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

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

doi:10.1038/s41467-021-27585-x

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

Journal Article · 15 December 2021 · Nature Communications

DOI: https://doi.org/10.1038/s41467-021-27585-x · OSTI ID:1854846

Cochrane, Katherine A. ^[1];

^[2];

^[3]; Haber, Jonah B. ^[2]; Zhang, Tianyi ^[4]; Kozhakhmetov, Azimkhan ^[4]; Robinson, Joshua A. ^[4]; Terrones, Mauricio ^[4];

^[5]; Neaton, Jeffrey B. ^[6]; Weber-Bargioni, Alexander ^[1];

^[7]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Technical Univ. of Munich, Garching (Germany)
Pennsylvania State Univ., University Park, PA (United States)
Univ. of Regensburg (Germany). Inst. for Experimental and Applied Physics
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States); Kavli Energy NanoSciences Institute, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf, (Switzerland)

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 μ_B 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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1854846

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 12; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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