High
tolerance regarding photovoltaic performance in terms of donor:acceptor
(D:A) composition ratio is reported for all-polymer solar cells (all-PSCs),
which is a crucial advantage in producing large-scale devices with
high reproducibility. To understand the origin of high D:A ratio tolerance
in all-PSCs, we investigate the molecular weight (MW) effects of the
P(NDI2OD-T2) polymer acceptor (P
A) on
photovoltaic and mechanical robustness of PBDB-T:P(NDI2OD-T2) all-PSCs.
Also, we compare the all-PSCs with other types of PSCs consisting
of the same polymer donor but using small molecule acceptors (SMAs)
including ITIC and PC71BM. We observe that the D:A ratio
tolerances of both the photovoltaic and mechanical properties are
highly dependent on the P
A MW and the
acceptor material types. For example, at a high D:A ratio of 15:1,
all-PSCs using high MW P
A (number-average
molecular weight (M
n) = 97 kg mol–1) exhibit 13 times higher normalized power conversion
efficiency (PCE) than all-PSCs using low MW P
A (M
n = 11 kg mol–1), and 20 times higher than ITIC-based PSCs. In addition, the electron
mobilities in all-PSCs based on high MW P
A are well-maintained even at very high D:A ratio, whereas the electron
mobilities in low MW P
A all-PSCs and SMA-based
PSCs decrease by 3- and 4-orders of magnitude, respectively, when
the D:A ratio increases from 1:1 to 15:1. Thus, we suggest that the
formation of tie molecules and chain entanglements by long polymer
chains bridging adjacent crystalline domains is the main origin of
excellent D:A tolerance in both mechanical robustness and photovoltaic
performance. This work provides an important material design guideline
for the reproducible production of flexible and stretchable all-PSCs.