Giant Huang-Rhys Factor for Electron Capture by the Iodine Interstitial in Perovskite Solar Cells

TL;DR

This paper investigates the electron trapping mechanism of iodine interstitial defects in perovskite solar cells, revealing a giant Huang-Rhys factor indicating strong electron-phonon coupling, which impacts defect tolerance.

Contribution

It provides a quantum mechanical analysis showing fast, irreversible electron capture by iodine interstitials with an exceptionally high Huang-Rhys factor, highlighting the role of phonon modes in defect processes.

Findings

Effective Huang-Rhys factor exceeds 300

Electron capture coefficient is 10^{-10} cm^3 s^{-1}

Suppression of octahedral rotations may improve defect tolerance

Abstract

Improvement in the optoelectronic performance of halide perovskite semiconductors requires the identification and suppression of non-radiative carrier trapping processes. The iodine interstitial has been established as a deep level defect, and implicated as an active recombination centre. We analyse the quantum mechanics of carrier trapping. Fast and irreversible electron capture by the neutral iodine interstitial is found. The effective Huang-Rhys factor exceeds 300, indicative of the strong electron-phonon coupling that is possible in soft semiconductors. The accepting phonon mode has a frequency of 53 cm$^{-1}$ and has an associated electron capture coefficient of 10$^{-10}$cm$^3$s$^{-1}$. The inverse participation ratio is used to quantify the localisation of phonon modes associated with the transition. We infer that suppression of octahedral rotations is an important factor to enhance defect tolerance.