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

Author

Listed:
  • Katherine A. Cochrane

    (Lawrence Berkeley National Laboratory)

  • Jun-Ho Lee

    (Lawrence Berkeley National Laboratory
    University of California at Berkeley)

  • Christoph Kastl

    (Technical University of Munich)

  • Jonah B. Haber

    (Lawrence Berkeley National Laboratory
    University of California at Berkeley)

  • Tianyi Zhang

    (The Pennsylvania State University
    The Pennsylvania State University)

  • Azimkhan Kozhakhmetov

    (The Pennsylvania State University)

  • Joshua A. Robinson

    (The Pennsylvania State University
    The Pennsylvania State University)

  • Mauricio Terrones

    (The Pennsylvania State University
    The Pennsylvania State University
    The Pennsylvania State University)

  • Jascha Repp

    (University of Regensburg)

  • Jeffrey B. Neaton

    (Lawrence Berkeley National Laboratory
    University of California at Berkeley
    Kavli Energy Nanosciences Institute at Berkeley)

  • Alexander Weber-Bargioni

    (Lawrence Berkeley National Laboratory)

  • Bruno Schuler

    (Lawrence Berkeley National Laboratory
    Empa—Swiss Federal Laboratories for Materials Science and Technology)

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.

Suggested Citation

  • 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 Webe, 2021. "Spin-dependent vibronic response of a carbon radical ion in two-dimensional WS2," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-27585-x
    DOI: 10.1038/s41467-021-27585-x
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    Cited by:

    1. John C. Thomas & Wei Chen & Yihuang Xiong & Bradford A. Barker & Junze Zhou & Weiru Chen & Antonio Rossi & Nolan Kelly & Zhuohang Yu & Da Zhou & Shalini Kumari & Edward S. Barnard & Joshua A. Robinson, 2024. "A substitutional quantum defect in WS2 discovered by high-throughput computational screening and fabricated by site-selective STM manipulation," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Song Li & Gergő Thiering & Péter Udvarhelyi & Viktor Ivády & Adam Gali, 2022. "Carbon defect qubit in two-dimensional WS2," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    3. Feifei Xiang & Lysander Huberich & Preston A. Vargas & Riccardo Torsi & Jonas Allerbeck & Anne Marie Z. Tan & Chengye Dong & Pascal Ruffieux & Roman Fasel & Oliver Gröning & Yu-Chuan Lin & Richard G. , 2024. "Charge state-dependent symmetry breaking of atomic defects in transition metal dichalcogenides," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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