Gibson Andrew J, Temperton Robert H, Handrup Karsten, Weston Matthew, Mayor Louise C, O'Shea James N
School of Physics and Astronomy and Nottingham Nanotechnology and Nanoscience Centre (NNNC), University of Nottingham, Nottingham NG7 2RD, United Kingdom.
J Chem Phys. 2014 Jun 21;140(23):234708. doi: 10.1063/1.4882867.
The interaction of the dye molecule N3 (cis-bis(isothiocyanato)bis(2,2-bipyridyl-4,4'-dicarbo-xylato)-ruthenium(II)) with the ultra-thin oxide layer on a AlNi(110) substrate, has been studied using synchrotron radiation based photoelectron spectroscopy, resonant photoemission spectroscopy, and near edge X-ray absorption fine structure spectroscopy. Calibrated X-ray absorption and valence band spectra of the monolayer and multilayer coverages reveal that charge transfer is possible from the molecule to the AlNi(110) substrate via tunnelling through the ultra-thin oxide layer and into the conduction band edge of the substrate. This charge transfer mechanism is possible from the LUMO+2 and 3 in the excited state but not from the LUMO, therefore enabling core-hole clock analysis, which gives an upper limit of 6.0 ± 2.5 fs for the transfer time. This indicates that ultra-thin oxide layers are a viable material for use in dye-sensitized solar cells, which may lead to reduced recombination effects and improved efficiencies of future devices.
利用基于同步辐射的光电子能谱、共振光发射光谱和近边X射线吸收精细结构光谱,研究了染料分子N3(顺式-双(异硫氰酸根)双(2,2-联吡啶-4,4'-二羧酸根)钌(II))与AlNi(110)衬底上的超薄氧化层之间的相互作用。单层和多层覆盖的校准X射线吸收光谱和价带光谱表明,电荷可以通过超薄氧化层隧穿到衬底的导带边缘,从而从分子转移到AlNi(110)衬底。这种电荷转移机制在激发态下可能从LUMO + 2和3发生,但不是从LUMO发生,因此可以进行芯孔时钟分析,得出转移时间的上限为6.0±2.5 fs。这表明超薄氧化层是用于染料敏化太阳能电池的可行材料,这可能会降低未来器件的复合效应并提高效率。