Bachellier N, Verlhac B, Garnier L, Zaldívar J, Rubio-Verdú C, Abufager P, Ormaza M, Choi D-J, Bocquet M-L, Pascual J I, Lorente N, Limot L
Université de Strasbourg, CNRS, IPCMS, UMR 7504, F-67000, Strasbourg, France.
CIC nanoGUNE, 20018, Donostia-San Sebastián, Spain.
Nat Commun. 2020 Apr 1;11(1):1619. doi: 10.1038/s41467-020-15266-0.
The electrical control and readout of molecular spin states are key for high-density storage. Expectations are that electrically-driven spin and vibrational excitations in a molecule should give rise to new conductance features in the presence of magnetic anisotropy, offering alternative routes to study and, ultimately, manipulate molecular magnetism. Here, we use inelastic electron tunneling spectroscopy to promote and detect the excited spin states of a prototypical molecule with magnetic anisotropy. We demonstrate the existence of a vibron-assisted spin excitation that can exceed in energy and in amplitude a simple excitation among spin states. This excitation, which can be quenched by structural changes in the magnetic molecule, is explained using first-principles calculations that include dynamical electronic correlations.
分子自旋态的电控制和读出是高密度存储的关键。预计在存在磁各向异性的情况下,分子中的电驱动自旋和振动激发将产生新的电导特征,为研究并最终操控分子磁性提供替代途径。在此,我们使用非弹性电子隧穿光谱来激发并检测具有磁各向异性的典型分子的激发自旋态。我们证明了存在一种振动子辅助的自旋激发,其能量和幅度可超过自旋态之间的简单激发。这种激发可被磁性分子的结构变化淬灭,我们使用包含动态电子关联的第一性原理计算对其进行了解释。