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First-principles calculations of quantum defects in bulk WS2: Effect of carbon doping in spin-photon interfaces

Petros-Panagis Filippatos1, Tom J. P. Irons1, Navaratnarajah Kuganathan2, and Alexander Chroneos2,3

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Phys. Rev. B 113, 165202 – Published 6 April, 2026

DOI: https://doi.org/10.1103/d3bx-gnhq

Abstract

Point defects in two-dimensional and layered materials have attracted considerable interest as promising qubit candidates for quantum information processing due to their highly localized electronic states and spin-dependent optical properties. In this work, we use r2SCAN density functional calculations combined with complete active space self-consistent field theory to investigate bulk carbon-doped tungsten disulfide (WS2) as a potential platform for scalable quantum technologies. The meta-generalized gradient approximation exchange-correlation functional r2SCAN is found to offer a balance between accuracy and computational efficiency for specific properties, while its performance has not been tested in bulk WS2 before. By substituting sulphur atoms with carbon impurities, we achieve stable paramagnetic excited states characterized by well-defined defect levels deep within the band gap. Moreover, we investigate the zero-phonon line, radiative lifetime, and zero-field splitting due to the carbon impurities. The presence of tungsten introduces relativistic effects which are desired for some quantum applications, facilitating efficient initialization, coherent manipulation, and readout of defect spin states. We elucidate the role of carbon in lowering the emission energies into technologically relevant wavelengths for quantum information science, while we compare the present results with the extensively investigated monolayer structure. Our results highlight carbon-doped WS2 as an attractive solid-state quantum platform due to its zero-phonon line, zero-field splitting, and radiative lifetime values, enabling robust optical control and manipulation of spin states for quantum applications.

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Phys. Rev. B 113, 165202– Published 6 April, 2026
  • Received 20 June 2025
  • Revised 18 November 2025
  • Accepted 6 March 2026
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