As
one of the polymer modification strategies, carboxylate functionalization
has proved effective in downshifting the energy levels and enhancing
polymer crystallinity and aggregation. However, high-performance carboxylate-containing
polymers are still limited for organic solar cells (OSCs), especially
with open-circuit voltage (V
OC) above
1.0 V. Herein, we utilize two carboxylate-functionalized wide-band
gap (WBG) donor polymers (TTC-F and TTC-Cl) to pair with two WBG electron acceptors (BTA5 and F-BTA5) for high-voltage OSCs. Due to the deeper molecular
energy levels, chlorinated polymer TTC-Cl shows higher V
OC than fluorinated polymer TTC-F. Furthermore, because of the stronger aggregation in the film, the TTC-Cl-based devices attain suppressed energetic disorders
and trap-assisted recombination, decreasing voltage loss and J
SC loss. Finally, the TTC-Cl: F-BTA5 blend achieves a higher V
OC of 1.17 V and an excellent PCE of 10.98%, one of the best results
for high-voltage carboxylate-containing polymers. In addition, the TTC-Cl: BTA5 combination demonstrates the highest V
OC of 1.25 V with an ultralow nonradiative energy
loss of 0.17 eV. Our results indicate that the carboxylate-containing
polymer donors have significant application potential for high-voltage
OSCs due to reduced energy loss and improved charge transport and
dissociation. Furthermore, the matched absorption spectra with the
indoor light sources and low voltage loss promote these material combinations
to construct high-performance indoor photovoltaics.