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Tuning perovskite recombination by hydrogen interstitial oxidation state.

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  • 1State Key Laboratory of Materials Low-Carbon Recycling, Beijing Key Lab of Microstructure and Properties of Advanced Materials, College of Materials Science and Engineering, School of Information Science and Technology Key Laboratory Optoelectronics Technology of Ministry of Education, Beijing University of Technology Beijing 100124 China chenxiaoqing@bjut.edu.cn zilong.zheng@bjut.edu.cn.

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The oxidation state of hydrogen interstitial defects significantly impacts perovskite recombination rates. Chlorine passivation neutralizes these defects, enhancing carrier lifetime for improved solar cell performance.

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Area of Science:

  • Materials Science
  • Solid-State Physics
  • Computational Chemistry

Background:

  • Nonradiative recombination is a major factor limiting perovskite solar cell efficiency.
  • Hydrogen interstitial defects are known to influence charge carrier dynamics in perovskites.

Purpose of the Study:

  • To investigate the role of hydrogen interstitial defect oxidation states on recombination dynamics in FAPbI3.
  • To elucidate the atomistic mechanisms behind defect-induced recombination.
  • To explore defect passivation strategies for enhancing perovskite performance.

Main Methods:

  • Combined time-dependent density functional theory (TD-DFT) with nonadiabatic molecular dynamics (NAMD) simulations.
  • Analyzed the impact of different hydrogen interstitial oxidation states (H0i, Hi+, Hi-) on recombination lifetimes.
  • Investigated the effect of chlorine passivation (Cl@H0i) on defect properties and carrier dynamics.

Main Results:

  • Recombination lifetime varied by three orders of magnitude depending on hydrogen interstitial oxidation state (0.1 ns for H0i, 44 ns for Hi+, 72 ns for Hi-).
  • The neutral hydrogen interstitial (H0i) introduced a deep-level defect state, significantly increasing nonadiabatic coupling (0.35 meV to 1.56 meV).
  • Chlorine passivation (Cl@H0i) neutralized H0i defects, reduced nonadiabatic coupling to 0.30 meV, and extended carrier lifetime to 87 ns.

Conclusions:

  • The oxidation state of hydrogen interstitials critically governs nonradiative recombination in FAPbI3.
  • Chlorine passivation is an effective strategy to mitigate recombination losses caused by H0i defects.
  • Atomistic insights into defect dynamics are crucial for designing high-performance perovskite materials.