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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Solid-State Physics

Background:

  • The bulk photovoltaic effect (BPVE) describes current generation in materials lacking inversion symmetry under illumination.
  • The ballistic current, arising from asymmetric carrier generation via scattering, is a key but less understood component of BPVE.
  • Understanding both shift and ballistic currents is vital for advancing photovoltaic technologies.

Purpose of the Study:

  • To derive a first-principles-calculable formula for the ballistic current in BPVE materials.
  • To quantify the ballistic current contribution in the prototypical material BaTiO3.
  • To assess the impact of structural changes on ballistic current for future materials design.

Main Methods:

  • A perturbative approach was employed to derive the ballistic current formula.
  • Quantum-mechanical density functional theory (DFT) was used for calculations.
  • The intrinsic electron-phonon scattering was considered as the scattering mechanism.

Main Results:

  • A formula for ballistic current amenable to first-principles calculations was derived.
  • The ballistic current in BaTiO3 was calculated and found to be comparable in magnitude to the shift current.
  • The combined shift and ballistic currents accurately reproduced experimental photocurrent spectra.

Conclusions:

  • The ballistic current is a significant contributor to the bulk photovoltaic effect.
  • The derived theoretical framework enables accurate prediction and understanding of BPVE.
  • The sensitivity of ballistic current to structural changes offers a pathway for designing improved photovoltaic materials.