TY  - JOUR
A1  - Roland, Steffen
A1  - Kniepert, Juliane
A1  - Love, John A.
A1  - Negi, Vikas
A1  - Liu, Feilong
A1  - Bobbert, Peter
A1  - Melianas, Armantas
A1  - Kemerink, Martijn
A1  - Hofacker, Andreas
A1  - Neher, Dieter
T1  - Equilibrated Charge Carrier Populations Govern Steady-State Nongeminate Recombination in Disordered Organic Solar Cells
JF  - The journal of physical chemistry letters
N2  - We employed bias-assisted charge extraction techniques to investigate the transient and steady-state recombination of photogenerated charge carriers in complete devices of a disordered polymer-fullerene blend. Charge recombination is shown to be dispersive, with a significant slowdown of the recombination rate over time, consistent with the results from kinetic Monte Carlo simulations. Surprisingly, our experiments reveal little to no contributions from early time recombination of nonequilibrated charge carriers to the steady-state recombination properties. We conclude that energetic relaxation of photogenerated carriers outpaces any significant nongeminate recombination under application-relevant illumination conditions. With equilibrated charges dominating the steady-state recombination, quasi-equilibrium concepts appear suited for describing the open-circuit voltage of organic solar cells despite pronounced energetic disorder.
Y1  - 2019
U6  - https://doi.org/10.1021/acs.jpclett.9b00516
SN  - 1948-7185
VL  - 10
IS  - 6
SP  - 1374
EP  - 1381
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Kniepert, Juliane
A1  - Paulke, Andreas
A1  - Perdigon-Toro, Lorena
A1  - Kurpiers, Jona
A1  - Zhang, Huotian
A1  - Gao, Feng
A1  - Yuan, Jun
A1  - Zou, Yingping
A1  - Le Corre, Vincent M.
A1  - Koster, Lambert Jan Anton
A1  - Neher, Dieter
T1  - Reliability of charge carrier recombination data determined with charge extraction methods
JF  - Journal of applied physics
N2  - Charge extraction methods are popular for measuring the charge carrier density in thin film organic solar cells and to draw conclusions about the order and coefficient of nongeminate charge recombination. However, results from such studies may be falsified by inhomogeneous steady state carrier profiles or surface recombination. Here, we present a detailed drift-diffusion study of two charge extraction methods, bias-assisted charge extraction (BACE) and time-delayed collection field (TDCF). Simulations are performed over a wide range of the relevant parameters. Our simulations reveal that both charge extraction methods provide reliable information about the recombination order and coefficient if the measurements are performed under appropriate conditions. However, results from BACE measurements may be easily affected by surface recombination, in particular for small active layer thicknesses and low illumination densities. TDCF, on the other hand, is more robust against surface recombination due to its transient nature but also because it allows for a homogeneous high carrier density to be inserted into the active layer. Therefore, TDCF is capable to provide meaningful information on the order and coefficient of recombination even if the model conditions are not exactly fulfilled. We demonstrate this for an only 100 nm thick layer of a highly efficient nonfullerene acceptor (NFA) blend, comprising the donor polymer PM6 and the NFA Y6. TDCF measurements were performed as a function of delay time for different laser fluences and bias conditions. The full set of data could be consistently fitted by a strict second order recombination process, with a bias- and fluence-independent bimolecular recombination coefficient k(2) = 1.7 x 10(-17)m(3) s(-1). BACE measurements performed on the very same layer yielded the identical result, despite the very different excitation conditions. This proves that recombination in this blend is mostly through processes in the bulk and that surface recombination is of minor importance despite the small active layer thickness. Published under license by AIP Publishing.
Y1  - 2019
U6  - https://doi.org/10.1063/1.5129037
SN  - 0021-8979
SN  - 1089-7550
VL  - 126
IS  - 20
PB  - American Institute of Physics
CY  - Melville
ER  - 
TY  - JOUR
A1  - Paulke, Andreas
A1  - Stranks, Samuel D.
A1  - Kniepert, Juliane
A1  - Kurpiers, Jona
A1  - Wolff, Christian Michael
A1  - Schön, Natalie
A1  - Snaith, Henry J.
A1  - Brenner, Thomas J. K.
A1  - Neher, Dieter
T1  - Charge carrier recombination dynamics in perovskite and polymer solar cells
JF  - Applied physics letters
N2  - Time-delayed collection field experiments are applied to planar organometal halide perovskite (CH3NH3PbI3) based solar cells to investigate charge carrier recombination in a fully working solar cell at the nanosecond to microsecond time scale. Recombination of mobile (extractable) charges is shown to follow second-order recombination dynamics for all fluences and time scales tested. Most importantly, the bimolecular recombination coefficient is found to be time-dependent, with an initial value of ca. 10(-9) cm(3)/s and a progressive reduction within the first tens of nanoseconds. Comparison to the prototypical organic bulk heterojunction device PTB7:PC71BM yields important differences with regard to the mechanism and time scale of free carrier recombination. (C) 2016 AIP Publishing LLC.
Y1  - 2016
U6  - https://doi.org/10.1063/1.4944044
SN  - 0003-6951
SN  - 1077-3118
VL  - 108
SP  - 252
EP  - 262
PB  - American Institute of Physics
CY  - Melville
ER  - 
TY  - JOUR
A1  - Neher, Dieter
A1  - Kniepert, Juliane
A1  - Elimelech, Arik
A1  - Koster, L. Jan Anton
T1  - A New Figure of Merit for Organic Solar Cells with Transport-limited Photocurrents
JF  - Scientific reports
N2  - Compared to their inorganic counterparts, organic semiconductors suffer from relatively low charge carrier mobilities. Therefore, expressions derived for inorganic solar cells to correlate characteristic performance parameters to material properties are prone to fail when applied to organic devices. This is especially true for the classical Shockley-equation commonly used to describe current-voltage (JV)-curves, as it assumes a high electrical conductivity of the charge transporting material. Here, an analytical expression for the JV-curves of organic solar cells is derived based on a previously published analytical model. This expression, bearing a similar functional dependence as the Shockley-equation, delivers a new figure of merit a to express the balance between free charge recombination and extraction in low mobility photoactive materials. This figure of merit is shown to determine critical device parameters such as the apparent series resistance and the fill factor.
Y1  - 2016
U6  - https://doi.org/10.1038/srep24861
SN  - 2045-2322
VL  - 6
SP  - E2348
EP  - E2349
PB  - Nature Publ. Group
CY  - London
ER  - 
TY  - JOUR
A1  - Lange, Ilja
A1  - Reiter, Sina
A1  - Kniepert, Juliane
A1  - Piersimoni, Fortunato
A1  - Paetzel, Michael
A1  - Hildebrandt, Jana
A1  - Brenner, Thomas J. K.
A1  - Hecht, Stefan
A1  - Neher, Dieter
T1  - Zinc oxide modified with benzylphosphonic acids as transparent electrodes in regular and inverted organic solar cell structures
JF  - Applied physics letters
N2  - An approach is presented to modify the work function of solution-processed sol-gel derived zinc oxide (ZnO) over an exceptionally wide range of more than 2.3 eV. This approach relies on the formation of dense and homogeneous self-assembled monolayers based on phosphonic acids with different dipole moments. This allows us to apply ZnO as charge selective bottom electrodes in either regular or inverted solar cell structures, using poly(3-hexylthiophene): phenyl-C71-butyric acid methyl ester as the active layer. These devices compete with or even surpass the performance of the reference on indium tin oxide/poly(3,4-ethylenedioxythiophene) polystyrene sulfonate. Our findings highlight the potential of properly modified ZnO as electron or hole extracting electrodes in hybrid optoelectronic devices. (C) 2015 AIP Publishing LLC.
Y1  - 2015
U6  - https://doi.org/10.1063/1.4916182
SN  - 0003-6951
SN  - 1077-3118
VL  - 106
IS  - 11
PB  - American Institute of Physics
CY  - Melville
ER  - 
TY  - JOUR
A1  - Kniepert, Juliane
A1  - Lange, Ilja
A1  - Heidbrink, Jan
A1  - Kurpiers, Jona
A1  - Brenner, Thomas J. K.
A1  - Koster, L. Jan Anton
A1  - Neher, Dieter
T1  - Effect of Solvent Additive on Generation, Recombination, and Extraction in PTB7:PCBM Solar Cells: A Conclusive Experimental and Numerical Simulation Study
JF  - The journal of physical chemistry : C, Nanomaterials and interfaces
N2  - Time-delayed collection field (TDCF), bias-assisted charge extraction (BACE), and space charge-limited current (SCLC) measurements are combined with complete numerical device simulations to unveil the effect of the solvent additive 1,8-diiodooctane (DIO) on the performance of PTB7:PCBM bulk heterojunction solar cells. DIO is shown to increase the charge generation rate, reduce geminate and bimolecular recombination, and increase the electron mobility. In total, the reduction of loss currents by processing with the additive raises the power conversion efficiency of the PTB7:PCBM blend by a factor of almost three. The lower generation rates and higher geminate recombination losses in devices without DIO are consistent with a blend morphology comprising large fullerene clusters embedded within a PTB7-rich matrix, while the low electron mobility suggests that these fullerene clusters are themselves composed of smaller pure fullerene aggregates separated by disordered areas. Our device simulations show unambiguously that the effect of the additive on the shape of the currentvoltage curve (J-V) cannot be ascribed to the variation of only the mobility, the recombination, or the field dependence of generation. It is only when the changes of all three parameters are taken into account that the simulation matches the experimental J-V characteristics under all illumination conditions and for a wide range of voltages.
Y1  - 2015
U6  - https://doi.org/10.1021/jp512721e
SN  - 1932-7447
VL  - 119
IS  - 15
SP  - 8310
EP  - 8320
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Bartesaghi, Davide
A1  - Perez, Irene del Carmen
A1  - Kniepert, Juliane
A1  - Roland, Steffen
A1  - Turbiez, Mathieu
A1  - Neher, Dieter
A1  - Koster, L. Jan Anton
T1  - Competition between recombination and extraction of free charges determines the fill factor of organic solar cells
JF  - Nature Communications
N2  - Among the parameters that characterize a solar cell and define its power-conversion efficiency, the fill factor is the least well understood, making targeted improvements difficult. Here we quantify the competition between charge extraction and recombination by using a single parameter theta, and we demonstrate that this parameter is directly related to the fill factor of many different bulk-heterojunction solar cells. Our finding is supported by experimental measurements on 15 different donor: acceptor combinations, as well as by drift-diffusion simulations of organic solar cells in which charge-carrier mobilities, recombination rate, light intensity, energy levels and active-layer thickness are all varied over wide ranges to reproduce typical experimental conditions. The results unify the fill factors of several very different donor: acceptor combinations and give insight into why fill factors change so much with thickness, light intensity and materials properties. To achieve fill factors larger than 0.8 requires further improvements in charge transport while reducing recombination.
Y1  - 2015
U6  - https://doi.org/10.1038/ncomms8083
SN  - 2041-1723
VL  - 6
PB  - Nature Publ. Group
CY  - London
ER  - 
TY  - JOUR
A1  - Foertig, Alexander
A1  - Kniepert, Juliane
A1  - Gluecker, Markus
A1  - Brenner, Thomas J. K.
A1  - Dyakonov, Vladimir
A1  - Neher, Dieter
A1  - Deibel, Carsten
T1  - Nongeminate and geminate recombination in PTB7: PCBM solar cells
JF  - Advanced functional materials
KW  - organic semiconductors
KW  - organic solar cells
KW  - conjugated polymers
KW  - charge carrier recombination
Y1  - 2014
U6  - https://doi.org/10.1002/adfm.201302134
SN  - 1616-301X
SN  - 1616-3028
VL  - 24
IS  - 9
SP  - 1306
EP  - 1311
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Kniepert, Juliane
A1  - Lange, Ilja
A1  - van der Kaap, Niels J.
A1  - Koster, L. Jan Anton
A1  - Neher, Dieter
T1  - A conclusive view on charge generation, recombination, and extraction in As-prepared and annealed P3HT:PCBM blends: combined experimental and simulation work
JF  - dvanced energy materials
N2  - Time-delayed collection field (TDCF) and bias-amplified charge extraction (BACE) are applied to as-prepared and annealed poly(3-hexylthiophene):[6,6]-phenyl C-71 butyric acid methyl ester (P3HT:PCBM) blends coated from chloroform. Despite large differences in fill factor, short-circuit current, and power conversion efficiency, both blends exhibit a negligible dependence of photogeneration on the electric field and strictly bimolecular recombination (BMR) with a weak dependence of the BMR coefficient on charge density. Drift-diffusion simulations are performed using the measured coefficients and mobilities, taking into account bimolecular recombination and the possible effects of surface recombination. The excellent agreement between the simulation and the experimental data for an intensity range covering two orders of magnitude indicates that a field-independent generation rate and a density-independent recombination coefficient describe the current-voltage characteristics of the annealed P3HT: PCBM devices, while the performance of the as-prepared blend is shown to be limited by space charge effects due to a low hole mobility. Finally, even though the bimolecular recombination coefficient is small, surface recombination is found to be a negligible loss mechanism in these solar cells.
Y1  - 2014
U6  - https://doi.org/10.1002/aenm.201301401
SN  - 1614-6832
SN  - 1614-6840
VL  - 4
IS  - 7
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  -