Ultrafast atomic-scale scanning tunnelling spectroscopy of a single vacancy in a monolayer crystal

Ultrafast atomic-scale scanning tunnelling spectroscopy of a single vacancy in a monolayer crystal

June 2024 | C. Roelcke, L. Z. Kastner, M. Graml, A. Biereder, J. Wilhelm, J. Repp, R. Huber & Y. A. Gerasimenko
This study presents a novel ultrafast atomic-scale scanning tunnelling spectroscopy (LW-STS) technique to investigate the dynamics of a single selenium (Se) vacancy in a moiré-distorted WSe₂ monolayer. The method combines atomic spatial resolution, sub-picosecond temporal resolution, and millielectronvolt energy resolution to directly observe how electron-phonon coupling modulates the spin-orbit-split energy levels of the vacancy. By locally exciting lattice vibrations and taking ultrafast energy-resolved snapshots, the researchers measure the impact of phonon interactions on the electronic structure of the defect. The results show that the lowest bound defect state experiences transient energy shifts of up to 40 meV, which are larger than thermal smearing at room temperature. This technique enables the disentanglement of key microscopic interactions in complex quantum materials, offering insights into the role of local electron-phonon coupling in emerging quantum phases. The study demonstrates the ability to control single-defect energy through ultrafast atomic motion, revealing how lattice vibrations dynamically influence defect states. The findings highlight the potential of LW-STS for studying quantum materials, providing a unique tool to engineer defect-based functionalities using phonons. The results also show that the observed energy shifts are primarily due to mechanical out-of-plane motion of the monolayer, with the oscillations in the tunnelling current attributed to changes in the tip-sample distance. The study underscores the importance of understanding electron-phonon coupling in quantum materials, paving the way for future advancements in quantum technologies.This study presents a novel ultrafast atomic-scale scanning tunnelling spectroscopy (LW-STS) technique to investigate the dynamics of a single selenium (Se) vacancy in a moiré-distorted WSe₂ monolayer. The method combines atomic spatial resolution, sub-picosecond temporal resolution, and millielectronvolt energy resolution to directly observe how electron-phonon coupling modulates the spin-orbit-split energy levels of the vacancy. By locally exciting lattice vibrations and taking ultrafast energy-resolved snapshots, the researchers measure the impact of phonon interactions on the electronic structure of the defect. The results show that the lowest bound defect state experiences transient energy shifts of up to 40 meV, which are larger than thermal smearing at room temperature. This technique enables the disentanglement of key microscopic interactions in complex quantum materials, offering insights into the role of local electron-phonon coupling in emerging quantum phases. The study demonstrates the ability to control single-defect energy through ultrafast atomic motion, revealing how lattice vibrations dynamically influence defect states. The findings highlight the potential of LW-STS for studying quantum materials, providing a unique tool to engineer defect-based functionalities using phonons. The results also show that the observed energy shifts are primarily due to mechanical out-of-plane motion of the monolayer, with the oscillations in the tunnelling current attributed to changes in the tip-sample distance. The study underscores the importance of understanding electron-phonon coupling in quantum materials, paving the way for future advancements in quantum technologies.
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Understanding Ultrafast atomic-scale scanning tunnelling spectroscopy of a single vacancy in a monolayer crystal