We have studied the utilization of PCDTBT, an alternating poly(2,7-carbazole) derivative, in organic bulk heterojunction solar cells. The effect of polymer molecular weight, PCDTBT:[60]PCBM ratio, and active layer thickness on the device performance is reported. The best performance was obtained when the number-average molecular weights (Mn) are around 20 kDa with a polydispersity index around 2.2. Both PCDTBT:[60]PCBM ratio and active layer thickness affect the light absorption and the charge transport properties. By optimizing these two parameters, power conversion efficiency (PCE) up to 4.35% was reached under calibrated AM1.5G illumination of 100 mW cm−2. When blended with [70]PCBM, PCDTBT exhibited a PCE up to 4.6%.
    
         
            
                     
                    
                        
                            
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