Coherent Vibrations Promote Charge-Transfer across a Graphene-Based Interface,Journal of the American Chemical Society

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Coherent Vibrations Promote Charge-Transfer across a Graphene-Based Interface
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-05-20 , DOI: 10.1021/jacs.3c12705
Andrea Casotto _{1,

2} , Pavel S Rukin ₃ , Elisa Fresch ₄ , Deborah Prezzi ₃ , Sonia Freddi ₁ , Luigi Sangaletti ₁ , Carlo A Rozzi ₃ , Elisabetta Collini ₄ , Stefania Pagliara ₁

Affiliation

Discerning the impact of the coherent motion of the nuclei on the timing and efficiency of charge transfer at the donor–acceptor interface is essential for designing performance-enhanced optoelectronic devices. Here, we employ an experimental approach using photocurrent detection in coherent multidimensional spectroscopy to excite a donor aromatic macrocycle and collect the charge transferred to a 2D acceptor layer. For this purpose, we prepared a cobalt phthalocyanine-graphene (CoPc–Gr) interface. Unlike blends, the well-ordered architecture achieved through the physical separation of the two layers allows us to unambiguously collect the electrical signal from graphene alone and associate it with a microscopic understanding of the whole process. The CoPc–Gr interface exhibits an ultrafast electron-transfer signal, stemming from an interlayer mechanism. Remarkably, the signal presents an oscillating time evolution modulated by coherent vibrations originating from the laser-excited CoPc states. By performing Fourier analysis on the beatings and correlating it with the Raman features, along with a comprehensive first-principles characterization of the vibrational coupling in the CoPc excited states, we successfully identify both the orbitals and molecular vibrations that promote the charge transfer at the interface.

中文翻译：

相干振动促进石墨烯界面上的电荷转移

辨别原子核的相干运动对供体-受体界面电荷转移的时间和效率的影响对于设计性能增强的光电器件至关重要。在这里，我们采用了一种实验方法，使用相干多维光谱中的光电流检测来激发供体芳香大环并收集转移到二维受体层的电荷。为此，我们制备了钴酞菁-石墨烯（CoPc-Gr）界面。与共混物不同，通过两层的物理分离实现的有序结构使我们能够明确地仅从石墨烯收集电信号，并将其与整个过程的微观理解联系起来。 CoPc-Gr 界面表现出源自层间机制的超快电子转移信号。值得注意的是，该信号呈现出由源自激光激发 CoPc 态的相干振动调制的振荡时间演化。通过对跳动进行傅立叶分析并将其与拉曼特征相关联，以及对 CoPc 激发态振动耦合的全面第一原理表征，我们成功地识别了促进界面处电荷转移的轨道和分子振动。

更新日期：2024-05-20

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