Spin-dependent vibronic response of a carbon radical ion in two-dimensional WS2

Katherine A. Cochrane, Jun Ho Lee, Christoph Kastl, Jonah B. Haber, Tianyi Zhang, Azimkhan Kozhakhmetov, Joshua A. Robinson, Mauricio Terrones, Jascha Repp, Jeffrey B. Neaton, Alexander Weber-Bargioni, Bruno Schuler

Research output: Contribution to journalArticlepeer-review

19 Scopus citations

Abstract

Atomic spin centers in 2D materials are a highly anticipated building block for quantum technologies. Here, we demonstrate the creation of an effective spin-1/2 system via the atomically controlled generation of magnetic carbon radical ions (CRIs) in synthetic two-dimensional transition metal dichalcogenides. Hydrogenated carbon impurities located at chalcogen sites introduced by chemical doping are activated with atomic precision by hydrogen depassivation using a scanning probe tip. In its anionic state, the carbon impurity is computed to have a magnetic moment of 1 μB resulting from an unpaired electron populating a spin-polarized in-gap orbital. We show that the CRI defect states couple to a small number of local vibrational modes. The vibronic coupling strength critically depends on the spin state and differs for monolayer and bilayer WS2. The carbon radical ion is a surface-bound atomic defect that can be selectively introduced, features a well-understood vibronic spectrum, and is charge state controlled.

Original languageEnglish (US)
Article number7287
JournalNature communications
Volume12
Issue number1
DOIs
StatePublished - Dec 2021

All Science Journal Classification (ASJC) codes

  • General Chemistry
  • General Biochemistry, Genetics and Molecular Biology
  • General Physics and Astronomy

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