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  • 1.
    Berggren, Elin
    et al.
    Uppsala Univ, Sweden.
    Weng, Yi-Chen
    Uppsala Univ, Sweden.
    Li, Qifan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Johansson, Fredrik O. L.
    KTH Royal Inst Technol, Sweden; Sorbonne Univ, France.
    Cappel, Ute B.
    KTH Royal Inst Technol, Sweden.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Lindblad, Andreas
    Uppsala Univ, Sweden.
    Charge Transfer in the P(g<sub>4</sub>2T-T):BBL Organic Polymer Heterojunction Measured with Core-Hole Clock Spectroscopy2023In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 127, no 49, p. 23733-23742Article in journal (Refereed)
    Abstract [en]

    The conductivity of organic polymer heterojunction devices relies on the electron dynamics occurring along interfaces between the acceptor and donor moieties. To investigate these dynamics with chemical specificity, spectroscopic techniques are employed to obtain localized snapshots of the electron behavior at selected interfaces. In this study, charge transfer in blends (by weight 10, 50, 90, and 100%) of p-type polymer P(g(4)2T-T) (bithiophene-thiophene) and n-type polymer BBL (poly(benzimidazo-benzo-phenanthroline)) was measured by resonant Auger spectroscopy. Electron spectra emanating from the decay of core-excited states created upon X-ray absorption in the donor polymer P(g(4)2T-T) were measured in the sulfur KL2,3L2,3 Auger kinetic energy region as a function of the excitation energy. By tuning the photon energy across the sulfur K-absorption edge, it is possible to differentiate between decay paths in which the core-excited electron remained on the atom with the core-hole and those where it tunneled away. Analyzing the competing decay modes of these localized and delocalized (charge-transfer) processes facilitated the computation of charge-transfer times as a function of excitation energy using the core-hole clock method. The electron delocalization times derived from the measurements were found to be in the as/fs regime for all polymer blends, with the fastest charge transfer occurring in the sample with an equal amount of donor and acceptor polymer. These findings highlight the significance of core-hole clock spectroscopy as a chemically specific tool for examining the local charge tunneling propensity, which is fundamental to understanding macroscopic conductivity. Additionally, the X-ray absorption spectra near the sulfur K-edge in the P(g(4)2T-T) polymer for different polymer blends were analyzed to compare molecular structure, orientation, and ordering in the polymer heterojunctions. The 50% donor sample exhibited the most pronounced angular dependence of absorption, indicating a higher level of ordering compared to the other weight blends. Our studies on the electron dynamics of this type of all-polymer donor-acceptor systems, in which spontaneous ground-state electron transfer occurs, provide us with critical insights to further advance the next generation of organic conductors with mixed electron-hole conduction characteristics suitable for highly stable electrodes of relevance for electronic, electrochemical, and optoelectronic applications.

  • 2.
    Chen, Yongzhen
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Wu, Hanyan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kolhe, Nagesh B.
    Univ Washington, WA 98195 USA; Univ Washington, WA 98195 USA.
    Jenekhe, Samson A.
    Univ Washington, WA 98195 USA; Univ Washington, WA 98195 USA.
    Liu, Xianjie
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Braun, Slawomir
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fahlman, Mats
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    In Situ Spectroscopic and Electrical Investigations of Ladder-type Conjugated Polymers Doped with Alkali Metals2022In: Macromolecules, ISSN 0024-9297, E-ISSN 1520-5835, Vol. 55, no 16, p. 7294-7302Article in journal (Refereed)
    Abstract [en]

    Ladder-type conjugated polymers exhibit a remarkable performance in (opto)electronic devices. Their double-stranded planar structure promotes an extended pi-conjugation compared to inter-ring-twisted analogues, providing an excellent basis for exploring the effects of charge localization on polaron formation. Here, we investigated alkali-metal n -doping of the ladder-type conjugated polymer (polybenzimidazobenzophe-nanthroline) (BBL) through detailed in situ spectroscopic and electrical characterizations. Photoelectron spectroscopy and ultraviolet-visible-near-infrared (UV-vis-NIR) spectroscopy indicate polaron formation upon potassium (K) doping, which agrees well with theoretical predictions. The semiladder BBB displays a similar evolution in the valence band with the appearance of two new features below the Fermi level upon K-doping. Compared to BBL, distinct differences appear in the UV-vis-NIR spectra due to more localized polaronic states in BBB. The high conductivity (2 S cm(-1)) and low activation energy (44 meV) measured for K-doped BBL suggest disorder-free polaron transport. An even higher conductivity (37 S cm(-1)) is obtained by changing the dopant from K to lithium (Li). We attribute the enhanced conductivity to a decreased perturbation of the polymer nanostructure induced by the smaller Li ions. These results highlight the importance of polymer chain planarity and dopant size for the polaronic state in conjugated polymers.

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  • 3.
    Darabi, Sozan
    et al.
    Chalmers Univ Technol, Sweden; Chalmers Univ Technol, Sweden.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. n Ink AB, Sweden.
    Li, Zerui
    Chalmers Univ Technol, Sweden; Sichuan Univ, Peoples R China.
    Huang, Jun-Da
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Hummel, Michael
    Aalto Univ, Finland.
    Sixta, Herbert
    Aalto Univ, Finland.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. n Ink AB, Sweden.
    Mueller, Christian
    Chalmers Univ Technol, Sweden; Chalmers Univ Technol, Sweden.
    Polymer-Based n-Type Yarn for Organic Thermoelectric Textiles2023In: Advanced Electronic Materials, E-ISSN 2199-160X, Vol. 9, no 4, article id 2201235Article in journal (Refereed)
    Abstract [en]

    A conjugated-polymer-based n-type yarn for thermoelectric textiles is presented. Thermoelectric textile devices are intriguing power sources for wearable electronic devices. The use of yarns comprising conjugated polymers is desirable because of their potentially superior mechanical properties compared to other thermoelectric materials. While several examples of p-type conducting yarns exist, there is a lack of polymer-based n-type yarns. Here, a regenerated cellulose yarn is spray-coated with an n-type conducting-polymer-based ink composed of poly(benzimidazobenzophenanthroline) (BBL) and poly(ethyleneimine) (PEI). The n-type yarns display a bulk electrical conductivity of 8 x 10(-3) S cm(-1) and Seebeck coefficient of -79 mu V K-1. A promising level of air-stability for at least 13 days can be achieved by applying an additional thermoplastic elastomer coating. A prototype in-plane thermoelectric textile, produced with the developed n-type yarns and p-type yarns, composed of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)-coated regenerated cellulose, displays a stable device performance in air for at least 4 days with an open-circuit voltage per temperature difference of 1 mV degrees C-1. Evidently, polymer-based n-type yarns are a viable component for the construction of thermoelectric textile devices.

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  • 4.
    Gerasimov, Jennifer
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tu, Deyu
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Hitaishi, Vivek
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Padinhare, Harikesh
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Abrahamsson, Tobias
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Karami Rad, Meysam
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Donahue, Mary
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Silverå Ejneby, Malin
    Linköping University, Department of Biomedical Engineering, Division of Biomedical Engineering. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Forchheimer, Robert
    Linköping University, Department of Electrical Engineering, Information Coding. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    A Biologically Interfaced Evolvable Organic Pattern Classifier2023In: Advanced Science, E-ISSN 2198-3844, Vol. 10, no 14, article id 2207023Article in journal (Refereed)
    Abstract [en]

    Future brain-computer interfaces will require local and highly individualized signal processing of fully integrated electronic circuits within the nervous system and other living tissue. New devices will need to be developed that can receive data from a sensor array, process these data into meaningful information, and translate that information into a format that can be interpreted by living systems. Here, the first example of interfacing a hardware-based pattern classifier with a biological nerve is reported. The classifier implements the Widrow-Hoff learning algorithm on an array of evolvable organic electrochemical transistors (EOECTs). The EOECTs channel conductance is modulated in situ by electropolymerizing the semiconductor material within the channel, allowing for low voltage operation, high reproducibility, and an improvement in state retention by two orders of magnitude over state-of-the-art OECT devices. The organic classifier is interfaced with a biological nerve using an organic electrochemical spiking neuron to translate the classifiers output to a simulated action potential. The latter is then used to stimulate muscle contraction selectively based on the input pattern, thus paving the way for the development of adaptive neural interfaces for closed-loop therapeutic systems.

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  • 5.
    Guo, Han
    et al.
    Southern Univ Sci & Technol SUSTech, Peoples R China.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zhang, Xianhe
    Southern Univ Sci & Technol SUSTech, Peoples R China.
    Motta, Alessandro
    Univ Roma La Sapienza, Italy; UdR Roma, Italy.
    Feng, Kui
    Southern Univ Sci & Technol SUSTech, Peoples R China.
    Xia, Yu
    Flexterra Corp, IL 60077 USA.
    Shi, Yongqiang
    Southern Univ Sci & Technol SUSTech, Peoples R China.
    Wu, Ziang
    Department of Chemistry, Korea University, Seoul, South Korea.
    Yang, Kun
    Southern Univ Sci & Technol SUSTech, Peoples R China.
    Chen, Jianhua
    Southern Univ Sci & Technol SUSTech, Peoples R China.
    Liao, Qiaogan
    Southern Univ Sci & Technol SUSTech, Peoples R China.
    Tang, Yumin
    Southern Univ Sci & Technol SUSTech, Peoples R China.
    Sun, Huiliang
    Southern Univ Sci & Technol SUSTech, Peoples R China.
    Woo, Han Young
    Korea Univ, South Korea.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Facchetti, Antonio
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Flexterra Corp, IL 60077 USA; Northwestern Univ, IL 60208 USA; Northwestern Univ, IL 60208 USA.
    Guo, Xugang
    Southern Univ Sci & Technol SUSTech, Peoples R China.
    Transition metal-catalysed molecular n-doping of organic semiconductors2021In: Nature, ISSN 0028-0836, E-ISSN 1476-4687, Vol. 599, no 7883, p. 67-73Article in journal (Refereed)
    Abstract [en]

    Electron doping of organic semiconductors is typically inefficient, but here a precursor molecular dopant is used to deliver higher n-doping efficiency in a much shorter doping time. Chemical doping is a key process for investigating charge transport in organic semiconductors and improving certain (opto)electronic devices(1-9). N(electron)-doping is fundamentally more challenging than p(hole)-doping and typically achieves a very low doping efficiency (eta) of less than 10%(1,10). An efficient molecular n-dopant should simultaneously exhibit a high reducing power and air stability for broad applicability(1,5,6,9,11), which is very challenging. Here we show a general concept of catalysed n-doping of organic semiconductors using air-stable precursor-type molecular dopants. Incorporation of a transition metal (for example, Pt, Au, Pd) as vapour-deposited nanoparticles or solution-processable organometallic complexes (for example, Pd-2(dba)(3)) catalyses the reaction, as assessed by experimental and theoretical evidence, enabling greatly increased eta in a much shorter doping time and high electrical conductivities (above 100 S cm(-1); ref. (12)). This methodology has technological implications for realizing improved semiconductor devices and offers a broad exploration space of ternary systems comprising catalysts, molecular dopants and semiconductors, thus opening new opportunities in n-doping research and applications(12, 13).

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  • 6.
    Li, Qifan
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Huang, Jun-Da
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Liu, Tiefeng
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    van der Pol, Tom
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zhang, Qilun
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Wallenberg Wood Science Center.
    Jeong, Sang Young
    Korea Univ, South Korea.
    Stoeckel, Marc-Antoine
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, SE-60221 Norrkoping, Sweden.
    Wu, Hanyan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zhang, Silan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Liu, Xianjie
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Woo, Han Young
    Korea Univ, South Korea.
    Fahlman, Mats
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, SE-60221 Norrkoping, Sweden.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, SE-60221 Norrkoping, Sweden.
    A Highly Conductive n-Type Conjugated Polymer Synthesized in Water2024In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126Article in journal (Refereed)
    Abstract [en]

    Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is a benchmark hole-transporting (p-type) polymer that finds applications in diverse electronic devices. Most of its success is due to its facile synthesis in water, exceptional processability from aqueous solutions, and outstanding electrical performance in ambient. Applications in fields like (opto-)electronics, bioelectronics, and energy harvesting/storage devices often necessitate the complementary use of both p-type and n-type (electron-transporting) materials. However, the availability of n-type materials amenable to water-based polymerization and processing remains limited. Herein, we present a novel synthesis method enabling direct polymerization in water, yielding a highly conductive, water-processable n-type conjugated polymer, namely, poly[(2,2 '-(2,5-dihydroxy-1,4-phenylene)diacetic acid)-stat-3,7-dihydrobenzo[1,2-b:4,5-b ']difuran-2,6-dione] (PDADF), with remarkable electrical conductivity as high as 66 S cm(-1), ranking among the highest for n-type polymers processed using green solvents. The new n-type polymer PDADF also exhibits outstanding stability, maintaining 90% of its initial conductivity after 146 days of storage in air. Our synthetic approach, along with the novel polymer it yields, promises significant advancements for the sustainable development of organic electronic materials and devices.

  • 7.
    Liu, Tiefeng
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Heimonen, Johanna
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zhang, Qilun
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Norrkoping, Sweden.
    Huang, Jun-Da
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Norrkoping, Sweden.
    Wu, Hanyan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Stoeckel, Marc-Antoine
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Norrkoping, Sweden.
    van der Pol, Tom
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Li, Yuxuan
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Jeong, Sang Young
    Korea Univ, South Korea.
    Marks, Adam
    Univ Oxford, England.
    Wang, Xin-Yi
    Peking Univ, Peoples R China.
    Puttisong, Yuttapoom
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Shimolo, Asaminew Yerango
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Liu, Xianjie
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zhang, Silan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Li, Qifan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Massetti, Matteo
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Chen, Weimin
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Woo, Han Young
    Korea Univ, South Korea.
    Pei, Jian
    Peking Univ, Peoples R China.
    McCulloch, Iain
    Univ Oxford, England.
    Gao, Feng
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Fahlman, Mats
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kroon, Renee
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Norrkoping, Sweden.
    Ground-state electron transfer in all-polymer donor:acceptor blends enables aqueous processing of water-insoluble conjugated polymers2023In: Nature Communications, E-ISSN 2041-1723, Vol. 14, no 1, article id 8454Article in journal (Refereed)
    Abstract [en]

    Water-based conductive inks are vital for the sustainable manufacturing and widespread adoption of organic electronic devices. Traditional methods to produce waterborne conductive polymers involve modifying their backbone with hydrophilic side chains or using surfactants to form and stabilize aqueous nanoparticle dispersions. However, these chemical approaches are not always feasible and can lead to poor material/device performance. Here, we demonstrate that ground-state electron transfer (GSET) between donor and acceptor polymers allows the processing of water-insoluble polymers from water. This approach enables macromolecular charge-transfer salts with 10,000x higher electrical conductivities than pristine polymers, low work function, and excellent thermal/solvent stability. These waterborne conductive films have technological implications for realizing high-performance organic solar cells, with efficiency and stability superior to conventional metal oxide electron transport layers, and organic electrochemical neurons with biorealistic firing frequency. Our findings demonstrate that GSET offers a promising avenue to develop water-based conductive inks for various applications in organic electronics. Chemical approaches to improve aqueous dispersions of conjugated polymers are limited by the feasibility of modifying the backbone or lead to poor performance. Here, Liu et al. show that ground-state electron transfer in donor:acceptor blends aids aqueous dispersion, for high conductivity and solubility.

  • 8.
    Lu, Yang
    et al.
    Tech Univ Dresden, Germany; Tech Univ Dresden, Germany.
    Zhang, Yingying
    Tech Univ Dresden, Germany; Tech Univ Dresden, Germany.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Revuelta, Sergio
    Inst Madrileno Estudios Avanzados Nanociencia IMD, Spain.
    Qi, Haoyuan
    Tech Univ Dresden, Germany; Tech Univ Dresden, Germany; Univ Ulm, Germany.
    Huang, Chuanhui
    Tech Univ Dresden, Germany; Tech Univ Dresden, Germany.
    Jin, Wenlong
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Li, Zichao
    Helmholtz Zentrum Dresden Rossendorf, Germany.
    Vega-Mayoral, Victor
    Inst Madrileno Estudios Avanzados Nanociencia IMD, Spain.
    Liu, Yannan
    Tech Univ Dresden, Germany; Tech Univ Dresden, Germany.
    Huang, Xing
    Tech Univ Dresden, Germany; Tech Univ Dresden, Germany.
    Pohl, Darius
    Tech Univ Dresden, Germany.
    Polozij, Miroslav
    Tech Univ Dresden, Germany; Tech Univ Dresden, Germany.
    Zhou, Shengqiang
    Helmholtz Zentrum Dresden Rossendorf, Germany.
    Canovas, Enrique
    Inst Madrileno Estudios Avanzados Nanociencia IMD, Spain.
    Heine, Thomas
    Tech Univ Dresden, Germany; Tech Univ Dresden, Germany.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Feng, Xinliang
    Tech Univ Dresden, Germany; Tech Univ Dresden, Germany; Max Planck Inst Microstruct Phys, Germany.
    Dong, Renhao
    Tech Univ Dresden, Germany; Tech Univ Dresden, Germany; Shandong Univ, Peoples R China.
    Precise tuning of interlayer electronic coupling in layered conductive metal-organic frameworks2022In: Nature Communications, E-ISSN 2041-1723, Vol. 13, no 1, article id 7240Article in journal (Refereed)
    Abstract [en]

    Layered metal-organic frameworks attract interests for optoelectronics and spintronics. Here, the authors report a strategy to tune interlayer charge transport and thermoelectric properties via side-chain induced control of the layer spacing. Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have attracted increasing interests for (opto)-electronics and spintronics. They generally consist of van der Waals stacked layers and exhibit layer-depended electronic properties. While considerable efforts have been made to regulate the charge transport within a layer, precise control of electronic coupling between layers has not yet been achieved. Herein, we report a strategy to precisely tune interlayer charge transport in 2D c-MOFs via side-chain induced control of the layer spacing. We design hexaiminotriindole ligands allowing programmed functionalization with tailored alkyl chains (HATI_CX, X = 1,3,4; X refers to the carbon numbers of the alkyl chains) for the synthesis of semiconducting Ni-3(HATI_CX)(2). The layer spacing of these MOFs can be precisely varied from 3.40 to 3.70 angstrom, leading to widened band gap, suppressed carrier mobilities, and significant improvement of the Seebeck coefficient. With this demonstration, we further achieve a record-high thermoelectric power factor of 68 +/- 3 nW m(-1) K-2 in Ni-3(HATI_C3)(2), superior to the reported holes-dominated MOFs.

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  • 9.
    Padinhare, Harikesh
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tu, Deyu
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gerasimov, Jennifer
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Manan Dar, Abdul Manan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Armada Moreira, Adam
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Massetti, Matteo
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kroon, Renee
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Bliman, David
    Univ Gothenburg, Sweden.
    Olsson, Roger
    Univ Gothenburg, Sweden; Lund Univ, Sweden.
    Stavrinidou, Eleni
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Tekn Ringen 7, SE-58330 Linkoping, Sweden.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Tekn Ringen 7, SE-58330 Linkoping, Sweden.
    Organic electrochemical neurons and synapses with ion mediated spiking2022In: Nature Communications, E-ISSN 2041-1723, Vol. 13, no 1, article id 901Article in journal (Refereed)
    Abstract [en]

    Future brain-machine interfaces, prosthetics, and intelligent soft robotics will require integrating artificial neuromorphic devices with biological systems. Due to their poor biocompatibility, circuit complexity, low energy efficiency, and operating principles fundamentally different from the ion signal modulation of biology, traditional Silicon-based neuromorphic implementations have limited bio-integration potential. Here, we report the first organic electrochemical neurons (OECNs) with ion-modulated spiking, based on all-printed complementary organic electrochemical transistors. We demonstrate facile bio-integration of OECNs with Venus Flytrap (Dionaea muscipula) to induce lobe closure upon input stimuli. The OECNs can also be integrated with all-printed organic electrochemical synapses (OECSs), exhibiting short-term plasticity with paired-pulse facilitation and long-term plasticity with retention &gt;1000 s, facilitating Hebbian learning. These soft and flexible OECNs operate below 0.6 V and respond to multiple stimuli, defining a new vista for localized artificial neuronal systems possible to integrate with bio-signaling systems of plants, invertebrates, and vertebrates. The integration of artificial neuromorphic devices with biological systems plays a fundamental role for future brain-machine interfaces, prosthetics, and intelligent soft robotics. Harikesh et al. demonstrate all-printed organic electrochemical neurons on Venus flytrap that is controlled to open and close.

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  • 10.
    Padinhare, Harikesh
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Wu, Hanyan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zhang, Silan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Donahue, Mary
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Caravaca, April S.
    Karolinska Inst, Sweden.
    Huang, Jun-Da
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Olofsson, Peder S.
    Karolinska Inst, Sweden.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. n Ink AB, Sweden.
    Tu, Deyu
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. n Ink AB, Sweden.
    Ion-tunable antiambipolarity in mixed ion-electron conducting polymers enables biorealistic organic electrochemical neurons2023In: Nature Materials, ISSN 1476-1122, E-ISSN 1476-4660, Vol. 22, p. 242-248Article in journal (Refereed)
    Abstract [en]

    Biointegrated neuromorphic hardware holds promise for new protocols to record/regulate signalling in biological systems. Making such artificial neural circuits successful requires minimal device/circuit complexity and ion-based operating mechanisms akin to those found in biology. Artificial spiking neurons, based on silicon-based complementary metal-oxide semiconductors or negative differential resistance device circuits, can emulate several neural features but are complicated to fabricate, not biocompatible and lack ion-/chemical-based modulation features. Here we report a biorealistic conductance-based organic electrochemical neuron (c-OECN) using a mixed ion-electron conducting ladder-type polymer with stable ion-tunable antiambipolarity. The latter is used to emulate the activation/inactivation of sodium channels and delayed activation of potassium channels of biological neurons. These c-OECNs can spike at bioplausible frequencies nearing 100 Hz, emulate most critical biological neural features, demonstrate stochastic spiking and enable neurotransmitter-/amino acid-/ion-based spiking modulation, which is then used to stimulate biological nerves in vivo. These combined features are impossible to achieve using previous technologies.

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  • 11.
    Wu, Hanyan
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Huang, Jun-Da
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. n Ink AB, Sweden.
    Jeong, Sang Young
    Korea Univ, South Korea.
    Liu, Tiefeng
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Wu, Ziang
    Korea Univ, South Korea.
    van der Pol, Tom
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Wang, Qingqing
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Stoeckel, Marc-Antoine
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. n Ink AB, Sweden.
    Li, Qifan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fahlman, Mats
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tu, Deyu
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Woo, Han Young
    Korea Univ, South Korea.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. n Ink AB, Sweden.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. n Ink AB, Sweden.
    Stable organic electrochemical neurons based on p-type and n-type ladder polymers2023In: Materials Horizons, ISSN 2051-6347, E-ISSN 2051-6355, no 10, p. 4213-4223Article in journal (Refereed)
    Abstract [en]

    Organic electrochemical transistors (OECTs) are a rapidly advancing technology that plays a crucial role in the development of next-generation bioelectronic devices. Recent advances in p-type/n-type organic mixed ionic-electronic conductors (OMIECs) have enabled power-efficient complementary OECT technologies for various applications, such as chemical/biological sensing, large-scale logic gates, and neuromorphic computing. However, ensuring long-term operational stability remains a significant challenge that hinders their widespread adoption. While p-type OMIECs are generally more stable than n-type OMIECs, they still face limitations, especially during prolonged operations. Here, we demonstrate that simple methylation of the pyrrole-benzothiazine-based (PBBT) ladder polymer backbone results in stable and high-performance p-type OECTs. The methylated PBBT (PBBT-Me) exhibits a 25-fold increase in OECT mobility and an impressive 36-fold increase in & mu;C* (mobility x volumetric capacitance) compared to the non-methylated PBBT-H polymer. Combining the newly developed PBBT-Me with the ladder n-type poly(benzimidazobenzophenanthroline) (BBL), we developed complementary inverters with a record-high DC gain of 194 V V-1 and excellent stability. These state-of-the-art complementary inverters were used to demonstrate leaky integrate-and-fire type organic electrochemical neurons (LIF-OECNs) capable of biologically relevant firing frequencies of about 2 Hz and of operating continuously for up to 6.5 h. This achievement represents a significant improvement over previous results and holds great potential for developing stable bioelectronic circuits capable of in-sensor computing.

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  • 12.
    Wu, Hanyan
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Li, Qifan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kolhe, Nagesh B.
    Univ Washington, WA 98195 USA; Univ Washington, WA 98195 USA.
    Strakosas, Xenofon
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Stoeckel, Marc-Antoine
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Wu, Ziang
    Korea Univ, South Korea.
    Jin, Wenlong
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Savvakis, Marios
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kroon, Renee
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tu, Deyu
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Woo, Han Young
    Korea Univ, South Korea.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Tekn Ringen 7, SE-58330 Linkoping, Sweden.
    Jenekhe, Samson A.
    Univ Washington, WA 98195 USA; Univ Washington, WA 98195 USA.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Tekn Ringen 7, SE-58330 Linkoping, Sweden.
    Influence of Molecular Weight on the Organic Electrochemical Transistor Performance of Ladder-Type Conjugated Polymers2022In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 34, no 4, article id 2106235Article in journal (Refereed)
    Abstract [en]

    Organic electrochemical transistors (OECTs) hold promise for developing a variety of high-performance (bio-)electronic devices/circuits. While OECTs based on p-type semiconductors have achieved tremendous progress in recent years, n-type OECTs still suffer from low performance, hampering the development of power-efficient electronics. Here, it is demonstrated that fine-tuning the molecular weight of the rigid, ladder-type n-type polymer poly(benzimidazobenzophenanthroline) (BBL) by only one order of magnitude (from 4.9 to 51 kDa) enables the development of n-type OECTs with record-high geometry-normalized transconductance (g(m,norm) approximate to 11 S cm(-1)) and electron mobility x volumetric capacitance (mu C* approximate to 26 F cm(-1) V-1 s(-1)), fast temporal response (0.38 ms), and low threshold voltage (0.15 V). This enhancement in OECT performance is ascribed to a more efficient intermolecular charge transport in high-molecular-weight BBL than in the low-molecular-weight counterpart. OECT-based complementary inverters are also demonstrated with record-high voltage gains of up to 100 V V-1 and ultralow power consumption down to 0.32 nW, depending on the supply voltage. These devices are among the best sub-1 V complementary inverters reported to date. These findings demonstrate the importance of molecular weight in optimizing the OECT performance of rigid organic mixed ionic-electronic conductors and open for a new generation of power-efficient organic (bio-)electronic devices.

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  • 13.
    Xing, Yi
    et al.
    Donghua Univ, Peoples R China.
    Zhou, Mingjie
    Fudan Univ, Peoples R China.
    Si, Yueguang
    Fudan Univ, Peoples R China.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Feng, Liang-Wen
    Sichuan Univ, Peoples R China.
    Wu, Qilin
    Donghua Univ, Peoples R China.
    Wang, Fei
    Fudan Univ, Peoples R China.
    Wang, Xiaomin
    Fudan Univ, Peoples R China.
    Huang, Wei
    Univ Elect Sci & Technol China, Peoples R China.
    Cheng, Yuhua
    Univ Elect Sci & Technol China, Peoples R China.
    Zhang, Ruilin
    Chinese Acad Sci, Peoples R China.
    Duan, Xiaozheng
    Chinese Acad Sci, Peoples R China.
    Liu, Jun
    Natl Key Lab Electromagnet Environm Effects & Elet, Peoples R China.
    Song, Ping
    Natl Key Lab Electromagnet Environm Effects & Elet, Peoples R China.
    Sun, Hengda
    Donghua Univ, Peoples R China.
    Wang, Hongzhi
    Donghua Univ, Peoples R China.
    Zhang, Jiayi
    Fudan Univ, Peoples R China.
    Jiang, Su
    Fudan Univ, Peoples R China.
    Zhu, Meifang
    Donghua Univ, Peoples R China.
    Wang, Gang
    Donghua Univ, Peoples R China.
    Integrated opposite charge grafting induced ionic-junction fiber2023In: Nature Communications, E-ISSN 2041-1723, Vol. 14, no 1, article id 2355Article in journal (Refereed)
    Abstract [en]

    The emergence of ionic-junction devices has attracted growing interests due to the potential of serving as signal transmission and translation media between electronic devices and biological systems using ions. Among them, fiber-shaped iontronics possesses a great advantage in implantable applications owing to the unique one-dimensional geometry. However, fabricating stable ionic-junction on curved surfaces remains a challenge. Here, we developed a polyelectrolyte based ionic-junction fiber via an integrated opposite charge grafting method capable of large-scale continuous fabrication. The ionic-junction fibers can be integrated into functions such as ionic diodes and ionic bipolar junction transistors, where rectification and switching of input signals are implemented. Moreover, synaptic functionality has also been demonstrated by utilizing the fiber memory capacitance. The connection between the ionic-junction fiber and sciatic nerves of the mouse simulating end-to-side anastomosis is further performed to realize effective nerve signal conduction, verifying the capability for next-generation artificial neural pathways in implantable bioelectronics. Ionic-junction devices are difficult to integrate with fiber-shaped tissues like nerves and muscles for applications in implantable bioelectronics due to their large size and bulk structure. Authors realize here easy to implant fiber-shaped iontronics through an integrated opposite charge grafting process, enabling the construction of ionic logic gates and artificial neural pathways.

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  • 14.
    Xu, Kai
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Yanshan Univ, Peoples R China.
    Ruoko, Tero-Petri
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Tampere Univ, Finland.
    Shokrani, Morteza
    Heidelberg Univ, Germany.
    Scheunemann, Dorothea
    Heidelberg Univ, Germany.
    Abdalla, Hassan
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Sun, Hengda
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. Donghua Univ, Peoples R China.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Puttisong, Yuttapoom
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Kolhe, Nagesh B.
    Univ Washington, WA 98195 USA; Univ Washington, WA 98195 USA.
    Mendoza Figueroa, Silvestre
    Linköping University, Department of Physics, Chemistry and Biology, Biophysics and bioengineering. Linköping University, Faculty of Science & Engineering.
    Oshaug Pedersen, Jonas
    Linköping University, Department of Physics, Chemistry and Biology, Biophysics and bioengineering. Linköping University, Faculty of Science & Engineering.
    Ederth, Thomas
    Linköping University, Department of Physics, Chemistry and Biology, Biophysics and bioengineering. Linköping University, Faculty of Science & Engineering.
    Chen, Weimin
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Teknikringen 7, SE-58330 Linkoping, Sweden.
    Jenekhe, Samson A.
    Univ Washington, WA 98195 USA; Univ Washington, WA 98195 USA.
    Fazzi, Daniele
    Univ Bologna, Italy; Univ Cologne, Germany.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering. Heidelberg Univ, Germany.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Teknikringen 7, SE-58330 Linkoping, Sweden.
    On the Origin of Seebeck Coefficient Inversion in Highly Doped Conducting Polymers2022In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 32, no 20, article id 2112276Article in journal (Refereed)
    Abstract [en]

    A common way of determining the majority charge carriers of pristine and doped semiconducting polymers is to measure the sign of the Seebeck coefficient. However, a polarity change of the Seebeck coefficient has recently been observed to occur in highly doped polymers. Here, it is shown that the Seebeck coefficient inversion is the result of the density of states filling and opening of a hard Coulomb gap around the Fermi energy at high doping levels. Electrochemical n-doping is used to induce high carrier density (&gt;1 charge/monomer) in the model system poly(benzimidazobenzophenanthroline) (BBL). By combining conductivity and Seebeck coefficient measurements with in situ electron paramagnetic resonance, UV-vis-NIR, Raman spectroelectrochemistry, density functional theory calculations, and kinetic Monte Carlo simulations, the formation of multiply charged species and the opening of a hard Coulomb gap in the density of states, which is responsible for the Seebeck coefficient inversion and drop in electrical conductivity, are uncovered. The findings provide a simple picture that clarifies the roles of energetic disorder and Coulomb interactions in highly doped polymers and have implications for the molecular design of next-generation conjugated polymers.

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  • 15.
    Xu, Kai
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Sun, Hengda
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ruoko, Tero-Petri
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Wang, Gang
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kroon, Renee
    Chalmers Univ Technol, Sweden.
    Kolhe, Nagesh B.
    Univ Washington, WA 98195 USA.
    Puttisong, Yuttapoom
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Liu, Xianjie
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fazzi, Daniele
    Univ Cologne, Germany.
    Shibata, Koki
    Chiba Univ, Japan.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Sun, Ning
    Yunnan Univ, Peoples R China.
    Persson, Gustav
    Chalmers Univ Technol, Sweden.
    Yankovich, Andrew B.
    Chalmers Univ Technol, Sweden.
    Olsson, Eva
    Chalmers Univ Technol, Sweden.
    Yoshida, Hiroyuki
    Chiba Univ, Japan; Chiba Univ, Japan.
    Chen, Weimin
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fahlman, Mats
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kemerink, Martijn
    Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Jenekhe, Samson A.
    Univ Washington, WA 98195 USA.
    Mueller, Christian
    Chalmers Univ Technol, Sweden.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ground-state electron transfer in all-polymer donor-acceptor heterojunctions2020In: Nature Materials, ISSN 1476-1122, E-ISSN 1476-4660, Vol. 19, no 7, p. 738-744Article in journal (Refereed)
    Abstract [en]

    Doping of organic semiconductors is crucial for the operation of organic (opto)electronic and electrochemical devices. Typically, this is achieved by adding heterogeneous dopant molecules to the polymer bulk, often resulting in poor stability and performance due to dopant sublimation or aggregation. In small-molecule donor-acceptor systems, charge transfer can yield high and stable electrical conductivities, an approach not yet explored in all-conjugated polymer systems. Here, we report ground-state electron transfer in all-polymer donor-acceptor heterojunctions. Combining low-ionization-energy polymers with high-electron-affinity counterparts yields conducting interfaces with resistivity values five to six orders of magnitude lower than the separate single-layer polymers. The large decrease in resistivity originates from two parallel quasi-two-dimensional electron and hole distributions reaching a concentration of similar to 10(13) cm(-2). Furthermore, we transfer the concept to three-dimensional bulk heterojunctions, displaying exceptional thermal stability due to the absence of molecular dopants. Our findings hold promise for electro-active composites of potential use in, for example, thermoelectrics and wearable electronics. Doping through spontaneous electron transfer between donor and acceptor polymers is obtained by selecting organic semiconductors with suitable electron affinity and ionization energy, achieving high conductivity in blends and bilayer configuration.

  • 16.
    Yang, Chiyuan
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Stoeckel, Marc-Antoine
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ruoko, Tero-Petri
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Wu, Hanyan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Liu, Xianjie
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kolhe, Nagesh B.
    Univ Washington, WA 98195 USA; Univ Washington, WA 98195 USA.
    Wu, Ziang
    Korea Univ, South Korea.
    Puttisong, Yuttapoom
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Musumeci, Chiara
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Massetti, Matteo
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Sun, Hengda
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Xu, Kai
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tu, Deyu
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Chen, Weimin
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Woo, Han Young
    Korea Univ, South Korea.
    Fahlman, Mats
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Jenekhe, Samson A.
    Univ Washington, WA 98195 USA; Univ Washington, WA 98195 USA.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, S-58330 Linkoping, Sweden.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, S-58330 Linkoping, Sweden.
    A high-conductivity n-type polymeric ink for printed electronics2021In: Nature Communications, E-ISSN 2041-1723, Vol. 12, no 1, article id 2354Article in journal (Refereed)
    Abstract [en]

    Conducting polymers, such as the p-doped poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), have enabled the development of an array of opto- and bio-electronics devices. However, to make these technologies truly pervasive, stable and easily processable, n-doped conducting polymers are also needed. Despite major efforts, no n-type equivalents to the benchmark PEDOT:PSS exist to date. Here, we report on the development of poly(benzimidazobenzophenanthroline):poly(ethyleneimine) (BBL:PEI) as an ethanol-based n-type conductive ink. BBL:PEI thin films yield an n-type electrical conductivity reaching 8Scm(-1), along with excellent thermal, ambient, and solvent stability. This printable n-type mixed ion-electron conductor has several technological implications for realizing high-performance organic electronic devices, as demonstrated for organic thermoelectric generators with record high power output and n-type organic electrochemical transistors with a unique depletion mode of operation. BBL:PEI inks hold promise for the development of next-generation bioelectronics and wearable devices, in particular targeting novel functionality, efficiency, and power performance. The development of n-type conductive polymer inks is critical for the development of next-generation opto-electronic devices that rely on efficient hole and electron transport. Here, the authors report an alcohol-based, high performance and stable n-type conductive ink for printed electronics.

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  • 17.
    Yang, Chiyuan
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tu, Deyu
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ruoko, Tero-Petri
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gerasimov, Jennifer
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Wu, Hanyan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Padinhare, Harikesh
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Massetti, Matteo
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Stoeckel, Marc-Antoine
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Kroon, Renee
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Muller, Christian
    Chalmers Univ Technol, Sweden.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Teknikringen 7, SE-58330 Linkoping, Sweden.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering. N Ink AB, Teknikringen 7, SE-58330 Linkoping, Sweden.
    Low-Power/High-Gain Flexible Complementary Circuits Based on Printed Organic Electrochemical Transistors2022In: Advanced Electronic Materials, E-ISSN 2199-160X, Vol. 8, no 3, article id 2100907Article in journal (Refereed)
    Abstract [en]

    The ability to accurately extract low-amplitude voltage signals is crucial in several fields, ranging from single-use diagnostics and medical technology to robotics and the Internet of Things (IoT). The organic electrochemical transistor (OECT), which features large transconductance values at low operating voltages, is ideal for monitoring small signals. Here, low-power and high-gain flexible circuits based on printed complementary OECTs are reported. This work leverages the low threshold voltage of both p-type and n-type enhancement-mode OECTs to develop complementary voltage amplifiers that can sense voltages as low as 100 mu V, with gains of 30.4 dB and at a power consumption of 0.1-2.7 mu W (single-stage amplifier). At the optimal operating conditions, the voltage gain normalized to power consumption reaches 169 dB mu W-1, which is &gt;50 times larger than state-of-the-art OECT-based amplifiers. In a monolithically integrated two-stage configuration, these complementary voltage amplifiers reach voltage gains of 193 V/V, which are among the highest for emerging complementary metal-oxide-semiconductor-like technologies operating at supply voltages below 1 V. These flexible complementary circuits based on printed OECTs define a new power-efficient platform for sensing and amplifying low-amplitude voltage signals in several emerging beyond-silicon applications.

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  • 18.
    Zhang, Qilun
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Zhang, Huotian
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Wu, Ziang
    Korea Univ, South Korea.
    Wang, Chuanfei
    Ocean Univ China, Peoples R China.
    Zhang, Rui
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Gao, Feng
    Linköping University, Department of Physics, Chemistry and Biology, Electronic and photonic materials. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Woo, Han Young
    Korea Univ, South Korea.
    Ek, Monica
    KTH Royal Inst Technol, Sweden.
    Liu, Xianjie
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fahlman, Mats
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Natural Product Betulin-Based Insulating Polymer Filler in Organic Solar Cells2022In: Solar RRL, E-ISSN 2367-198X, Vol. 6, no 9, article id 2200381Article in journal (Refereed)
    Abstract [en]

    Introduction of filler materials into organic solar cells (OSCs) are a promising strategy to improve device performance and thermal/mechanical stability. However, the complex interactions between the state-of-the-art OSC materials and filler require careful selection of filler materials and OSC fabrication to achieve lower cost and improved performance. In this work, the introduction of a natural product betulin-based insulating polymer as filler in various OSCs is investigated. Donor-acceptor-insulator ternary OSCs are developed with improved open-circuit voltage due to decreased trap-assisted recombination. Furthermore, filler-induced vertical phase separation due to mismatched surface energy can strongly affect charge collection at the bottom interface and limit the filler ratio. A quasi-bilayer strategy is used in all-polymer systems to circumvent this problem. Herein, the variety of filler materials in OSCs to biomass is broadened, and the filler strategy is made a feasible and promising strategy toward highly efficient, eco, and low-cost OSCs.

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  • 19.
    Zhang, Silan
    et al.
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Massetti, Matteo
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Ruoko, Tero-Petri
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Tu, Deyu
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Yang, Chiyuan
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Liu, Xianjie
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Wu, Ziang
    Korea Univ, South Korea.
    Lee, Yoonjoo
    Korea Univ, South Korea.
    Kroon, Renee
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Persson, Per O A
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Woo, Han Young
    Korea Univ, South Korea.
    Berggren, Magnus
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Muller, Christian
    Chalmers Univ Technol, Sweden; Chalmers Univ Technol, Sweden.
    Fahlman, Mats
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Fabiano, Simone
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Synergistic Effect of Multi-Walled Carbon Nanotubes and Ladder-Type Conjugated Polymers on the Performance of N-Type Organic Electrochemical Transistors2022In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 32, no 1, article id 2106447Article in journal (Refereed)
    Abstract [en]

    Organic electrochemical transistors (OECTs) have the potential to revolutionize the field of organic bioelectronics. To date, most of the reported OECTs include p-type (semi-)conducting polymers as the channel material, while n-type OECTs are yet at an early stage of development, with the best performing electron-transporting materials still suffering from low transconductance, low electron mobility, and slow response time. Here, the high electrical conductivity of multi-walled carbon nanotubes (MWCNTs) and the large volumetric capacitance of the ladder-type pi-conjugated redox polymer poly(benzimidazobenzophenanthroline) (BBL) are leveraged to develop n-type OECTs with record-high performance. It is demonstrated that the use of MWCNTs enhances the electron mobility by more than one order of magnitude, yielding fast transistor transient response (down to 15 ms) and high mu C* (electron mobility x volumetric capacitance) of about 1 F cm(-1) V-1 s(-1). This enables the development of complementary inverters with a voltage gain of &gt;16 and a large worst-case noise margin at a supply voltage of &lt;0.6 V, while consuming less than 1 mu W of power.

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