Warner Ben, Oberg Jenny C, Gill Tobias G, El Hallak Fadi, Hirjibehedin Cyrus F, Serri Michele, Heutz Sandrine, Arrio Marie-Anne, Sainctavit Philippe, Mannini Matteo, Poneti Giordano, Sessoli Roberta, Rosa Patrick
#Department of Materials and London Centre for Nanotechnology, Imperial College London, London, United Kingdom.
¶Institut de Minéralogie et de Physique des Milieux Condensés, UMR7590, Université Pierre et Marie Curie, Paris, France.
J Phys Chem Lett. 2013 May 2;4(9):1546-52. doi: 10.1021/jz4005619. Epub 2013 Apr 22.
Using X-ray absorption techniques, we show that temperature- and light-induced spin crossover properties are conserved for a submonolayer of the [Fe(H2B(pz)2)2(2,2'-bipy)] complex evaporated onto a Au(111) surface. For a significant fraction of the molecules, we see changes in the absorption at the L2,3 edges that are consistent with those observed in bulk and thick film references. Assignment of these changes to spin crossover is further supported by multiplet calculations to simulate the X-ray absorption spectra. As others have observed in experiments on monolayer coverages, we find that many molecules in our submonolayer system remain pinned in one of the two spin states. Our results clearly demonstrate that temperature- and light-induced spin crossover is possible for isolated molecules on surfaces but that interactions with the surface may play a key role in determining when this can occur.
利用X射线吸收技术,我们表明,蒸发到Au(111)表面的[Fe(H2B(pz)2)2(2,2'-联吡啶)]配合物亚单层的温度和光诱导自旋交叉性质得以保留。对于相当一部分分子,我们观察到L2,3边缘处吸收的变化,这与在体相和厚膜参比物中观察到的变化一致。通过多重态计算来模拟X射线吸收光谱,进一步支持了将这些变化归因于自旋交叉。正如其他人在单层覆盖实验中所观察到的那样,我们发现在我们的亚单层系统中,许多分子保持固定在两种自旋态之一。我们的结果清楚地表明,表面上的孤立分子可能发生温度和光诱导自旋交叉,但与表面的相互作用可能在决定何时会发生这种情况方面起关键作用。