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arXiv 2011.09870cond-mat.mes-hall
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原子力显微镜探测分子激发态

Probing molecular excited states by atomic force microscopy

Shadi Fatayer, Florian Albrecht, Ivano Tavernelli, Mats Persson, Nikolaj Moll, Leo Gross

摘要:

采用单电荷注入原子力显微镜,我们研究了一个分子在多层绝缘膜上的氧化还原反应。首先,我们通过连接一个空穴使分子带正电。然后,我们通过附加一个电子来中和它,并观察到三个中和通道。我们合理化,这三个通道对应于过渡到中性基态,最低能量的三重态激发态和最低能量的单重态激发态。通过单电子隧穿光谱,我们测量了三重态和单重态激发态能量的跃迁之间的能量差。实验值与密度泛函理论计算的激发态能量进行了比较。我们的研究结果表明,激发态的分子可以制备和光学带隙的能量可以通过控制单电荷注入量化。我们的工作展示了访问,并提供洞察,无处不在的电子附着过程相关的激发态跃迁的重要电子转移和分子光电子学现象的表面。

英文摘要:

By employing single charge injections with an atomic force microscope, we investigated redox reactions of a molecule on a multilayer insulating film. First, we charged the molecule positively by attaching a single hole. Then we neutralized it by attaching an electron and observed three channels for the neutralization. We rationalize that the three channels correspond to transitions to the neutral ground state, to the lowest energy triplet excited states and to the lowest energy singlet excited states. By single-electron tunneling spectroscopy we measured the energy differences between the transitions obtaining triplet and singlet excited state energies. The experimental values are compared with density functional theory calculations of the excited state energies. Our results show that molecules in excited states can be prepared and that energies of optical gaps can be quantified by controlled single-charge injections. Our work demonstrates the access to, and provides insight into, ubiquitous electron-attachment processes related to excited-state transitions important in electron transfer and molecular optoelectronics phenomena on surfaces.

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