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Enrico, A., Buchmann, S., De Ferrari, F., Lin, Y., Wang, Y., Yue, W., . . . Zeglio, E. (2024). Cleanroom‐Free Direct Laser Micropatterning of Polymers for Organic Electrochemical Transistors in Logic Circuits and Glucose Biosensors. Advanced Science
Open this publication in new window or tab >>Cleanroom‐Free Direct Laser Micropatterning of Polymers for Organic Electrochemical Transistors in Logic Circuits and Glucose Biosensors
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2024 (English)In: Advanced Science, E-ISSN 2198-3844Article in journal (Refereed) Published
Abstract [en]

Organic electrochemical transistors (OECTs) are promising devices for bioelectronics, such as biosensors. However, current cleanroom-based microfabrication of OECTs hinders fast prototyping and widespread adoption of this technology for low-volume, low-cost applications. To address this limitation, a versatile and scalable approach for ultrafast laser microfabrication of OECTs is herein reported, where a femtosecond laser to pattern insulating polymers (such as parylene C or polyimide) is first used, exposing the underlying metal electrodes serving as transistor terminals (source, drain, or gate). After the first patterning step, conducting polymers, such as poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), or semiconducting polymers, are spin-coated on the device surface. Another femtosecond laser patterning step subsequently defines the active polymer area contributing to the OECT performance by disconnecting the channel and gate from the surrounding spin-coated film. The effective OECT width can be defined with high resolution (down to 2 µm) in less than a second of exposure. Micropatterning the OECT channel area significantly improved the transistor switching performance in the case of PEDOT:PSS-based transistors, speeding up the devices by two orders of magnitude. The utility of this OECT manufacturing approach is demonstrated by fabricating complementary logic (inverters) and glucose biosensors, thereby showing its potential to accelerate OECT research.

Place, publisher, year, edition, pages
Wiley, 2024
Keywords
conjugated polymer, direct writing, organic electrochemical transistor, poly(3, 4-ethylenedioxythiophene) polystyrene sulfonate, ultrashort pulsed lasers
National Category
Organic Chemistry Other Electrical Engineering, Electronic Engineering, Information Engineering Other Materials Engineering
Identifiers
urn:nbn:se:kth:diva-342521 (URN)10.1002/advs.202307042 (DOI)001142422700001 ()2-s2.0-85182492139 (Scopus ID)
Funder
Swedish Research Council, 2018‐03483Swedish Research Council, 2022‐04060Swedish Research Council, 2022‐02855Knut and Alice Wallenberg Foundation, 2015.0178Knut and Alice Wallenberg Foundation, 2020.0206Knut and Alice Wallenberg Foundation, 2021.0312Swedish Research Council, 2022-00374
Note

QC 20240123

Available from: 2024-01-23 Created: 2024-01-23 Last updated: 2024-02-06Bibliographically approved
Zeglio, E., Wang, Y., Jain, S., Lin, Y., Avila Ramirez, A. E., Feng, K., . . . Herland, A. (2024). Mixing Insulating Commodity Polymers with Semiconducting n‐type Polymers Enables High‐Performance Electrochemical Transistors. Advanced Materials, Article ID adma.202302624.
Open this publication in new window or tab >>Mixing Insulating Commodity Polymers with Semiconducting n‐type Polymers Enables High‐Performance Electrochemical Transistors
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2024 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, article id adma.202302624Article in journal (Refereed) Published
Abstract [en]

Diluting organic semiconductors with a host insulating polymer is used to increase the electronic mobility in organic electronic devices, such as thin film transistors, while considerably reducing material costs. In contrast to organic electronics, bioelectronic devices such as the organic electrochemical transistor (OECT) rely on both electronic and ionic mobility for efficient operation, making it challenging to integrate hydrophobic polymers as the predominant blend component. This work shows that diluting the n-type conjugated polymer p(N-T) with high molecular weight polystyrene (10 KDa) leads to OECTs with over three times better mobility-volumetric capacitance product (µC*) with respect to the pristine p(N-T) (from 4.3 to 13.4 F V−1 cm−1 s−1) while drastically decreasing the amount of conjugated polymer (six times less). This improvement in µC* is due to a dramatic increase in electronic mobility by two orders of magnitude, from 0.059 to 1.3 cm2 V−1 s−1 for p(N-T):Polystyrene 10 KDa 1:6. Moreover, devices made with this polymer blend show better stability, retaining 77% of the initial drain current after 60 minutes operation in contrast to 12% for pristine p(N-T). These results open a new generation of low-cost organic mixed ionic-electronic conductors where the bulk of the film is made by a commodity polymer.

Place, publisher, year, edition, pages
Wiley, 2024
National Category
Polymer Technologies Materials Engineering Nano Technology Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-345903 (URN)10.1002/adma.202302624 (DOI)2-s2.0-85187136336 (Scopus ID)
Funder
Knut and Alice Wallenberg Foundation, KAW2015.0178 2020.0206Knut and Alice Wallenberg Foundation, 2021.0312Swedish Research Council, 2018–03483Swedish Research Council, 2022‐04060Swedish Research Council, 2022‐02855Karolinska Institute, 1‐249/2019KTH Royal Institute of Technology, VF‐2019‐0110
Note

QC 20240429

Available from: 2024-04-25 Created: 2024-04-25 Last updated: 2024-04-29Bibliographically approved
Toldrà Filella, A., Chondrogiannis, G. & Hamedi, M. (2023). A 3D paper microfluidic device for enzyme-linked assays: Application to DNA analysis. Biotechnology Journal, 18(9), Article ID 2300143.
Open this publication in new window or tab >>A 3D paper microfluidic device for enzyme-linked assays: Application to DNA analysis
2023 (English)In: Biotechnology Journal, ISSN 1860-6768, E-ISSN 1860-7314, Vol. 18, no 9, article id 2300143Article in journal (Refereed) Published
Abstract [en]

A paper microfluidic device capable of conducting enzyme-linked assays is presented: a microfluidic enzyme-linked paper analytical device (μEL-PAD). The system exploits a wash-free sandwich coupling to form beads/analyte/enzyme complexes, which are subsequently added to the vertical flow device composed of wax-printed paper, waxed nitrocellulose membrane and absorbent/barrier layers. The nitrocellulose retains the bead complexes without disrupting the flow, enabling for an efficient washing step. The entrapped complexes then interact with the chromogenic substrate stored on the detection paper, generating a color change on it, quantified with an open-source smartphone software. This is a universal paper-based technology suitable for high-sensitivity quantification of many analytes, such as proteins or nucleic acids, with different enzyme-linked formats. Here, the potential of the μEL-PAD is demonstrated to detect DNA from Staphylococcus epidermidis. After generation of isothermally amplified genomic DNA from bacteria, Biotin/FITC-labeled products were analyzed with the μEL-PAD, exploiting streptavidin-coated beads and antiFITC-horseradish peroxidase. The μEL-PAD achieved a limit of detection (LOD) and quantification <10 genome copies/μL, these being at least 70- and 1000-fold lower, respectively, than a traditional lateral flow assay (LFA) exploiting immobilized streptavidin and antiFITC-gold nanoparticles. It is envisaged that the device will be a good option for low-cost, simple, quantitative, and sensitive paper-based point-of-care testing.

Place, publisher, year, edition, pages
Wiley, 2023
Keywords
high-sensitivity paper analytical device, lateral flow test, point-of-care diagnostics, quantitative multi-step assay, smartphone colorimetric readout, vertical flow μPAD
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-338571 (URN)10.1002/biot.202300143 (DOI)000999468200001 ()37222181 (PubMedID)2-s2.0-85161407012 (Scopus ID)
Note

QC 20231107

Available from: 2023-11-07 Created: 2023-11-07 Last updated: 2023-11-07Bibliographically approved
Wang, Z., Heasman, P., Rostami, J., Benselfelt, T., Linares, M., Li, H., . . . Wågberg, L. (2023). Dynamic Networks of Cellulose Nanofibrils Enable Highly Conductive and Strong Polymer Gel Electrolytes for Lithium-Ion Batteries. Advanced Functional Materials, 33(30), Article ID 2212806.
Open this publication in new window or tab >>Dynamic Networks of Cellulose Nanofibrils Enable Highly Conductive and Strong Polymer Gel Electrolytes for Lithium-Ion Batteries
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2023 (English)In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 33, no 30, article id 2212806Article in journal (Refereed) Published
Abstract [en]

Tunable dynamic networks of cellulose nanofibrils (CNFs) are utilized to prepare high-performance polymer gel electrolytes. By swelling an anisotropically dewatered, but never dried, CNF gel in acidic salt solutions, a highly sparse network is constructed with a fraction of CNFs as low as 0.9%, taking advantage of the very high aspect ratio and the ultra-thin thickness of the CNFs (micrometers long and 2–4 nm thick). These CNF networks expose high interfacial areas and can accommodate massive amounts of the ionic conductive liquid polyethylene glycol-based electrolyte into strong homogeneous gel electrolytes. In addition to the reinforced mechanical properties, the presence of the CNFs simultaneously enhances the ionic conductivity due to their excellent strong water-binding capacity according to computational simulations. This strategy renders the electrolyte a room-temperature ionic conductivity of 0.61 ± 0.12 mS cm−1 which is one of the highest among polymer gel electrolytes. The electrolyte shows superior performances as a separator for lithium iron phosphate half-cells in high specific capacity (161 mAh g−1 at 0.1C), excellent rate capability (5C), and cycling stability (94% capacity retention after 300 cycles at 1C) at 60 °C, as well as stable room temperature cycling performance and considerably improved safety compared with commercial liquid electrolyte systems.

Place, publisher, year, edition, pages
Wiley, 2023
Keywords
cellulose nanofibrils, composites, energy storages, lithium-ion batteries, polymer electrolytes
National Category
Materials Chemistry Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-338472 (URN)10.1002/adfm.202212806 (DOI)000973324900001 ()2-s2.0-85152801974 (Scopus ID)
Note

QC 20231115

Available from: 2023-11-15 Created: 2023-11-15 Last updated: 2023-11-15Bibliographically approved
Chondrogiannis, G., Reu, P. & Hamedi, M. (2023). Paper-Based Bacterial Lysis Enables Sample-to-Answer Home-based DNA Testing. Advanced Materials Technologies, 8(4), 2201004, Article ID 2201004.
Open this publication in new window or tab >>Paper-Based Bacterial Lysis Enables Sample-to-Answer Home-based DNA Testing
2023 (English)In: Advanced Materials Technologies, E-ISSN 2365-709X, Vol. 8, no 4, p. 2201004-, article id 2201004Article in journal (Refereed) Published
Abstract [en]

Nucleic acid amplification testing (NAAT) is the gold standard for infectious disease diagnostics. Currently NAATs are mainly limited to centralized laboratories, while paper-based antigen tests are used for rapid home-based diagnostics. DNA extraction, the initial sample preparation step in NAATs, remains a bottleneck that hinders its development toward home-based kits. This step requires the use of compounds detrimental to the enzymes in downstream DNA amplification. Here, this work overcomes this bottleneck by immobilizing the enzyme achromopeptidase (ACP) on nitrocellulose, to both store and enable the separation of the enzymes from the other steps. This work provides proof-of-concept that immobilized ACP is effective at lysis and release of amplifiable DNA from gram-positive Staphylococcus epidermidis and enables the use of the lysate directly for DNA amplification, without the need for heat deactivation of the enzyme. This sample preparation method requires only incubation at 37 °C and mild agitation, which allows to implement it with fully disposable and affordable equipment. Consequently, this work enables to combine the paper-based DNA extraction method with the isothermal recombinase polymerase amplification (RPA) followed by lateral flow detection to demonstrate a sample-to-answer NAAT packaged as an instrument free self-test kit expanding the capabilities of home-testing beyond antigen tests. 

Place, publisher, year, edition, pages
Wiley, 2023
Keywords
nucleic acid tests, paper-based, point-of-care, recombinase polymerase amplification, sample preparation, sample-to-answer, Antigens, Diagnosis, DNA, Extraction, Instrument testing, Paper, DNA extraction, Home-based, Nucleic acid test, Nucleic acids amplification, Point of care, Recombinases, Enzymes
National Category
Biochemistry and Molecular Biology
Identifiers
urn:nbn:se:kth:diva-329002 (URN)10.1002/admt.202201004 (DOI)000888373100001 ()2-s2.0-85142391697 (Scopus ID)
Note

QC 20230614

Available from: 2023-06-14 Created: 2023-06-14 Last updated: 2023-06-14Bibliographically approved
Hanze, M., Khaliliazar, S., Reu, P., Toldrà Filella, A. & Hamedi, M. (2023). Toward Continuous Molecular Testing Using Gold-Coated Threads as Multi-Target Electrochemical Biosensors. Biosensors, 13(9), Article ID 844.
Open this publication in new window or tab >>Toward Continuous Molecular Testing Using Gold-Coated Threads as Multi-Target Electrochemical Biosensors
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2023 (English)In: Biosensors, ISSN 2079-6374, Vol. 13, no 9, article id 844Article in journal (Refereed) Published
Abstract [en]

Analytical systems based on isothermal nucleic acid amplification tests (NAATs) paired with electroanalytical detection enable cost-effective, sensitive, and specific digital pathogen detection for various in situ applications such as point-of-care medical diagnostics, food safety monitoring, and environmental surveillance. Self-assembled monolayers (SAMs) on gold surfaces are reliable platforms for electroanalytical DNA biosensors. However, the lack of automation and scalability often limits traditional chip-based systems. To address these challenges, we propose a continuous thread-based device that enables multiple electrochemical readings on a functionalized working electrode Au thread with a single connection point. We demonstrate the possibility of rolling the thread on a spool, which enables easy manipulation in a roll-to-roll architecture for high-throughput applications. As a proof of concept, we have demonstrated the detection of recombinase polymerase amplification (RPA) isothermally amplified DNA from the two toxic microalgae species Ostreopsis cf. ovata and Ostreopsis cf. siamensis by performing a sandwich hybridization assay (SHA) with electrochemical readout.

Place, publisher, year, edition, pages
MDPI AG, 2023
Keywords
chronoamperometry, isothermal DNA amplification, metal-coated threads, roll-to-roll, sandwich hybridization assay, self-assembled monolayers
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:kth:diva-338402 (URN)10.3390/bios13090844 (DOI)001074469800001 ()37754078 (PubMedID)2-s2.0-85172180625 (Scopus ID)
Note

QC 20231023

Available from: 2023-10-23 Created: 2023-10-23 Last updated: 2023-10-24Bibliographically approved
Subramaniyam, C. M., Kang, M., Li, J., Mohammadi, A. V. & Hamedi, M. (2022). Additive-free red phosphorus/Ti3C2TxMXene nanocomposite anodes for metal-ion batteries. Energy Advances (12), 999-1008
Open this publication in new window or tab >>Additive-free red phosphorus/Ti3C2TxMXene nanocomposite anodes for metal-ion batteries
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2022 (English)In: Energy Advances, E-ISSN 2753-1457, no 12, p. 999-1008Article in journal (Refereed) Published
Abstract [en]

Herein, we report on scalable, environmentally benign, and additive-free, high-performance anodes for alkali-metal-ion batteries (MIBs, where M = Li+, Na+, K+). The intercalators in these anodes are the red phosphorus (RP) nanoparticles of uniform size (~40 nm), which are dispersible and blend with water-dispersed Ti3C2Tx MXene, forming a highly viscous aqueous slurry to fabricate additive-free nanocomposite electrodes. We further enhanced their performance using a very low weight percentage of various carbonaceous nanomaterials. Our RP-MWCNT/MXene nanocomposite anodes exhibited enhanced ion transport and low charge transfer resistance, delivering specific capacities of 1293.7 mA h g-1 at 500 mA g-1 and 263.3 mA h g-1 at 2600 mA g-1 for 10 000 cycles in Li+ cells, 371.6 mA h g-1 at 500 mA g-1 in Na+ cells, and 732.8 mA h g-1 at 50 mA g-1 in K+ cells. Our work shows a path towards fabricating nanoarchitectured electrodes using sustainable materials to eliminate inert polymer binders, toxic processing solvents, and rare earth elements from the battery fabrication process for next-generation alkali-metal-ion batteries.

Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC), 2022
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-330971 (URN)10.1039/d2ya00168c (DOI)001105927300001 ()2-s2.0-85151304605 (Scopus ID)
Note

QC 20230705

Available from: 2023-07-05 Created: 2023-07-05 Last updated: 2023-12-11Bibliographically approved
Cui, Y., Subramaniyam, C. M., Li, L., Han, T., Kang, M., Li, J., . . . Hamedi, M. (2022). Hierarchical soot nanoparticle self-assemblies for enhanced performance as sodium-ion battery anodes. Journal of Materials Chemistry A, 10(16), 9059-9066
Open this publication in new window or tab >>Hierarchical soot nanoparticle self-assemblies for enhanced performance as sodium-ion battery anodes
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2022 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, E-ISSN 2050-7496, Vol. 10, no 16, p. 9059-9066Article in journal (Refereed) Published
Abstract [en]

The drawbacks of amorphous hard carbon are its low conductivity and structural instability, due to its large volume change and the occurrence of side reactions with the electrolyte during cycling. Here, we propose a simple and rapid method to address these disadvantages; we used an emulsion solvent-evaporation method to create hierarchically structured microparticles of hard carbon nanoparticles, derived from soot, and multi-walled-carbon-nanotubes at a very low threshold of 2.8 wt%. These shrub-ball like microparticles have well-defined void spaces between different nanostructures of carbon, leading to an increased surface area, lower charge-resistance and side reactions, and higher electronic conductivity for Na+ insertion and de-insertion. They can be slurry cast to assemble Na+ anodes, exhibiting an initial discharge capacity of 713.3 mA h g(-1) and showing long-term stability with 120.8 mA h g(-1) at 500 mA g(-1) after 500 cycles, thus outperforming neat hard carbon nanoparticles by an order of magnitude. Our work shows that hierarchical self-assembly is attractive for increasing the performance of microparticles used for battery production.

Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC), 2022
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-311641 (URN)10.1039/d1ta10889a (DOI)000780328500001 ()2-s2.0-85127876353 (Scopus ID)
Note

QC 20220502

Available from: 2022-05-02 Created: 2022-05-02 Last updated: 2022-11-29Bibliographically approved
Melianas, A., Kang, M., VahidMohammadi, A., Quill, T. J., Tian, W., Gogotsi, Y., . . . Hamedi, M. (2022). High-Speed Ionic Synaptic Memory Based on 2D Titanium Carbide MXene. Advanced Functional Materials, 32(12), 2109970, Article ID 2109970.
Open this publication in new window or tab >>High-Speed Ionic Synaptic Memory Based on 2D Titanium Carbide MXene
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2022 (English)In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, Vol. 32, no 12, p. 2109970-, article id 2109970Article in journal (Refereed) Published
Abstract [en]

Synaptic devices with linear high-speed switching can accelerate learning in artificial neural networks (ANNs) embodied in hardware. Conventional resistive memories however suffer from high write noise and asymmetric conductance tuning, preventing parallel programming of ANN arrays. Electrochemical random-access memories (ECRAMs), where resistive switching occurs by ion insertion into a redox-active channel, aim to address these challenges due to their linear switching and low noise. ECRAMs using 2D materials and metal oxides however suffer from slow ion kinetics, whereas organic ECRAMs enable high-speed operation but face challenges toward on-chip integration due to poor temperature stability of polymers. Here, ECRAMs using 2D titanium carbide (Ti3C2Tx) MXene that combine the high speed of organics and the integration compatibility of inorganic materials in a single high-performance device are demonstrated. These ECRAMs combine the speed, linearity, write noise, switching energy, and endurance metrics essential for parallel acceleration of ANNs, and importantly, they are stable after heat treatment needed for back-end-of-line integration with Si electronics. The high speed and performance of these ECRAMs introduces MXenes, a large family of 2D carbides and nitrides with more than 30 stoichiometric compositions synthesized to date, as promising candidates for devices operating at the nexus of electrochemistry and electronics.

Place, publisher, year, edition, pages
Wiley, 2022
Keywords
2D materials, analog resistive memories, electrochemical random-access memories, linear switching, mixed ionic–electronic conductors, molecular self-assembly, MXenes, neuromorphic computing, Functional materials, Neural networks, Self assembly, 2d material, Analog resistive memory, Electrochemical random-access memory, Electrochemicals, Mixed ionic-electronic conductors, Molecular self assembly, Random access memory, Resistive memory, Switching
National Category
Other Physics Topics
Identifiers
urn:nbn:se:kth:diva-313255 (URN)10.1002/adfm.202109970 (DOI)000720741200001 ()2-s2.0-85119507500 (Scopus ID)
Note

QC 20220615

Available from: 2022-06-15 Created: 2022-06-15 Last updated: 2022-12-12Bibliographically approved
Toldrà Filella, A., Ainla, A., Khaliliazar, S., Landin, R., Chondrogiannis, G., Hanze, M., . . . Hamedi, M. (2022). Portable electroanalytical nucleic acid amplification tests using printed circuit boards and open-source electronics. The Analyst, 147(19), 4249-4256
Open this publication in new window or tab >>Portable electroanalytical nucleic acid amplification tests using printed circuit boards and open-source electronics
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2022 (English)In: The Analyst, ISSN 0003-2654, E-ISSN 1364-5528, Vol. 147, no 19, p. 4249-4256Article in journal (Refereed) Published
Abstract [en]

The realization of electrochemical nucleic acid amplification tests (NAATs) at the point of care (POC) is highly desirable, but it remains a challenge given their high cost and lack of true portability/miniaturization. Here we show that mass-produced, industrial standardized, printed circuit boards (PCBs) can be repurposed to act as near-zero cost electrodes for self-assembled monolayer-based DNA biosensing, and further integration with a custom-designed and low-cost portable potentiostat. To show the analytical capability of this system, we developed a NAAT using isothermal recombinase polymerase amplification, bypassing the need of thermal cyclers, followed by an electrochemical readout relying on a sandwich hybridization assay. We used our sensor and device for analytical detection of the toxic microalgae Ostreopsis cf. ovata as a proof of concept. This work shows the potential of PCBs and open-source electronics to be used as powerful POC DNA biosensors at a low-cost. 

Place, publisher, year, edition, pages
Royal Society of Chemistry (RSC), 2022
Keywords
Biosensing Techniques, DNA, Electronics, Nucleic Acid Amplification Techniques, Recombinases, Costs, Nucleic acids, Self assembled monolayers, Timing circuits, Voltage regulators, recombinase, DNA biosensing, Electrochemicals, High costs, Low-costs, Miniaturisation, Nucleic acids amplification, Open-source, Point of care, Potentiostats, genetic procedures, genetics, Printed circuit boards
National Category
Analytical Chemistry
Identifiers
urn:nbn:se:kth:diva-327273 (URN)10.1039/d2an00923d (DOI)000842617500001 ()35993403 (PubMedID)2-s2.0-85138024123 (Scopus ID)
Note

QC 20230523

Available from: 2023-05-23 Created: 2023-05-23 Last updated: 2023-05-23Bibliographically approved
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0001-9088-1064

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