Tip-induced creation and Jahn-Teller distortions of sulfur vacancies in single-layer MoS$_{2}$

TL;DR

This paper introduces a precise STM-based method to create and manipulate sulfur vacancies in single-layer MoS₂, revealing Jahn-Teller distortions and hybrid orbitals, with potential for engineering electronic properties.

Contribution

The study demonstrates a novel technique combining STM and Fe atoms to controllably create and analyze sulfur vacancies and their distortions in MoS₂.

Findings

STM tip can induce Jahn-Teller distorted states in sulfur vacancies

Density functional theory supports experimental observations

Evidence of hybrid orbitals in vacancy dimers

Abstract

We present an atomically precise technique to create sulfur vacancies and control their atomic configurations in single-layer MoS$_{2}$. It involves adsorbed Fe atoms and the tip of a scanning tunneling microscope, which enables single sulfur removal from the top sulfur layer at the initial position of Fe. Using scanning tunneling spectroscopy, we show that the STM tip can also induce two Jahn-Teller distorted states with reduced orbital symmetry in the sulfur vacancies. Density functional theory calculations rationalize our experimental results. Additionally, we provide evidence for molecule-like hybrid orbitals in artificially created sulfur vacancy dimers, which illustrates the potential of our technique for the development of extended defect lattices and tailored electronic band structures.