Suchergebnisse

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. ; Funding Agencies|Knut and Alice Wallenberg foundationKnut & Alice Wallenberg Foundation; Swedish Research CouncilSwedish Research CouncilEuropean Commission [2016-03979, 2020-03243]; AForsk [18-313, 19-310]; Olle Engkvists Stiftelse [204-0256]; VINNOVAVinnova [2020-05223]; European Commission through the Marie Sklodowska-Curie project HORATES [GA-955837]; FET-OPEN project MITICS [GA-964677]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [SFO-Mat-LiU 2009-00971]; National Research Foundation of KoreaNational Research Foundation of Korea [NRF-2019R1A2C2085290, 2019R1A6A1A11044070]; National Science FoundationNational Science Foundation (NSF) [DMR-2003518]

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 (>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. ; Funding Agencies|Swedish Research CouncilSwedish Research CouncilEuropean Commission [2020-03243]; Olle Engkvists Stiftelse [204-0256]; European CommissionEuropean CommissionEuropean Commission Joint Research Centre [GA-955837, GA-799477]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [SFO-Mat-LiU 2009-00971]; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germanys Excellence Strategy via the Excellence Cluster 3D Matter Made to OrderGerman Research Foundation (DFG) [EXC-2082/1-390761711]; Carl Zeiss Foundation; Deutsche ForschungsgemeinschaftGerman Research Foundation (DFG) [FA 1502/1-1]; National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [52173156]; Swedish Foundation for Strategic ResearchSwedish Foundation for Strategic Research [ITM17-0316]

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 (>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. ; Research funding the Swedish Research Council. Grant Number: 2020-03243 Olle Engkvists Stiftelse. Grant Number: 204-0256 European Commission. Grant Numbers: GA-955837, GA-799477 Swedish Government Strategic Research. Grant Number: 2009-00971 Deutsche Forschungsgemeinschaft. Grant Numbers: EXC-2082/1-390761711, FA 1502/1-1 National Natural Science Foundation of China. Grant Number: 52173156 the Swedish Foundation for Strategic Research

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. ; Funding Agencies|Knut and Alice Wallenberg foundationKnut & Alice Wallenberg Foundation; Swedish Research CouncilSwedish Research CouncilEuropean Commission [2016-03979, 2020-03243]; AForsk [18-313, 19-310]; Olle Engkvists Stiftelse [204-0256]; VINNOVAVinnova [2020-05223]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [SFO-Mat-LiU 2009-00971]; National Research Foundation of KoreaNational Research Foundation of Korea [NRF2020M3H4A3081814, 2019R1A6A1A11044070]; National Science FoundationNational Science Foundation (NSF) [DMR-2003518]