TY - JOUR A1 - Steyrleuthner, Robert A1 - Schubert, Marcel A1 - Jaiser, Frank A1 - Blakesley, James C. A1 - Chen, Zhihua A1 - Facchetti, Antonio A1 - Neher, Dieter T1 - Bulk electron transport and charge injection in a high mobility n-type semiconducting polymer N2 - Bulk electron transport in a high mobility n-type polymer is studied by time-of-flight photocurrent measurements and electron-only devices. Bulk electron mobilities of similar to 5 x 10(-3) cm(2)/Vs are obtained. The analysis of the electron currents suggests the presence of an injection barrier for all conventionally used low workfunction cathodes. Y1 - 2010 UR - http://www3.interscience.wiley.com/cgi-bin/jhome/10008336 U6 - https://doi.org/10.1002/adma.201000232 SN - 0935-9648 ER - TY - JOUR A1 - Lu, Guanghao A1 - Blakesley, James C. A1 - Himmelberger, Scott A1 - Pingel, Patrick A1 - Frisch, Johannes A1 - Lieberwirth, Ingo A1 - Salzmann, Ingo A1 - Oehzelt, Martin A1 - Di Pietro, Riccardo A1 - Salleo, Alberto A1 - Koch, Norbert A1 - Neher, Dieter T1 - Moderate doping leads to high performance of semiconductor/insulator polymer blend transistors JF - Nature Communications N2 - Polymer transistors are being intensively developed for next-generation flexible electronics. Blends comprising a small amount of semiconducting polymer mixed into an insulating polymer matrix have simultaneously shown superior performance and environmental stability in organic field-effect transistors compared with the neat semiconductor. Here we show that such blends actually perform very poorly in the undoped state, and that mobility and on/off ratio are improved dramatically upon moderate doping. Structural investigations show that these blend layers feature nanometre-scale semiconductor domains and a vertical composition gradient. This particular morphology enables a quasi three-dimensional spatial distribution of semiconductor pathways within the insulating matrix, in which charge accumulation and depletion via a gate bias is substantially different from neat semiconductor, and where high on-current and low off-current are simultaneously realized in the stable doped state. Adding only 5 wt% of a semiconducting polymer to a polystyrene matrix, we realized an environmentally stable inverter with gain up to 60. Y1 - 2013 U6 - https://doi.org/10.1038/ncomms2587 SN - 2041-1723 VL - 4 IS - 1-2 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Blakesley, James C. A1 - Clubb, Helen S. A1 - Greenham, Neil C. T1 - Temperature-dependent electron and hole transport in disordered semiconducting polymers : analysis of energetic disorder N2 - We have used space-charge limited current measurements to study the mobility of holes and electrons in two fluorene-based copolymers for temperatures from 100 to 300 K. Interpreting the results using the standard analytical model produced an Arrhenius-type temperature dependence for a limited temperature range only and mobility was found to be apparently dependent on the thickness of the polymer film. To improve on this, we have interpreted our data using a numerical model that takes into account the effects of the carrier concentration and energetic disorder on transport. This accounted for the thickness dependence and gave a more consistent temperature dependence across the full range of temperatures, giving support to the extended Gaussian disorder model for transport in disordered polymers. Furthermore, we find that the same model adequately describes both electron and hole transport without the need to explicitly include a distribution of electron traps. Room-temperature mobilities were found to be in the region of 4 x 10(-8) and 2 x 10(- 8) cm(2) V-1 s(-1) in the limit of zero field and zero carrier density with disorders of 110+/-10 and 100+/-10 meV for polymers poly{9,9-dioctylfluorene-co-bis[N,N'-(4-butylphenyl)]bis(N, N'-phenyl-1,4-phenylene)diamine} and poly(9,9-dioctylfluorene-co-benzothiadiazole), respectively. Y1 - 2010 UR - http://prb.aps.org/ U6 - https://doi.org/10.1103/Physrevb.81.045210 SN - 1098-0121 ER - TY - JOUR A1 - Lange, Ilja A1 - Blakesley, James C. A1 - Frisch, Johannes A1 - Vollmer, Antje A1 - Koch, Norbert A1 - Neher, Dieter T1 - Band bending in conjugated polymer layers JF - Physical review letters N2 - We use the Kelvin probe method to study the energy-level alignment of four conjugated polymers deposited on various electrodes. Band bending is observed in all polymers when the substrate work function exceeds critical values. Through modeling, we show that the band bending is explained by charge transfer from the electrodes into a small density of states that extends several hundred meV into the band gap. The energetic spread of these states is correlated with charge-carrier mobilities, suggesting that the same states also govern charge transport in the bulk of these polymers. Y1 - 2011 U6 - https://doi.org/10.1103/PhysRevLett.106.216402 SN - 0031-9007 VL - 106 IS - 21 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Al-Sa'di, Mahmoud A1 - Jaiser, Frank A1 - Bagnich, Sergey A. A1 - Unger, Thomas A1 - Blakesley, James C. A1 - Wilke, Andreas A1 - Neher, Dieter T1 - Electrical and optical simulations of a polymer-based phosphorescent organic light-emitting diode with high efficiency JF - Journal of polymer science : B, Polymer physics N2 - A comprehensive numerical device simulation of the electrical and optical characteristics accompanied with experimental measurements of a new highly efficient system for polymer-based light-emitting diodes doped with phosphorescent dyes is presented. The system under investigation comprises an electron transporter attached to a polymer backbone blended with an electronically inert small molecule and an iridium-based green phosphorescent dye which serves as both emitter and hole transporter. The device simulation combines an electrical and an optical model. Based on the known highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) levels of all components as well as the measured electrical and optical characteristics of the devices, we model the emissive layer as an effective medium using the dye's HOMO as hole transport level and the polymer LUMO as electron transport level. By fine-tuning the injection barriers at the electron and hole-injecting contact, respectively, in simulated devices, unipolar device characteristics were fitted to the experimental data. Simulations using the so-obtained set of parameters yielded very good agreement to the measured currentvoltage, luminancevoltage characteristics, and the emission profile of entire bipolar light-emitting diodes, without additional fitting parameters. The simulation was used to gain insight into the physical processes and the mechanisms governing the efficiency of the organic light-emitting diode, including the position and extent of the recombination zone, carrier concentration profiles, and field distribution inside the device. The simulations show that the device is severely limited by hole injection, and that a reduction of the hole-injection barrier would improve the device efficiency by almost 50%. KW - conjugated polymers KW - high performance polymers KW - organic electronics KW - organic light-emitting diode KW - simulations KW - TCAD Y1 - 2012 U6 - https://doi.org/10.1002/polb.23158 SN - 0887-6266 VL - 50 IS - 22 SP - 1567 EP - 1576 PB - Wiley-Blackwell CY - Hoboken ER - TY - JOUR A1 - Gao, Feng A1 - Wang, Jianpu A1 - Blakesley, James C. A1 - Hwang, Inchan A1 - Li, Zhe A1 - Greenham, Neil C. T1 - Quantifying loss mechanisms in polymer Fullerene photovoltaic devices JF - dvanced energy materials KW - organic photovoltaics KW - recombination KW - bulk heterojunctions KW - loss mechanisms KW - drift-diffusion models Y1 - 2012 U6 - https://doi.org/10.1002/aenm.201200073 SN - 1614-6832 VL - 2 IS - 8 SP - 956 EP - 961 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Kniepert, Juliane A1 - Schubert, Marcel A1 - Blakesley, James C. A1 - Neher, Dieter T1 - Photogeneration and recombination in P3HT/PCBM solar cells probed by time-delayed collection field experiments JF - The journal of physical chemistry letters N2 - Time-delayed collection field (TDCF) experiments are performed on bulk heterojunction solar cells comprised of a blend of poly(3-hexylthiophene) and [6,6]-phenyl C-71 butyric acid methyl ester. TDCF is analogous to a pump-probe experiment using optical excitation and an electrical probe with a resolution of < 100 ns. The number of free charge carriers extracted after a short delay is found to be independent of the electric field during illumination. Also, experiments performed with a variable delay between the optical excitation and the electrical probe do not reveal any evidence for the generation of charge via field-assisted dissociation of bound long-lived polaron pairs. Photocurrent transients are well fitted by computational drift diffusion simulations with only direct generation of free charge carriers. With increasing delay times between pump and probe, two loss mechanisms are identified; first, charge-carriers are swept out of the device by the internal electric field, and second, bimolecular recombination of the remaining carriers takes place with a reduced recombination coefficient. Y1 - 2011 U6 - https://doi.org/10.1021/jz200155b SN - 1948-7185 VL - 2 IS - 7 SP - 700 EP - 705 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Blakesley, James C. A1 - Neher, Dieter T1 - Relationship between energetic disorder and open-circuit voltage in bulk heterojunction organic solar cells JF - Physical review : B, Condensed matter and materials physics N2 - We simulate organic bulk heterojunction solar cells. The effects of energetic disorder are incorporated through a Gaussian or exponential model of density of states. Analytical models of open-circuit voltage (V(OC)) are derived from the splitting of quasi-Fermi potentials. Their predictions are backed up by more complex numerical device simulations including effects such as carrier-density-dependent charge-carrier mobilities. It is predicted that the V(OC) depends on: (1) the donor-acceptor energy gap; (2) charge-carrier recombination rates; (3) illumination intensity; (4) the contact work functions (if not in the pinning regime); and (5) the amount of energetic disorder. A large degree of energetic disorder, or a high density of traps, is found to cause significant reductions in V(OC). This can explain why V(OC) is often less than expected in real devices. Energetic disorder also explains the nonideal temperature and intensity dependence of V(OC) and the superbimolecular recombination rates observed in many real bulk heterojunction solar cells. Y1 - 2011 U6 - https://doi.org/10.1103/PhysRevB.84.075210 SN - 1098-0121 VL - 84 IS - 7 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Kimber, Robin G. E. A1 - Wright, Edward N. A1 - O'Kane, Simon E. J. A1 - Walker, Alison B. A1 - Blakesley, James C. T1 - Mesoscopic kinetic Monte Carlo modeling of organic photovoltaic device characteristics JF - Physical review : B, Condensed matter and materials physics N2 - Measured mobility and current-voltage characteristics of single layer and photovoltaic (PV) devices composed of poly{9,9-dioctylfluorene-co-bis[N,N'-(4-butylphenyl)]bis(N,N'-phenyl-1,4-phenylene)diamine} (PFB) and poly(9,9-dioctylfluorene-co-benzothiadiazole) (F8BT) have been reproduced by a mesoscopic model employing the kinetic Monte Carlo (KMC) approach. Our aim is to show how to avoid the uncertainties common in electrical transport models arising from the need to fit a large number of parameters when little information is available, for example, a single current-voltage curve. Here, simulation parameters are derived from a series of measurements using a self-consistent "building-blocks" approach, starting from data on the simplest systems. We found that site energies show disorder and that correlations in the site energies and a distribution of deep traps must be included in order to reproduce measured charge mobility-field curves at low charge densities in bulk PFB and F8BT. The parameter set from the mobility-field curves reproduces the unipolar current in single layers of PFB and F8BT and allows us to deduce charge injection barriers. Finally, by combining these disorder descriptions and injection barriers with an optical model, the external quantum efficiency and current densities of blend and bilayer organic PV devices can be successfully reproduced across a voltage range encompassing reverse and forward bias, with the recombination rate the only parameter to be fitted, found to be 1 x 10(7) s(-1). These findings demonstrate an approach that removes some of the arbitrariness present in transport models of organic devices, which validates the KMC as an accurate description of organic optoelectronic systems, and provides information on the microscopic origins of the device behavior. Y1 - 2012 U6 - https://doi.org/10.1103/PhysRevB.86.235206 SN - 1098-0121 VL - 86 IS - 23 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Blakesley, James C. A1 - Schubert, Marcel A1 - Steyrleuthner, Robert A1 - Chen, Zhihua A1 - Facchetti, Antonio A1 - Neher, Dieter T1 - Time-of-flight measurements and vertical transport in a high electron-mobility polymer JF - Applied physics letters N2 - We investigate charge transport in a high-electron mobility polymer, poly(N, N-bis 2-octyldodecyl-naphthalene-1,4,5,8-bis dicarboximide-2,6-diyl-alt-5,5-2,2-bithiophene) [P(NDI2OD-T2), Polyera ActivInk (TM) N2200]. Time-of-flight measurements reveal electron mobilities approaching those measured in field-effect transistors, the highest ever recorded in a conjugated polymer using this technique. The modest temperature dependence and weak dispersion of the transients indicate low energetic disorder in this material. Steady-state electron-only current measurements reveal a barrier to injection of about 300 meV. We propose that this barrier is located within the P(NDI2OD-T2) film and arises from molecular orientation effects. Y1 - 2011 U6 - https://doi.org/10.1063/1.3657827 SN - 0003-6951 VL - 99 IS - 18 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Schubert, Marcel A1 - Preis, Eduard A1 - Blakesley, James C. A1 - Pingel, Patrick A1 - Scherf, Ullrich A1 - Neher, Dieter T1 - Mobility relaxation and electron trapping in a donor/acceptor copolymer JF - Physical review : B, Condensed matter and materials physics N2 - To address the nature of charge transport and the origin of severe (intrinsic) trapping in electron-transporting polymers, transient and steady-state charge transport measurements have been conducted on the prototype donor/acceptor copolymer poly[2,7-(9,9-dialkyl-fluorene)-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)] (PFTBTT). A charge-generation layer technique is used to selectively address transport of the desired charge carrier type, to perform time-of-flight measurements on samples with < 200 nm thickness, and to combine the time-of-flight and the photocharge extraction by linearly increasing voltage (photo-CELIV) techniques to investigate charge carrier dynamics over a wide time range. Significant trapping of free electrons is observed in the bulk of dioctyl-substituted PFTBTT (alt-PF8TBTT), introducing a strong relaxation of the charge carrier mobility with time. We used Monte-Carlo simulation to simulate the measured transient data and found that all measurements can be modeled with a single parameter set, with the charge transport behavior determined by multiple trapping and detrapping of electrons in an exponential trap distribution. The influence of the concomitant mobility relaxation on the transient photocurrent characteristics in photo-CELIV experiments is discussed and shown to explain subtle features that were seen in former publications but were not yet assigned to electron trapping. Comparable studies on PFTBTT copolymers with chemical modifications of the side chains and backbone suggest that the observed electron trapping is not caused by a distinct chemical species but rather is related to interchain interactions. Y1 - 2013 U6 - https://doi.org/10.1103/PhysRevB.87.024203 SN - 1098-0121 VL - 87 IS - 2 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Albrecht, Steve A1 - Schindler, Wolfram A1 - Kurpiers, Jona A1 - Kniepert, Juliane A1 - Blakesley, James C. A1 - Dumsch, Ines A1 - Allard, Sybille A1 - Fostiropoulos, Konstantinos A1 - Scherf, Ullrich A1 - Neher, Dieter T1 - On the field dependence of free charge carrier generation and recombination in blends of PCPDTBT/PC70BM influence of solvent additives JF - The journal of physical chemistry letters N2 - We have applied time-delayed collection field (TDCF) and charge extraction by linearly increasing voltage (CELIV) to investigate the photogeneration, transport, and recombination of charge carriers in blends composed of PCPDTBT/PC70BM processed with and without the solvent additive diiodooctane. The results suggest that the solvent additive has severe impacts on the elementary processes involved in the photon to collected electron conversion in these blends. First, a pronounced field dependence of the free carrier generation is found for both blends, where the field dependence is stronger without the additive. Second, the fate of charge carriers in both blends can be described with a rather high bimolecular recombination coefficients, which increase with decreasing internal field. Third, the mobility is three to four times higher with the additive. Both blends show a negative field dependence of mobility, which we suggest to cause bias-dependent recombination coefficients. Y1 - 2012 U6 - https://doi.org/10.1021/jz3000849 SN - 1948-7185 VL - 3 IS - 5 SP - 640 EP - 645 PB - American Chemical Society CY - Washington ER -