoption of these low-dimensional materials in an expanding range of device applications. Here, we report on the liquid-phase exfoliation (LPE) of molybdenum disulfide (MoS2) and tungsten disulfide (WS2) in aqueous ammonia (NH3(aq.)) as a greener alternative to commonly used but less environmentally friendly solvents. The synthesized nanosheets can be prepared in high concentrations (0.5–1 mg mL−1) and exhibit excellent stoichiometric and structural quality with a semiconducting character. These characteristics make them ideal for application in organic optoelectronics, where optical transparency and suitable energetics are two important prerequisites. When MoS2 and WS2 are used as the hole transport layer materials in organic photovoltaics, cells with a power conversion efficiency of 14.9 and 15.6%, respectively, are obtained, highlighting the potential of the aqueous ammonia-based LPE method for the preparation of high quality TMDs. The method could potentially be extended to other TMDs.
- Published
- 2020
26. Hybrid organic–metal oxide multilayer channel transistors with high operational stability
- Author
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Nikolaos A. Hastas, N. Pliatsikas, Xixiang Zhang, Wei Huang, Panos Patsalas, Leonidas Tsetseris, Donal D. C. Bradley, Wen Li, Hendrik Faber, Thomas D. Anthopoulos, Akmaral Seitkhan, Qiang Zhang, Yen-Hung Lin, and Dongyoon Khim
- Subjects
Electron mobility ,Materials science ,Oxide ,FOS: Physical sciences ,chemistry.chemical_element ,Nanoparticle ,Applied Physics (physics.app-ph) ,02 engineering and technology ,Zinc ,010402 general chemistry ,7. Clean energy ,01 natural sciences ,law.invention ,chemistry.chemical_compound ,law ,Electrical and Electronic Engineering ,Instrumentation ,Condensed Matter - Materials Science ,business.industry ,Doping ,Transistor ,Materials Science (cond-mat.mtrl-sci) ,Physics - Applied Physics ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,Electronic, Optical and Magnetic Materials ,chemistry ,Optoelectronics ,Polystyrene ,0210 nano-technology ,business ,Indium - Abstract
Metal oxide thin-film transistors are fast becoming a ubiquitous technology for application in driving backplanes of organic light-emitting diode displays. Currently all commercial products rely on metal oxides processed via physical vapor deposition methods. Transition to simpler, higher throughput manufacturing methods such as solution-based processes, are currently been explored as cost-effective alternatives. However, developing printable oxide transistors with high carrier mobility and bias-stable operation has proved challenging. Here we show that hybrid multilayer channels composed of alternating ultra-thin layers ($\leq$4 nm) of indium oxide, zinc oxide nanoparticles, ozone-treated polystyrene and a compact zinc oxide layer, all solution-processed in ambient atmosphere, can be used to create TFTs with remarkably high electron mobility (50 cm$^{2}$/Vs) and record operational stability. Insertion of the ozone-treated polystyrene interlayer is shown to reduce the concentration of electron traps at the metal oxide surfaces and heterointerfaces. The resulting transistors exhibit dramatically enhanced bias stability over 24 h continuous operation and while subjected to large electric field flux density (2.1$\times$10$^{-6}$ C/cm$^{2}$) with no adverse effects on the electron mobility. Density functional theory calculations identify the origin of this enhanced stability as the passivation of the oxygen vacancy-related gap states due to interaction between ozonolyzed styrene moieties and the oxides. Our results sets new design guidelines for bias-stress resilient metal oxide transistors.
- Published
- 2019
27. Low-Temperature Cross-Linking Benzocyclobutene Based Polymer Dielectric for Organic Thin Film Transistors on Plastic Substrates
- Author
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Maud V. C. Jenart, Alexandra F. Paterson, Helen Bristow, Rawad K. Hallani, Marios Neophytou, Hendrik Faber, Maximilian Moser, Thomas D. Anthopoulos, Emre Yarali, and Iain McCulloch
- Subjects
chemistry.chemical_classification ,chemistry.chemical_compound ,Differential scanning calorimetry ,chemistry ,Benzocyclobutene ,Thin-film transistor ,Organic Chemistry ,Substituent ,Polymer ,Dielectric ,Composite material ,Fourier transform infrared spectroscopy ,Curing (chemistry) - Abstract
The synthesis of a new benzocyclobutene based polymer, PSBBB, designed as a dielectric material for use in organic thin film transistors was reported. Compared to conventional benzocyclobutene-based materials, the introduction of a butoxide substituent at the 7-position of the benzocyclobutene pendant unit on the polymer allowed PSBBB to be cross-linked at temperatures of 120 °C, thus rendering it compatible with the processing requirements of flexible plastic substrates. The cross-linking behavior of PSBBB was investigated by Fourier transform infrared spectroscopy and differential scanning calorimetry, demonstrating cross-linking of the polymer after curing at 120 °C. Bottom-gate bottom-contact organic thin film transistors were fabricated using PSBBB as dielectric, affording a performance comparable to that of other dielectric polymeric materials.
- Published
- 2019
28. 14 GHz Schottky Diodes Using a p-Doped Organic Polymer
- Author
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Kalaivanan Loganathan, Alberto D. Scaccabarozzi, Hendrik Faber, Federico Ferrari, Zhanibek Bizak, Emre Yengel, Dipti R. Naphade, Murali Gedda, Qiao He, Olga Solomeshch, Begimai Adilbekova, Emre Yarali, Leonidas Tsetseris, Khaled N. Salama, Martin Heeney, Nir Tessler, and Thomas D. Anthopoulos
- Subjects
Technology ,EFFICIENCY ,Chemistry, Multidisciplinary ,Materials Science ,Schottky diodes ,Materials Science, Multidisciplinary ,09 Engineering ,Physics, Applied ,General Materials Science ,Nanoscience & Nanotechnology ,Organic semiconductor ,Science & Technology ,02 Physical Sciences ,Chemistry, Physical ,radio frequency electronics ,Mechanical Engineering ,Physics ,TRANSPORT ,Chemistry ,Physics, Condensed Matter ,Mechanics of Materials ,Physical Sciences ,TRANSISTORS ,Science & Technology - Other Topics ,printed electronics ,rectifier circuits ,03 Chemical Sciences - Abstract
The low carrier mobility of organic semiconductors and the high parasitic resistance and capacitance often encountered in conventional organic Schottky diodes, hinder their deployment in emerging radio frequency (RF) electronics. Here we overcome these limitations by combining self-aligned asymmetric nanogap electrodes (∼25 nm) produced by adhesion-lithography, with a high mobility organic semiconductor and demonstrate RF Schottky diodes able to operate in the 5G frequency spectrum. We used C16 IDT-BT, as the high hole mobility polymer, and studied the impact of p-doping on the diode performance. Pristine C16 IDT-BT-based diodes exhibit maximum intrinsic and extrinsic cutoff frequencies (fC ) of >100 and 6 GHz, respectively. This extraordinary performance is attributed primarily to the planar nature of the nanogap channel and the diode's small junction capacitance (< 2 pF). Doping of C16 IDT-BT with the molecular p-dopant C60 F48 , improves the diode's performance further by reducing the series resistance resulting to intrinsic and extrinsic fC of >100 and ∼14 GHz respectively, while the DC output voltage of a RF rectifier circuit increases by a tenfold. Our work highlights the importance of the planar nanogap architecture and paves the way for the use of organic Schottky diodes in large-area radio frequency electronics of the future. This article is protected by copyright. All rights reserved.
- Published
- 2021
29. A tri-channel oxide transistor concept for the rapid detection of biomolecules including the SARS-CoV-2 spike protein
- Author
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Po-Yu Lu, Thomas D. Anthopoulos, Wejdan S. Alghamdi, Pichaya Pattanasattayavong, Abhinav Sharma, Xi-Wen Xiao, Chien-Hao Liu, Martin Heeney, Yang Han, Hendrik Faber, Yen-Hung Lin, Akmaral Seitkhan, Alexander D. Mottram, Tzu-Hsuan Chang, and Wei-Zhi Lin
- Subjects
Analyte ,Electron mobility ,Materials science ,Transistors, Electronic ,Oxide ,Nanotechnology ,Bioengineering ,Biosensing Techniques ,Antibodies, Viral ,Indium ,Proof of Concept Study ,SARS‐CoV‐2 ,law.invention ,chemistry.chemical_compound ,COVID-19 Testing ,law ,Computer Systems ,metal oxide semiconductors ,solid‐state devices ,Humans ,General Materials Science ,Computer Simulation ,Research Articles ,chemistry.chemical_classification ,solution process ,SARS-CoV-2 ,Mechanical Engineering ,Biomolecule ,Transistor ,COVID-19 ,Heterojunction ,large‐area electronics ,DNA ,Equipment Design ,chemistry ,Mechanics of Materials ,Spike Glycoprotein, Coronavirus ,Microtechnology ,transistors sensors ,Angiotensin-Converting Enzyme 2 ,Zinc Oxide ,Biosensor ,Antibodies, Immobilized ,Communication channel ,Research Article - Abstract
Solid‐state transistor sensors that can detect biomolecules in real time are highly attractive for emerging bioanalytical applications. However, combining upscalable manufacturing with the required performance remains challenging. Here, an alternative biosensor transistor concept is developed, which relies on a solution‐processed In2O3/ZnO semiconducting heterojunction featuring a geometrically engineered tri‐channel architecture for the rapid, real‐time detection of important biomolecules. The sensor combines a high electron mobility channel, attributed to the electronic properties of the In2O3/ZnO heterointerface, in close proximity to a sensing surface featuring tethered analyte receptors. The unusual tri‐channel design enables strong coupling between the buried electron channel and electrostatic perturbations occurring during receptor–analyte interactions allowing for robust, real‐time detection of biomolecules down to attomolar (am) concentrations. The experimental findings are corroborated by extensive device simulations, highlighting the unique advantages of the heterojunction tri‐channel design. By functionalizing the surface of the geometrically engineered channel with severe acute respiratory syndrome coronavirus 2 (SARS‐CoV‐2) antibody receptors, real‐time detection of the SARS‐CoV‐2 spike S1 protein down to am concentrations is demonstrated in under 2 min in physiological relevant conditions., A solution‐processed metal oxide heterojunction channel with a geometrically engineered tri‐channel architecture several millimeters in size, is developed and used as a generic platform for robust, selective, and ultrasensitive detection of various biomolecules. As a proof‐of‐concept, selective sensing of the SARS‐CoV‐2 spike protein down to attomolar concentrations in under 2 min is demonstrated.
- Published
- 2021
30. Doping Approaches for Organic Semiconductors
- Author
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Filip Aniés, Alberto D. Scaccabarozzi, Ross Warren, Mohamad Insan Nugraha, Jian Liu, Yuliar Firdaus, Mariano Campoy-Quiles, Thomas D. Anthopoulos, Aniruddha Basu, Osnat Zapata-Arteaga, Yuanbao Lin, Christian Müller, Norbert Koch, Martin Heeney, Leonidas Tsetseris, King Abdullah University of Science and Technology, Wilkinson Charitable Foundation, Swedish Research Council, and Knut and Alice Wallenberg Foundation
- Subjects
Charge transfer ,Work (electrical) ,Semiconductors ,Chemistry ,Research council ,Foundation (engineering) ,Doping ,General Chemistry ,Molecules ,Management ,Impurities - Abstract
This article is part of the Organic Bioelectronics special issue., Electronic doping in organic materials has remained an elusive concept for several decades. It drew considerable attention in the early days in the quest for organic materials with high electrical conductivity, paving the way for the pioneering work on pristine organic semiconductors (OSCs) and their eventual use in a plethora of applications. Despite this early trend, however, recent strides in the field of organic electronics have been made hand in hand with the development and use of dopants to the point that are now ubiquitous. Here, we give an overview of all important advances in the area of doping of organic semiconductors and their applications. We first review the relevant literature with particular focus on the physical processes involved, discussing established mechanisms but also newly proposed theories. We then continue with a comprehensive summary of the most widely studied dopants to date, placing particular emphasis on the chemical strategies toward the synthesis of molecules with improved functionality. The processing routes toward doped organic films and the important doping–processing–nanostructure relationships, are also discussed. We conclude the review by highlighting how doping can enhance the operating characteristics of various organic devices., This work was from King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) under award nos. OSR-2018-CARF/CCF-3079 and OSR-2019- CRG8-4095.3. F.A. acknowledges the support from The Wilkinson Charitable Foundation. C.M. acknowledges financial support from the Swedish Research Council (grant no. 2018- 03824) and the Knut and Alice Wallenberg Foundation through a Wallenberg Academy Fellowship Prolongation grant.
- Published
- 2021
31. Planar refractive index patterning through microcontact photo-thermal annealing of a printable organic/inorganic hybrid material
- Author
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Hua-Kang Yuan, Natalie Stingelin, Kornelius Tetzner, Stefan Bachevillier, Thomas D. Anthopoulos, Paul N. Stavrinou, and Donal D. C. Bradley
- Subjects
chemistry.chemical_classification ,Vinyl alcohol ,Fabrication ,Materials science ,business.industry ,Annealing (metallurgy) ,Process Chemistry and Technology ,02 engineering and technology ,Polymer ,Photothermal therapy ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Titanium oxide ,chemistry.chemical_compound ,chemistry ,Mechanics of Materials ,Optoelectronics ,General Materials Science ,Electrical and Electronic Engineering ,0210 nano-technology ,Hybrid material ,business ,Refractive index - Abstract
We demonstrate proof-of-concept refractive-index structures with large refractive-index-gradient profiles, using a micro-contact photothermal annealing (μCPA) process to pattern organic/inorganic hybrid materials comprising titanium oxide hydrate within a poly(vinyl alcohol) binder. A significant refractive index modulation of up to Δn ≈ +0.05 can be achieved with μCPA within less than a second of pulsed lamp exposure, which promises the potential for a high throughput fabrication process of photonic structures with a polymer-based system.
- Published
- 2021
32. Significant performance improvement in n-channel organic field-effect transistors with C60:C70 co-crystals induced by poly(2-ethyl-2-oxazoline) nanodots
- Author
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Sungho Nam, Youngkyoo Kim, Peter D. Nellist, Aakash Varambhia, Thomas D. Anthopoulos, Dongyoon Khim, Gerardo T. Martinez, and Donal D. C. Bradley
- Subjects
chemistry.chemical_classification ,Electron mobility ,Materials science ,Fullerene ,business.industry ,Mechanical Engineering ,02 engineering and technology ,Polymer ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Flexible electronics ,0104 chemical sciences ,Semiconductor ,chemistry ,Chemical engineering ,Mechanics of Materials ,General Materials Science ,Field-effect transistor ,Work function ,Nanodot ,0210 nano-technology ,business - Abstract
Solution-processed organic field-effect transistors (OFETs) have attracted great interest due to their potential as logic devices for bendable and flexible electronics. In relation to n-channel structures, soluble fullerene semiconductors have been widely studied. However, they have not yet met the essential requirements for commercialization, primarily because of low charge carrier mobility, immature large-scale fabrication processes, and insufficient long-term operational stability. Interfacial engineering of the carrier-injecting source/drain (S/D) electrodes has been proposed as an effective approach to improve charge injection, leading also to overall improved device characteristics. Here, it is demonstrated that a non-conjugated neutral dipolar polymer, poly(2-ethyl-2-oxazoline) (PEOz), formed as a nanodot structure on the S/D electrodes, enhances electron mobility in n-channel OFETs using a range of soluble fullerenes. Overall performance is especially notable for (C60 -Ih )[5,6]fullerene (C60 ) and (C70 -D5h(6) )[5,6]fullerene (C70 ) blend films, with an increase from 0.1 to 2.1 cm2 V-1 s-1 . The high relative mobility and eighteen-fold improvement are attributed not only to the anticipated reduction in S/D electrode work function but also to the beneficial effects of PEOz on the formation of a face-centered-cubic C60 :C70 co-crystal structure within the blend films.
- Published
- 2021
33. Self-Powered Perovskite/CdS Heterostructure Photodetectors
- Author
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Zibo Li, Thomas D. Anthopoulos, Jieni Li, Ye Wang, Chun Ma, Ke Jiang, Henan Li, Shangchi Jiang, Yumeng Shi, and Dong Ding
- Subjects
Materials science ,business.industry ,Photodetector ,Heterojunction ,02 engineering and technology ,Methylammonium lead halide ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,chemistry.chemical_compound ,chemistry ,Optoelectronics ,General Materials Science ,0210 nano-technology ,business ,Photoconductive atomic force microscopy ,Perovskite (structure) - Abstract
Methylammonium lead halide perovskites have gained a lot of attention because of their remarkable physical properties and potential for numerous (opto)electronic applications. Here, high-performance photodetectors based on CH
- Published
- 2019
34. Performance and Stability Improvement of Layered NCM Lithium-Ion Batteries at High Voltage by a Microporous Al2O3 Sol–Gel Coating
- Author
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Xiaohe Miao, Kuo-Wei Huang, Mengliu Li, Guan Sheng, Yangxing Li, Wandi Wahyudi, Thomas D. Anthopoulos, Zhiping Lai, and Yingqiang Wu
- Subjects
chemistry.chemical_classification ,Materials science ,General Chemical Engineering ,chemistry.chemical_element ,High voltage ,General Chemistry ,Microporous material ,Polymer ,Sol gel coating ,Polyvinyl alcohol ,Article ,Cathode ,Ion ,law.invention ,chemistry.chemical_compound ,Chemistry ,chemistry ,Chemical engineering ,law ,Lithium ,QD1-999 - Abstract
A simple and low-cost polymer-aided sol–gel method was developed to prepare γ-Al2O3 protective layers for LiNi0.6Co0.2Mn0.2O2 (NCM622) cathode materials. The selected polyvinyl alcohol polymer additive not only facilitates the formation of a uniform and thin γ-Al2O3 layer on the irregular and rough cathode particle surface to protect it from corrosion but also serves as a pore-forming agent to generate micropores in the film after sintering to allow fast transport of lithium ions, which guaranteed the excellent and stable battery performance at high working voltage. Detailed studies in the full battery mode showed that the leached corrosion species from the cathode had a more profound harmful effect to the graphite anode, which seemed to be the dominating factor that caused the battery performance decay.
- Published
- 2019
35. One-step growth of reduced graphene oxide on arbitrary substrates
- Author
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Mingguang Chen, Thomas D. Anthopoulos, Emre Yengel, Junwei Zhang, Jing-Kai Huang, Chenxu Zhu, Chenhui Zhang, Mohamed N. Hedhili, Xixiang Zhang, and Xin He
- Subjects
Materials science ,Graphene ,business.industry ,Oxide ,Photodetector ,One-Step ,Nanotechnology ,02 engineering and technology ,General Chemistry ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,0104 chemical sciences ,Catalysis ,law.invention ,chemistry.chemical_compound ,chemistry ,law ,General Materials Science ,Field-effect transistor ,Electronics ,Photonics ,0210 nano-technology ,business - Abstract
Reduced graphene oxide (rGO) has inherited the outstanding electronic, optical, thermal and mechanical properties of graphene to a large extent, while maintaining sufficient chemically active sites. Therefore, it has attracted a great deal of research attention in the fields of energy storage, electronics, photonics, catalysis, environmental engineering, etc. Currently, the most popular way to prepare rGO is to reduce graphene oxide, which is obtained by modified Hummer methods using tedious treatments in a harsh environment, to rGO flakes. Industrial applications demand advanced preparation methods that can mass produce highly uniform rGO sheets on arbitrary substrates. In this work, a one-step growth process is introduced that utilizes cellulose acetate as a precursor, without any catalysts, to produce uniform ultrathin rGO films on various substrates and free-standing rGO powders. Systematic spectroscopic and microscopic studies on the resulting rGO are performed. Prototypes of electronic and optoelectronic devices, such as field effect transistors (FETs), photodetectors, and humidity sensors, are fabricated and tested, demonstrating the intriguing applications of our rGO materials across a wide range of fields.
- Published
- 2019
36. Highly sensitive and room temperature detection of ultra-low concentrations of O3 using self-powered sensing elements of Cu2O nanocubes
- Author
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Thomas D. Anthopoulos, E. Petromichelaki, E. Gagaoudakis, K. Moschovis, George Kiriakidis, Leonidas Tsetseris, and Vassilios Binas
- Subjects
Diffraction ,Ozone ,Materials science ,Scanning electron microscope ,business.industry ,General Engineering ,Bioengineering ,General Chemistry ,Trapping ,Atomic and Molecular Physics, and Optics ,Metal ,chemistry.chemical_compound ,chemistry ,Transmission electron microscopy ,visual_art ,visual_art.visual_art_medium ,Optoelectronics ,General Materials Science ,Density functional theory ,business ,Deposition (law) - Abstract
The fundamental development of the design of novel self-powered ozone sensing elements, operating at room temperature, based on p-type metal oxides paves the way to a new class of low cost, highly promising gas sensing devices. In this work, p-type Cu2O nanocubes were synthesized by a simple solution-based method and tested as a self-powered ozone sensing element, at room temperature (25 °C) for the first time. Highly crystalline Cu2O nanocubes with 30 nm size were characterized by X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy (TEM). Self-powered sensing elements of Cu2O nanocubes have been successfully fabricated by deposition of Cu2O nanocubes on interdigitated electrodes (IDEs) consisting of two connection tracks with 500 digits and a gap of 5 μm in order to investigate their response to ozone at room temperature. The experimental results showed that the use of nanocubes as sensing elements was suitable for detecting ultra-low concentrations of O3 down to 10 ppb at room temperature with very high sensitivity (28%) and a very low response/recovery time. The reversible sensing process of the relatively weak binding of O3 species by trapping sites on Cu2O facets with increased oxygen content was studied by using density functional theory (DFT) calculations.
- Published
- 2019
37. Zinc oxide solution-processed Schottky diodes operating at 5G frequencies
- Author
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James Semple, Thomas D. Anthopoulos, Abhay A. Sagade, and Dimitra G. Georgiadou
- Subjects
Materials science ,business.industry ,chemistry.chemical_element ,Schottky diode ,Zinc ,Cutoff frequency ,chemistry ,Hardware_GENERAL ,Electrode ,Hardware_INTEGRATEDCIRCUITS ,Optoelectronics ,Wafer ,business ,Lithography ,5G ,Diode - Abstract
5G networks are currently being deployed around the world, introducing a new era in machine-to-machine communications and reinforcing the Internet of Things. The 5G radiofrequency bands range from sub-1 GHz to 70 GHz, while the 6th generation (6G) is expected to cover bands at hundreds of GHz. There is a need for devices with high frequency performance and scalable manufacturing using inexpensive techniques and materials. Herein we present ZnO-based Schottky diodes, processed from solution on wafer scale with high yield. Coplanar nanogap electrodes are fabricated using a high-throughput low-cost technique, named adhesion lithography. The diodes’ cutoff frequency exceeds 100 GHz.
- Published
- 2021
38. An all-solid-state heterojunction oxide transistor for the rapid detection of biomolecules and SARS-CoV-2 spike S1 protein
- Author
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Tzu-Hsuan Chang, Pichaya Pattanasattayavong, Xi-Wen Xiao, Yen-Hung Lin, Thomas D. Anthopoulos, Martin Heeney, Alexander D. Mottram, Abhinav Sharma, Yang Han, Wejdan S. Alghamdi, Chien-Hao Liu, Hendrik Faber, and Akmaral Seitkhan
- Subjects
chemistry.chemical_classification ,Analyte ,Electron mobility ,Materials science ,business.industry ,Biomolecule ,Severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) ,Transistor ,Oxide ,Heterojunction ,law.invention ,chemistry.chemical_compound ,chemistry ,law ,Optoelectronics ,Spike (software development) ,business - Abstract
Solid-state transistor sensors that can detect biomolecules in real time are highly attractive for emerging bioanalytical applications. However, combining cost-effective manufacturing with high sensitivity, specificity and fast sensing response, remains challenging. Here we develop low-temperature solution-processed In2O3/ZnO heterojunction transistors featuring a geometrically engineered tri-channel architecture for rapid real-time detection of different biomolecules. The sensor combines a high electron mobility channel, attributed to the quasi-two-dimensional electron gas (q2DEG) at the buried In2O3/ZnO heterointerface, in close proximity to a sensing surface featuring tethered analyte receptors. The unusual tri-channel design enables strong coupling between the buried q2DEG and the minute electronic perturbations occurring during receptor-analyte interactions allowing for robust, real-time detection of biomolecules down to attomolar (aM) concentrations. By functionalizing the tri-channel surface with SARS-CoV-2 (Severe Acute Respiratory Syndrome Coronavirus 2) antibody receptors, we demonstrate real-time detection of the SARS-CoV-2 spike S1 protein down to attomolar concentrations in under two minutes.
- Published
- 2021
39. Over 14% efficiency all-polymer solar cells enabled by a low bandgap polymer acceptor with low energy loss and efficient charge separation
- Author
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Thomas D. Anthopoulos, Feng Liu, Qiaoshi An, Olle Inganäs, Yuxin Xia, Wenyan Su, Qunping Fan, Chunfeng Zhang, Lintao Hou, Qian Li, Fujun Zhang, Ergang Wang, Weiguo Zhu, Min Xiao, Wenhong Peng, Donghong Yu, Yuanbao Lin, Ellen Moons, and Ming Zhang
- Subjects
chemistry.chemical_classification ,Materials science ,Renewable Energy, Sustainability and the Environment ,Band gap ,business.industry ,Energy conversion efficiency ,Polymer ,Condensed Matter Physics ,Pollution ,Acceptor ,Polymer solar cell ,Nuclear Energy and Engineering ,chemistry ,Physical Sciences ,Environmental Chemistry ,Optoelectronics ,Fysik ,business ,Absorption (electromagnetic radiation) ,HOMO/LUMO ,Current density ,Den kondenserade materiens fysik - Abstract
Obtaining both high open-circuit voltage (V-oc) and short-circuit current density (J(sc)) has been a major challenge for efficient all-polymer solar cells (all-PSCs). Herein, we developed a polymer acceptor PF5-Y5 with excellent optical absorption capability (onset extending to similar to 880 nm and maximum absorption coefficient exceeding 105 cm(-1) in a film), high electron mobility (3.18 x 10(3) cm(2) V-1 s(-1)) and high LUMO level (-3.84 eV) to address such a challenge. As a result, the PBDB-T:PF5-Y5-based all-PSCs achieved a high power conversion efficiency of up to 14.45% with both a high Voc (0.946 V) and a high Jsc (20.65 mA cm(-2)), due to the high and broad absorption coverage, small energy loss (0.57 eV) and efficient charge separation and transport in the device, which are among the best values in the all-PSC field. In addition, the all-PSC shows a similar to 15% improvement in PCE compared to its counterpart small molecule acceptor (Y5)-based device. Our results suggest that PF5-Y5 is a very promising polymer acceptor candidate for applications in efficient all-PSCs. Funding Agencies|Swedish Research CouncilSwedish Research Council [2015-04853, 2016-06146, 2019-04683]; Swedish Research Council FormasSwedish Research CouncilSwedish Research Council Formas; Wallenberg Foundation [2017.0186, 2016.0059]; Innovation fund Denmark (INKA project); Sino-Danish Centre for Education and Research (SDC); King Abdullah University of Science and Technology (KAUST)King Abdullah University of Science & Technology [OSR-2018-CARF/CCF-3079]; Office of Sponsored Research (OSR) [OSR-2018-CARF/CCF-3079]; Jinan University Postdoctoral Science Foundation; China Postdoctoral Science FoundationChina Postdoctoral Science Foundation [2020M673054]; National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [22005121, 61805009]
- Published
- 2020
40. Heterojunction oxide thin-film transistors
- Author
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Thomas D. Anthopoulos, Emre Yarali, Emre Yengel, and Hendrik Faber
- Subjects
chemistry.chemical_compound ,Materials science ,chemistry ,business.industry ,Thin-film transistor ,Oxide ,Optoelectronics ,Heterojunction ,business - Published
- 2020
41. Over 18% ternary polymer solar cells enabled by a terpolymer as the third component
- Author
-
Sang Young Jeong, Thomas D. Anthopoulos, Vytautas Getautis, Wenhong Peng, Wandi Wahyudi, Han Young Woo, Ergang Wang, Zewdneh Genene, Yuanbao Lin, Artiom Magomedov, Jiyong Deng, Qiang Tao, Cailing Chen, Weiguo Zhu, Yu Han, and „Elsevier Science' grupė
- Subjects
chemistry.chemical_classification ,Materials science ,Ternary numeral system ,terpolymer donor ,Organic solar cell ,Renewable Energy, Sustainability and the Environment ,Energy conversion efficiency ,Photovoltaic system ,Polymer ,ternary organic solar cells ,Miscibility ,Polymer solar cell ,high efficiency ,Chemical engineering ,chemistry ,conjugated polymers ,General Materials Science ,Electrical and Electronic Engineering ,Ternary operation ,compatible - Abstract
“Ternary blending” and “random terpolymerization” strategies have both proven effective for enhancing the performance of organic solar cells (OSCs). However, reports on the combination of the two strategies remain rare. Here, a terpolymer PM6-Si30 was constructed by inserting chlorine and alkylsilyl-substituted benzodithiophene (BDT) unit (0.3 equivalent) into the state-of-the-art polymer PM6. The terpolymer exhibits deep highest-occupied-molecular-orbital and good miscibility with both PM6 and BTP-eC9 and enables its use as a third component into PM6:PM6-Si30:BTP-eC9 bulk-heterojunction for OSCs. The resulting cells exhibit maximum power conversion efficiency (PCE) of 18.27%, which is higher than that obtained for the optimized control binary PM6:C9-based OSC (17.38%). The enhanced performance of the PM6:PM6-Si30:BTP-eC9 cells is attributed to improved charge transport, favorable molecular arrangement, reduced energy loss and suppressed bimolecular recombination. The work demonstrates the potential of random terpolymer as a third component in OSCs and highlights a new strategy for the construction of a ternary system with improved photovoltaic performance.
- Published
- 2022
42. Amphipathic Side Chain of a Conjugated Polymer Optimizes Dopant Location toward Efficient N-Type Organic Thermoelectrics
- Author
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Thomas D. Anthopoulos, Chen Yao, Ryan C. Chiechi, Derya Baran, Hinderikus G. O. Potgieser, Remco W. A. Havenith, Diego Rosas Villalva, Giuseppe Portale, Jingjin Dong, Selim Sami, L. Jan Anton Koster, Gang Ye, Jian Liu, Marten Koopmans, Simone Fabiano, Xinkai Qiu, Hengda Sun, Xuwen Yang, Mohamad Insan Nugraha, Photophysics and OptoElectronics, Molecular Energy Materials, Theoretical Chemistry, and Macromolecular Chemistry & New Polymeric Materials
- Subjects
Materials science ,organic thermoelectrics ,Library science ,02 engineering and technology ,010402 general chemistry ,01 natural sciences ,MECHANISMS ,Polymerkemi ,conjugated polymers ,General Materials Science ,dopant location ,N‐ type doping ,Seebeck coefficient ,solution processing ,Mechanical Engineering ,type doping ,Polymer Chemistry ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,Chemistry ,Scholarship ,N‐ ,Mechanics of Materials ,Research council ,N-type doping ,0210 nano-technology - Abstract
There is no molecular strategy for selectively increasing the Seebeck coefficient without reducing the electrical conductivity for organic thermoelectrics. Here, it is reported that the use of amphipathic side chains in an n-type donor-acceptor copolymer can selectively increase the Seebeck coefficient and thus increase the power factor by a factor of approximate to 5. The amphipathic side chain contains an alkyl chain segment as a spacer between the polymer backbone and an ethylene glycol type chain segment. The use of this alkyl spacer does not only reduce the energetic disorder in the conjugated polymer film but can also properly control the dopant sites away from the backbone, which minimizes the adverse influence of counterions. As confirmed by kinetic Monte Carlo simulations with the host-dopant distance as the only variable, a reduced Coulombic interaction resulting from a larger host-dopant distance contributes to a higher Seebeck coefficient for a given electrical conductivity. Finally, an optimized power factor of 18 mu W m(-1) K-2 is achieved in the doped polymer film. This work provides a facile molecular strategy for selectively improving the Seebeck coefficient and opens up a new route for optimizing the dopant location toward realizing better n-type polymeric thermoelectrics. Funding Agencies|STW/NWOTechnologiestichting STWNetherlands Organization for Scientific Research (NWO) [VIDI 13476]; China Scholarship CouncilChina Scholarship Council; Center for Information Technology of the University of Groningen; Swedish Research CouncilSwedish Research Council [2016-03979]; Olle Engkvists Stiftelse [204-0256]; Advanced Functional Materials center at LiU [2009 00971]; King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) [OSR-CRG2018-3737]; NWO Exact and Natural Sciences [2020/ENW/00852342]
- Published
- 2020
43. Low Temperature Scalable Deposition of Copper(I) Thiocyanate Films via Aerosol-Assisted Chemical Vapor Deposition
- Author
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Lokeshwari Mohan, Sinclair R. Ratnasingham, Martyn A. McLachlan, Joe Briscoe, Julianna Panidi, Thomas D. Anthopoulos, and Russell Binions
- Subjects
0306 Physical Chemistry (incl. Structural) ,Materials science ,Thiocyanate ,business.industry ,Band gap ,chemistry.chemical_element ,General Chemistry ,Chemical vapor deposition ,Condensed Matter Physics ,Copper ,chemistry.chemical_compound ,Semiconductor ,chemistry ,Copper(I) thiocyanate ,Chemical engineering ,Thin-film transistor ,0302 Inorganic Chemistry ,Deposition (phase transition) ,General Materials Science ,Inorganic & Nuclear Chemistry ,business ,0912 Materials Engineering - Abstract
Copper(I) thiocyanate (CuSCN) is a stable, wide bandgap (>3.5 eV), low-cost p-type semiconductor widely used in a variety of optoelectronic applications, including thin film transistors, organic light-emitting diodes, and photovoltaic cells. For CuSCN to have impact in the commercial fabrication of such devices, large-area, low-cost deposition techniques are required. Here, we report a novel technique for deposition of CuSCN that addresses these challenges. Aerosol-assisted chemical vapor deposition (AACVD) is used to deposit highly crystalline CuSCN films at low temperature. AACVD is a commercially viable technique due to its low cost and inherent scalability. In this study, the deposition temperature, CuSCN concentration and carrier gas flow rate were studied and optimized, resulting in homogeneous films grown over areas approaching 30 cm2. At the optimized values, i.e., 60 °C using a 35 mg/mL solution and a carrier gas flow rate of 0.5 dm3/min, the film growth rate is around 100 nm/min. We present a thorough analysis of the film growth parameters and the subsequent morphology, composition, and structural and optical properties of the deposited thin films.
- Published
- 2020
44. Water stable molecular n-doping produces organic electrochemical transistors with high transconductance and record stability
- Author
-
Abdul-Hamid M. Emwas, Maximillian Moser, Iain McCulloch, Xingxing Chen, Thomas D. Anthopoulos, Shofarul Wustoni, Bryan D. Paulsen, Hendrik Faber, Jonathan Rivnay, Sahika Inal, Achilleas Savva, Iuliana P. Maria, Tania C. Hidalgo, Georgios Nikiforidis, Leonidas Tsetseris, Alexandra F. Paterson, Savva, Achilleas [0000-0002-0197-0290], Wustoni, Shofarul [0000-0002-3059-4503], Tsetseris, Leonidas [0000-0002-0330-0813], Paulsen, Bryan D [0000-0002-0923-8475], Hidalgo, Tania C [0000-0001-5299-9539], Rivnay, Jonathan [0000-0002-0602-6485], Anthopoulos, Thomas D [0000-0002-0978-8813], Inal, Sahika [0000-0002-1166-1512], and Apollo - University of Cambridge Repository
- Subjects
Materials science ,Science ,Transconductance ,General Physics and Astronomy ,02 engineering and technology ,Electrolyte ,Conjugated polymers ,010402 general chemistry ,01 natural sciences ,Capacitance ,Article ,4016 Materials Engineering ,General Biochemistry, Genetics and Molecular Biology ,law.invention ,law ,Electronic devices ,lcsh:Science ,40 Engineering ,chemistry.chemical_classification ,3403 Macromolecular and Materials Chemistry ,Bioelectronics ,Multidisciplinary ,34 Chemical Sciences ,Dopant ,business.industry ,Doping ,Transistor ,General Chemistry ,Polymer ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,chemistry ,Optoelectronics ,lcsh:Q ,0210 nano-technology ,business - Abstract
From established to emergent technologies, doping plays a crucial role in all semiconducting devices. Doping could, theoretically, be an excellent technique for improving repressively low transconductances in n-type organic electrochemical transistors – critical for advancing logic circuits for bioelectronic and neuromorphic technologies. However, the technical challenge is extreme: n-doped polymers are unstable in electrochemical transistor operating environments, air and water (electrolyte). Here, the first demonstration of doping in electron transporting organic electrochemical transistors is reported. The ammonium salt tetra-n-butylammonium fluoride is simply admixed with the conjugated polymer poly(N,N’-bis(7-glycol)-naphthalene-1,4,5,8-bis(dicarboximide)-co-2,2’-bithiophene-co-N,N’-bis(2-octyldodecyl)-naphthalene-1,4,5,8-bis(dicarboximide), and found to act as a simultaneous molecular dopant and morphology-additive. The combined effects enhance the n-type transconductance with improved channel capacitance and mobility. Furthermore, operational and shelf-life stability measurements showcase the first example of water-stable n-doping in a polymer. Overall, the results set a precedent for doping/additives to impact organic electrochemical transistors as powerfully as they have in other semiconducting devices., Improving electron transport and stability of n-type organic electrochemical transistors (OECTs) is required to realize a commercially-viable technology for bioelectronics applications. Here, the authors report water-stable doped n-type OECTs with enhanced transconductance and record stability.
- Published
- 2020
45. Colossal tunneling electroresistance in co-planar polymer ferroelectric tunnel junctions
- Author
-
Aniruddha Basu, Hendrik Faber, Thomas D. Anthopoulos, Kalaivanan Loganathan, Akmaral Seitkhan, Dimitra G. Georgiadou, Kamal Asadi, Emre Yengel, Dipti R Naphade, and Manasvi Kumar
- Subjects
chemistry.chemical_classification ,Materials science ,Foundation (engineering) ,Piezoelectric force microscopy ,02 engineering and technology ,Polymer ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Engineering physics ,Ferroelectricity ,0104 chemical sciences ,Electronic, Optical and Magnetic Materials ,Technical support ,Planar ,chemistry ,0210 nano-technology ,Quantum tunnelling - Abstract
Ferroelectric tunnel junctions (FTJs) are ideal resistance-switching devices due to their deterministic behavior and operation at low voltages. However, FTJs have remained mostly as a scientific curiosity due to three critical issues: lack of rectification in their current-voltage characteristic, small tunneling electroresistance (TER) effect, and absence of a straightforward lithography-based device fabrication method that would allow for their mass production. Co-planar FTJs that are fabricated using wafer-scale adhesion lithography technique are demonstrated, and a bi-stable rectifying behavior with colossal TER approaching 106% at room temperature is exhibited. The FTJs are based on poly(vinylidenefluoride-co-trifluoroethylene) [P(VDF-TrFE)], and employ asymmetric co-planar metallic electrodes separated by
- Published
- 2020
46. Core fluorination enhances solubility and ambient stability of an IDT‐based n‐type semiconductor in transistor devices
- Author
-
Thomas D. Anthopoulos, Florian Glöcklhofer, Adam V. Marsh, Aniruddha Basu, Haojie Dai, Karl J. Thorley, Julianna Panidi, Changsheng Wang, Thomas Hodsden, William Mitchell, Martin Heeney, Andrew J. P. White, EPSRC, and The Royal Society
- Subjects
Technology ,Materials science ,EFFICIENCY ,Chemistry, Multidisciplinary ,Materials Science ,Materials Science, Multidisciplinary ,02 engineering and technology ,010402 general chemistry ,INDACENODITHIOPHENE ,01 natural sciences ,09 Engineering ,law.invention ,Physics, Applied ,Biomaterials ,ambient stability ,law ,ORGANIC SOLAR-CELLS ,RECENT PROGRESS ,Electrochemistry ,Nanoscience & Nanotechnology ,OPTIMIZATION ,Materials ,organic field-effect transistors ,Extrinsic semiconductor ,Science & Technology ,02 Physical Sciences ,Chemistry, Physical ,n-type semiconductors ,Physics ,Transistor ,DESIGN STRATEGIES ,021001 nanoscience & nanotechnology ,Condensed Matter Physics ,Engineering physics ,Engineering and Physical Sciences ,fluorination ,TRANSPORT ,0104 chemical sciences ,Electronic, Optical and Magnetic Materials ,Chemistry ,small molecules ,Physics, Condensed Matter ,Research council ,HIGH-PERFORMANCE ,Physical Sciences ,Science & Technology - Other Topics ,0210 nano-technology ,03 Chemical Sciences ,CONJUGATED POLYMERS - Abstract
The synthesis of a novel fluorinated n‐type small molecule based on an indacenodithiophene core is reported. Fluorination is found to have a significant impact on the physical properties, including a surprisingly dramatic improvement in solubility, in addition to effectively stabilizing the lowest‐unoccupied molecular orbital energy (−4.24 eV). Single‐crystal analysis and density functional theory calculations indicate the improved solubility can be attributed to backbone torsion resulting from the positioning of the fluorine group in close proximity to the strongly electron‐withdrawing dicyanomethylene group. Organic thin‐film transistors made via blade coating display high electron mobility (up to 0.49 cm2 V−1 s−1) along with good retention of performance in ambient conditions.
- Published
- 2020
47. The crucial role of fluorine in fully alkylated ladder type carbazole based non-fullerene organic solar cells
- Author
-
Xuechen Jiao, Qiao He, Zhuping Fei, Tingmang Wu, Thomas D. Anthopoulos, Eliot Gann, Munazza Shahid, Christopher R. McNeill, Flurin Eisner, and Martin Heeney
- Subjects
Technology ,Materials science ,EFFICIENCY ,Organic solar cell ,fluorine effect ,fully alkylated side chains ,Band gap ,Materials Science ,Materials Science, Multidisciplinary ,02 engineering and technology ,010402 general chemistry ,01 natural sciences ,Miscibility ,Polymer solar cell ,09 Engineering ,PHOTOVOLTAIC PERFORMANCE ,chemistry.chemical_compound ,carbazole ,Molecule ,General Materials Science ,Nanoscience & Nanotechnology ,ELECTRON-ACCEPTORS ,chemistry.chemical_classification ,Science & Technology ,Carbazole ,Energy conversion efficiency ,UNITS ,organic solar cells ,ATOM ,Electron acceptor ,021001 nanoscience & nanotechnology ,0104 chemical sciences ,nonfullerene acceptors ,chemistry ,Chemical engineering ,Science & Technology - Other Topics ,POLYMERS ,0210 nano-technology ,BACKBONE ,03 Chemical Sciences - Abstract
Two fused ladder type non-fullerene acceptors, DTCCIC and DTCCIC-4F, based on an electron-donating alkylated dithienocyclopentacarbazole core flanked by electron-withdrawing non-fluorinated or fluorinated 1,1-dicyanomethylene-3-indanone (IC or IC-4F), are prepared and utilized in organic solar cells (OSCs). The two new molecules reveal planar structures and strong aggregation behavior, and fluorination is shown to red shift the optical band gap and down shift energy levels. OSCs based on DTCCIC-4F exhibit a power conversion efficiency of 12.6 %, much higher than that of DTCCIC based devices (6.2 %). Microstructural studies reveal that while both acceptors are highly crystalline, bulk heterojunction blends based on the non-fluorinated DTCCIC result in overly coarse domains, while blends based on the fluorinated DTCCIC-4F exhibit a more optimal nanoscale morphology. These results highlight the importance of end group fluorination in controlling molecular aggregation and miscibility.
- Published
- 2020
48. Polymer light‐emitting transistors with charge‐carrier mobilities exceeding 1 cm2 V−1 s−1
- Author
-
Martin Heeney, George Vourlias, Mujeeb Ullah Chaudhry, Donal D. C. Bradley, Thomas D. Anthopoulos, Yuliar Firdaus, Kornelius Tetzner, Julianna Panidi, Sungho Nam, Alice Smith, Jongchul Lim, Panos Patsalas, and Wai-Yu Sit
- Subjects
chemistry.chemical_classification ,Materials science ,business.industry ,Transistor ,02 engineering and technology ,Polymer ,010402 general chemistry ,021001 nanoscience & nanotechnology ,Laser ,01 natural sciences ,7. Clean energy ,0104 chemical sciences ,Electronic, Optical and Magnetic Materials ,law.invention ,Organic semiconductor ,chemistry ,law ,Optoelectronics ,Light emission ,Charge carrier ,Polymer blend ,0210 nano-technology ,Luminescence ,business - Abstract
The vast majority of conjugated polymer-based light emitting field-effect transistors (LEFETs) are characterized by low charge carrier mobilities typically in the range 10-5 to 10-3 cm2 V-1 s-1 range. Fast carrier transport is a highly desirable characteristic for high frequency LEFET operation and, potentially, for use in electrically-pumped lasers. Unfortunately, high mobility organic semiconductors are often characterised by strong intermolecular π-π interactions that reduce luminescence. Development of new materials and/or device concepts that overcome this hurdle are therefore required. We report single organic semiconductor layer, light-emitting transistors that combine the highest hole mobilities reported to date for any polymer-based LEFET, with encouraging light emission characteristics. We achieve this in a single polymer layer LEFET, which was further enhanced through the use of a small-molecule/conjugated polymer blend system that possesses a film microstructure which supports enhanced charge carrier mobility (3.2 cm2 V-1 s-1) and promising light emission characteristics (1600 cd m-2) as compared to polymer-only based LEFETs. This simple approach represents an attractive strategy to further advance the performance of solution-processed LEFETs.
- Published
- 2020
49. Modification of Indacenodithiophene-Based Polymers and Its Impact on Charge Carrier Mobility in Organic Thin-Film Transistors
- Author
-
Helen Bristow, Iain McCulloch, Henning Sirringhaus, Andrew Wadsworth, Thomas D. Anthopoulos, Alberto Salleo, Karl J. Thorley, Maximilian Moser, Hu Chen, Camila Cendra, and Mark Nikolka
- Subjects
chemistry.chemical_classification ,Charge carrier mobility ,Chemistry ,Transistor ,Nanotechnology ,General Chemistry ,Polymer ,010402 general chemistry ,01 natural sciences ,Biochemistry ,Catalysis ,0104 chemical sciences ,law.invention ,Colloid and Surface Chemistry ,law ,Thin-film transistor - Abstract
The polymer indacenodithiophene-co-benzothiadiazole (IDT-BT) has been thoroughly studied for its use in p-type organic thin-film transistors over the course of the past decade. While a variety of m...
- Published
- 2019
50. The effect of ring expansion in thienobenzo[b]indacenodithiophene polymers for organic field-effect transistors
- Author
-
Thomas D. Anthopoulos, Alberto Salleo, Iain McCulloch, Giovanni Costantini, Weimin Zhang, Hu Chen, Bryon W. Larson, Karl J. Thorley, Henning Sirringhaus, Chun Ma, Andrew Wadsworth, Camila Cendra, Mark Nikolka, Alexander M. T. Luci, Alice Nanni, Garry Rumbles, and Luís M. A. Perdigão
- Subjects
chemistry.chemical_classification ,Electron mobility ,Chemistry ,business.industry ,QH ,Transistor ,General Chemistry ,Polymer ,010402 general chemistry ,Ring (chemistry) ,01 natural sciences ,Biochemistry ,Catalysis ,Planarity testing ,0104 chemical sciences ,law.invention ,Colloid and Surface Chemistry ,law ,Optoelectronics ,Field-effect transistor ,QD ,Scanning tunneling microscope ,business ,Saturation (magnetic) - Abstract
A fused donor, thienobenzo[b]indacenodithiophene (TBIDT), was designed and synthesized using a novel acid-promoted cas-cade ring closure strategy, and copolymerized with a benzothiadiazole (BT) monomer. The backbone of TBIDT is an expan-sion of the well-known indacenodithiophene (IDT) unit and was expected to enhance the charge carrier mobility, by improving backbone planarity and facilitating short-contacts between polymer chains. However, the optimized field-effect transistors demonstrated an average saturation hole mobility of 0.9 cm2 V−1s−1, lower than the performance of IDT-BT (~1.5 cm2 V−1s−1). Mobilities extracted from time-resolved microwave conductivity (TRMC) measurements were consistent with the trend in hole mobilities in OFET devices. Scanning Tunneling Microscopy (STM) measurements and computational modelling illustrated that TBIDT-BT exhibits a less ordered microstructure in comparison to IDT-BT. This reveals that a regular side chain pack-ing density, independent of conformational isomers, is critical to avoid local free volume due to irregular packing, which can host trapping impurities. DFT calculations indicated that TBIDT-BT, despite containing a larger, planar unit, showed less stabilization of planar backbone geometries, in comparison to IDT-BT. This is due to the reduced electrostatic stabilizing inter-actions between the peripheral thiophene of the fused core with the BT unit, resulting in a reduction of the barrier to rotation around the single bond. These insights provide a greater understanding of the general structure-property relationships required for semiconducting polymer repeat units to ensure optimal backbone planarization, as illustrated with IDT-type units, guiding the design of novel semiconducting polymers with extended fused backbones for high-performance field-effect transistors.
- Published
- 2019
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