Enhanced performance of dye-sensitized solar cells by an Al2O3 charge-recombination barrier formed by low-temperature atomic layer deposition

Abstract

Al₂O₃ films are deposited conformally and uniformly by atomic layer deposition (ALD) at 150 °C throughout the surface of the nanoporous TiO₂electrode of dye-sensitized solar cells (DSSCs) to serve as charge recombination barriers (CRB). The self-limiting film growth of ALD enables detailed analysis of the thickness dependence of the CRB effects on the DSSCs, revealing the optimal Al₂O₃ CRB thickness to be that produced by 1 ALD cycle (nominal thickness = 0.1 nm), at which the CRB increases the power conversion efficiency (PCE) of the DSSCs by 14% (to up to 7.8% PCE). Above 1 cycle, the ALD films excessively raise the Fermi level of the TiO₂electrode surface, as determined by ultraviolet photoelectron spectroscopy (UPS), so as to block electron injection at the dye-to-TiO₂ heterojunction and to cause significant degradation in the DSSC performance. Instead of its nominal 0.1 nm thickness, the 1-cycle ALD film has an effective CRB thickness of 0.3 nm because of steric hindrance among the ALD precursor molecules and the dye molecules, as analyzed by a graphical model. The optimal thickness of the ALD Al₂O₃ CRB is considerably thinner than the 0.9–2.5 nm reported for Al₂O₃ CRB formed by conventional sol-gel processes, but it should better reflect the true value, considering the better infiltrating capability and finer thickness resolution of the ALD films. The low temperature and fine thickness control of the ALD process will broaden the utility of CRB.