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Ab Initio Self-Trapped Excitons.

Yunfei Bai1,2, Yaxian Wang1, Sheng Meng1,2,3

  • 1Beijing National Laboratory for Condensed Matter Physics and <a href="https://ror.org/05cvf7v30">Institute of Physics, Chinese Academy of Sciences</a>, Beijing 100190, China.

Physical Review Letters
|August 9, 2024
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Summary
This summary is machine-generated.

We developed a new computational method to study self-trapped excitons (STEs) in materials. This framework accurately predicts material properties like Stokes shift and phonon generation, guiding future experimental research.

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Computational Chemistry

Background:

  • Self-trapped excitons (STEs) are crucial for understanding optical and electronic properties of insulators and semiconductors.
  • Accurate theoretical prediction of STE behavior, including localization and energy dynamics, remains challenging.
  • Existing methods often struggle to capture the complex interplay between excitons and lattice vibrations.

Purpose of the Study:

  • To introduce a novel computational framework for first-principles study of STEs.
  • To enable accurate calculation of exciton-phonon coupling and STE properties.
  • To provide a predictive tool for material design and experimental guidance.

Main Methods:

  • Utilizing the many-body Bethe-Salpeter equation combined with perturbation theory.
  • Calculating mode- and momentum-resolved exciton-phonon coupling matrix elements.
  • Solving for real-space electron/hole localization and lattice distortion.
  • Computing STE potential energy surfaces, formation energies, and Stokes shifts.

Main Results:

  • Demonstrated the framework's efficacy on chromium trihalides and Beryllium Oxide (BeO).
  • Successfully computed STE properties including formation energy and Stokes shift.
  • Predicted coherent phonon generation in BeO, highlighting the role of dark excitons.

Conclusions:

  • The proposed computational framework offers an effective approach to study STEs.
  • This method provides accurate predictions for material properties relevant to optoelectronics.
  • The findings encourage experimental investigations in photoluminescence and transient absorption studies.