Pendlebury Stephanie R, Wang Xiuli, Le Formal Florian, Cornuz Maurin, Kafizas Andreas, Tilley S David, Grätzel Michael, Durrant James R
Department of Chemistry, Imperial College London, South Kensington Campus , London, SW7 2AZ, United Kingdom.
J Am Chem Soc. 2014 Jul 16;136(28):9854-7. doi: 10.1021/ja504473e. Epub 2014 Jul 2.
Transient absorption spectroscopy on subpicosecond to second time scales is used to investigate photogenerated charge carrier recombination in Si-doped nanostructured hematite (α-Fe2O3) photoanodes as a function of applied bias. For unbiased hematite, this recombination exhibits a 50% decay time of ~6 ps, ~10(3) times faster than that of TiO2 under comparable conditions. Anodic bias significantly retards hematite recombination dynamics, and causes the appearance of electron trapping on ps-μs time scales. These ultrafast recombination dynamics, their retardation by applied bias, and the associated electron trapping are discussed in terms of their implications for efficient water oxidation.
利用亚皮秒到秒时间尺度的瞬态吸收光谱来研究硅掺杂的纳米结构赤铁矿(α-Fe₂O₃)光阳极中光生电荷载流子的复合情况,该复合情况是施加偏压的函数。对于无偏压的赤铁矿,这种复合表现出约6皮秒的50%衰减时间,比在可比条件下的TiO₂快约10³倍。阳极偏压显著延缓了赤铁矿的复合动力学,并导致在皮秒到微秒时间尺度上出现电子俘获现象。根据它们对高效水氧化的影响,对这些超快复合动力学、施加偏压对其的延缓作用以及相关的电子俘获现象进行了讨论。