Intrinsic Defect-Induced Local Semiconducting-to-Metallic Regions Within Monolayer 1T-TiS2 Displayed by First-Principles Calculations and Scanning Tunneling Microscopy

Keeney, P. J.; Coelho, P. M.; Haraldsen, J. T.

doi:10.3390/cryst15030243

Intrinsic Defect-Induced Local Semiconducting-to-Metallic Regions Within Monolayer 1T-TiS2 Displayed by First-Principles Calculations and Scanning Tunneling Microscopy

Journal Article · Sun Mar 02 23:00:00 EST 2025 · Crystals

DOI:https://doi.org/10.3390/cryst15030243· OSTI ID:2525968

Keeney, P. J.; Coelho, P. M.;

Using density functional theory (DFT) and scanning tunneling microscopy (STM), the intrinsic point defects, formation energy, and electronic structure of 1T-TiS2 were investigated. Defect systems include single-atom vacancies, interstitial and adatom additions, and direct atomic substitution. Using a collective approach for analyzing realistic systems for point defect investigation, we provide a more straightforward comparison to the experimental measurements, reproducing more realistic environmental conditions related to thin film growth. STM images are compared to computationally simulated electron density images to identify specific geometries that result from favorable point defects. DFT suggests that titanium interstitials are the most energetically favorable intrinsic defect, and sulfur vacancies are more likely to form than titanium vacancies within this realistic analysis, which is in agreement with STM data. A pristine, stoichiometric monolayer system is calculated to have a direct band gap of 0.422 eV, which varies based on local point defects. Local semiconducting-to-metallic electronic transitions are predicted to occur based on the presence of Ti interstitials.

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Sponsoring Organization:: USDOE

OSTI ID:: 2525968

Journal Information:: Crystals, Journal Name: Crystals Journal Issue: 3 Vol. 15; ISSN CRYSBC; ISSN 2073-4352

Publisher:: MDPI AGCopyright Statement

Country of Publication:: Germany

Language:: English

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