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PreprintCC BYChemRxiv

Strain-Tunable Electron–Phonon Coupling Collapse in Oxide Perovskites: A First-Principles Route to Suppressed Hot-Carrier Thermalization

  • Naveen Kumar1,2
  • Anirban Mondal1,2
  1. 1Department of Chemistry
  2. 2Indian Institute of Technology Gandhinagar
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Abstract

Hot-carrier thermalization constitutes the dominant energy loss channel in perovskite photovoltaics, yet the role of epitaxial strain in controlling this process remains largely unexplored from first principles. We present a systematic firstprinciples study of strain-dependent hot-carrier cooling rates in six inorganic perovskiteshalides CsSnI3, CsSnBr3, and CsCaCl3, and oxides BaSnO3, BaZrO3, and KTaO3across a ±2% biaxial strain window. Eliashberg spectral functions ω2F (ε) are computed via density functional perturbation theory and Wannier interpolation, from which hot-carrier energy loss rates →dE/dt↑ are evaluated through the Fröhlich– EPW formalism for carrier temperatures up to 5000 K. Applying +1% tensile strain to BaZrO3 collapses the dominant-mode electron–phonon coupling constant from ϑ = 1.31 to ϑ = 0.011, suppressing the hot-carrier cooling rate by more than 90% relative to the least favorable strain condition and yielding a thermalization time ϖtherm = 1,585 fs and a hot-carrier figure of merit FOMHC = 1,348 fs, surpassing all halide configurations by more than an order of magnitude. Landau polynomial fitting of ε2 min (ϱ) confirms that no strain-induced structural phase transition occurs within ±2% for any compound, establishing a safe phonon engineering window. Orbital-projected densities of states reveal two mechanistically distinct coupling classes: gap-closure-driven coupling in BaSnO3 and CsCaCl3 [Spearman correlation ς(Eg, ϑ) ↓ ↔0.70] and purely phonon-mode-softening-driven coupling in BaZrO3 and KTaO3 (ς ↗ +0.72), the latter being invisible to band structure analysis alone.

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Cite

BibTeXRIS
BibTeX
@misc{kumar2026straintunable,
  title = {{Strain-Tunable Electron–Phonon Coupling Collapse in Oxide Perovskites: A First-Principles Route to Suppressed Hot-Carrier Thermalization}},
  author = {Naveen Kumar and Anirban Mondal},
  howpublished = {ChemRxiv},
  year = {2026},
  month = oct,
  doi = {10.26434/chemrxiv.15010951/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15010951/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Strain-Tunable Electron–Phonon Coupling Collapse in Oxide Perovskites: A First-Principles Route to Suppressed Hot-Carrier Thermalization
AU  - Naveen Kumar
AU  - Anirban Mondal
PY  - 2026
DA  - 2026/10/23
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15010951/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15010951/v1
AB  - Hot-carrier thermalization constitutes the dominant energy loss channel in perovskite photovoltaics, yet the role of epitaxial strain in controlling this process remains largely unexplored from first principles. We present a systematic firstprinciples study of strain-dependent hot-carrier cooling rates in six inorganic perovskiteshalides CsSnI3, CsSnBr3, and CsCaCl3, and oxides BaSnO3, BaZrO3, and KTaO3across a ±2% biaxial strain window. Eliashberg spectral functions ω2F (ε) are computed via density functional perturbation theory and Wannier interpolation, from which hot-carrier energy loss rates →dE/dt↑ are evaluated through the Fröhlich– EPW formalism for carrier temperatures up to 5000 K. Applying +1% tensile strain to BaZrO3 collapses the dominant-mode electron–phonon coupling constant from ϑ = 1.31 to ϑ = 0.011, suppressing the hot-carrier cooling rate by more than 90% relative to the least favorable strain condition and yielding a thermalization time ϖtherm = 1,585 fs and a hot-carrier figure of merit FOMHC = 1,348 fs, surpassing all halide configurations by more than an order of magnitude. Landau polynomial fitting of ε2 min (ϱ) confirms that no strain-induced structural phase transition occurs within ±2% for any compound, establishing a safe phonon engineering window. Orbital-projected densities of states reveal two mechanistically distinct coupling classes: gap-closure-driven coupling in BaSnO3 and CsCaCl3 [Spearman correlation ς(Eg, ϑ) ↓ ↔0.70] and purely phonon-mode-softening-driven coupling in BaZrO3 and KTaO3 (ς ↗ +0.72), the latter being invisible to band structure analysis alone.
ER  -