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Ultrahigh Concentration Hydrogen Doping into TiO2.

GyeongCheol Lim1, Muhammad Irfandi2, Ryo Nakayama1,3

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|November 7, 2024
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Ultrahigh concentration doping of hydrogen (H) into rutile titanium dioxide (TiO2) was achieved at low temperatures. This low-temperature irradiation created metastable in-gap states, altering electrical properties.

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Area of Science:

  • Materials Science
  • Solid State Physics
  • Surface Science

Background:

  • Rutile titanium dioxide (TiO2) is a widely studied material with applications in catalysis and electronics.
  • Controlling hydrogen incorporation in TiO2 is crucial for tuning its electronic and optical properties.
  • Previous studies were limited in achieving high hydrogen concentrations in TiO2.

Purpose of the Study:

  • To investigate ultrahigh concentration doping of hydrogen into rutile TiO2 (100) single crystals.
  • To understand the effects of low-temperature hydrogen irradiation on TiO2.
  • To characterize the resulting electronic properties and defect structures.

Main Methods:

  • Low-energy hydrogen ion beam irradiation at low temperature (50 K).
  • In situ nuclear reaction analysis (NRA) for hydrogen concentration measurement.
  • In situ transport and photoemission measurements.
  • Density functional theory (DFT) calculations.

Main Results:

  • Achieved ultrahigh hydrogen doping concentration up to H1.2TiO2, significantly higher than at room temperature.
  • Observed a large lattice expansion, indicating hydrogen occupation of interstitial sites.
  • Identified that excess hydrogen generates a deeper, metastable in-gap state (IGS).
  • Observed unusual electrical transport properties after postannealing.

Conclusions:

  • Low-temperature irradiation is an effective method for ultrahigh hydrogen doping in rutile TiO2.
  • The generated metastable IGS, possibly due to double interstitial hydrogens, significantly impacts electrical properties.
  • This work provides insights into defect engineering in TiO2 for potential electronic applications.