TY  - JOUR
AU  - Wang, Rong
AU  - Han, Leng
AU  - Li, Ning
AU  - Chochos, Christos L.
AU  - Gregoriou, Vasilis G.
AU  - Lüer, Larry
AU  - Brabec, Christoph
TI  - Reducing Voltage Losses in Organic Photovoltaics Requires Interfacial Disorder Management
JO  - Advanced energy materials
VL  - 14
IS  - 26
SN  - 1614-6832
CY  - Weinheim
PB  - Wiley-VCH
M1  - FZJ-2025-01013
SP  - 2400609
PY  - 2024
AB  - Thanks to the introduction of non-fullerene acceptors, efficiencies of organic photovoltaics are now approaching 20%. Closing the gap with inorganic photovoltaics requires minimizing voltage losses without penalizing charge extraction, for which microstructure control is crucial. However, the complex interplay between microstructure and charge generation, recombination, and extraction has so far not been unraveled. Here, a systematic study linking device performance to distinct microstructural features via machine learning is presented. Building bi-layer devices allows to separately study the influence of aggregation and disorder on the energies and lifetimes of bulk and interfacial states. Unambiguous assignments of specific structural motifs to the device photophysics are thus possible. It is found that the control of aggregation-caused quenching is decisive for the exciton splitting efficiency and thus the carrier generation. Furthermore, the static disorder at the donor–acceptor interface controls the nonradiative recombination by shifting the excited state population from the bulk toward the interface. Finally, the amount of disorder in the bulk is found decisive for charge extraction. The finding that charge generation, recombination, and extraction are controlled by distinct structural features, is the key to optimizing these motifs independently, which will pave the way for organic photovoltaics toward the detailed balance limit.
LB  - PUB:(DE-HGF)16
UR  - <Go to ISI:>//WOS:001207989700001
DO  - DOI:10.1002/aenm.202400609
UR  - https://juser.fz-juelich.de/record/1037870
ER  -