TY  - JOUR
A1  - Schubert, Marcel
A1  - Collins, Brian A.
A1  - Mangold, Hannah
A1  - Howard, Ian A.
A1  - Schindler, Wolfram
A1  - Vandewal, Koen
A1  - Roland, Steffen
A1  - Behrends, Jan
A1  - Kraffert, Felix
A1  - Steyrleuthner, Robert
A1  - Chen, Zhihua
A1  - Fostiropoulos, Konstantinos
A1  - Bittl, Robert
A1  - Salleo, Alberto
A1  - Facchetti, Antonio
A1  - Laquai, Frederic
A1  - Ade, Harald W.
A1  - Neher, Dieter
T1  - Correlated donor/acceptor crystal orientation controls photocurrent generation in all-polymer solar cells
JF  - Advanced functional materials
N2  - New polymers with high electron mobilities have spurred research in organic solar cells using polymeric rather than fullerene acceptors due to their potential of increased diversity, stability, and scalability. However, all-polymer solar cells have struggled to keep up with the steadily increasing power conversion efficiency of polymer: fullerene cells. The lack of knowledge about the dominant recombination process as well as the missing concluding picture on the role of the semi-crystalline microstructure of conjugated polymers in the free charge carrier generation process impede a systematic optimization of all-polymer solar cells. These issues are examined by combining structural and photo-physical characterization on a series of poly(3-hexylthiophene) (donor) and P(NDI2OD-T2) (acceptor) blend devices. These experiments reveal that geminate recombination is the major loss channel for photo-excited charge carriers. Advanced X-ray and electron-based studies reveal the effect of chloronaphthalene co-solvent in reducing domain size, altering domain purity, and reorienting the acceptor polymer crystals to be coincident with those of the donor. This reorientation correlates well with the increased photocurrent from these devices. Thus, effi cient split-up of geminate pairs at polymer/polymer interfaces may necessitate correlated donor/acceptor crystal orientation, which represents an additional requirement compared to the isotropic fullerene acceptors.
Y1  - 2014
U6  - https://doi.org/10.1002/adfm.201304216
SN  - 1616-301X
SN  - 1616-3028
VL  - 24
IS  - 26
SP  - 4068
EP  - 4081
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Steyrleuthner, Robert
A1  - Schubert, Marcel
A1  - Howard, Ian
A1  - Klaumünzer, Bastian
A1  - Schilling, Kristian
A1  - Chen, Zhihua
A1  - Saalfrank, Peter
A1  - Laquai, Frederic
A1  - Facchetti, Antonio
A1  - Neher, Dieter
T1  - Aggregation in a high-mobility n-type low-bandgap copolymer with implications on semicrystalline morphology
JF  - Journal of the American Chemical Society
N2  - We explore the photophysics of P(NDI2OD-T2), a high-mobility and air-stable n-type donor/acceptor polymer. Detailed steady-state UV-vis and photoluminescence (PL) measurements on solutions of P(NDI2OD-T2) reveal distinct signatures of aggregation. By performing quantum chemical calculations, we can assign these spectral features to unaggregated and stacked polymer chains. NMR measurements independently confirm the aggregation phenomena of P(NDI2OD-T2) in solution. The detailed analysis of the optical spectra shows that aggregation is a two-step process with different types of aggregates, which we confirm by time-dependent PL measurements. Analytical ultracentrifugation measurements suggest that aggregation takes place within the single polymer chain upon coiling. By transferring these results to thin P(NDI2OD-T2) films, we can conclude that film formation is mainly governed by the chain collapse, leading in general to a high aggregate content of similar to 45%. This process also inhibits the formation of amorphous and disordered P(NDI2OD-T2) films.
Y1  - 2012
U6  - https://doi.org/10.1021/ja306844f
SN  - 0002-7863
VL  - 134
IS  - 44
SP  - 18303
EP  - 18317
PB  - American Chemical Society
CY  - Washington
ER  -