Dataset Information

Ab Initio Time-Domain Study of Charge Relaxation and Recombination in N-Doped Cu₂O.

ABSTRACT: Cu₂O is a good photoelectric material with excellent performance, and its crystal structure, electronic structure, and optical properties have been extensively studied. To further illustrate the charge distribution and the carrier transport in this system, the e-h recombination dynamics was studied. It is found that N doping induced a shallower impurity band above the VBM, leading to significant charge localization around the impurity atom. NAMD simulation reveals that the N doping system possesses a longer e-h nonradiative recombination time scale. Therefore, we demonstrate that the formation of the impurity band and charge localization play an essential role in suppressing e-h recombination in N doping systems. This work is conducive for understanding the carrier transport mechanism in N-doped Cu₂O.

SUBMITTER: Su J

PROVIDER: S-EPMC10413821 | biostudies-literature | 2023 Aug

REPOSITORIES: biostudies-literature

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Ab Initio Time-Domain Study of Charge Relaxation and Recombination in N-Doped Cu<sub>2</sub>O.

Su Jianfeng J Zhang Jiao J Wang Yajie Y Wang Changqing C Niu Qiang Q Sun Ruirui R Zhang Weiying W

ACS omega 20230727 31

Cu<sub>2</sub>O is a good photoelectric material with excellent performance, and its crystal structure, electronic structure, and optical properties have been extensively studied. To further illustrate the charge distribution and the carrier transport in this system, the e-h recombination dynamics was studied. It is found that N doping induced a shallower impurity band above the VBM, leading to significant charge localization around the impurity atom. NAMD simulation reveals that the N doping sy ...[more]

PMID: 37576677

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Project description:Understanding nonradiative charge recombination mechanisms is a prerequisite for advancing perovskite solar cells. By performing time-domain density functional theory combined with nonadiabatic (NA) molecular dynamics simulations, we show that electron-hole recombination in perovskites strongly depends on the oxidation state of interstitial iodine and oxygen passivation. The simulations demonstrate that electron-hole recombination in CH3NH3PbI3 occurs within several nanoseconds, agreeing well with experiment. The negative interstitial iodine delays charge recombination by a factor of 1.3. The deceleration is attributed to the fact that interstitial iodine anion forms a chemical bond with its nearest lead atoms, eliminates the trap state, and decreases the NA electron-phonon coupling. The positive interstitial iodine attracts its neighbouring lattice iodine anions, resulting in the formation of an I-trimer and producing an electron trap. Electron trapping proceeds on a very fast timescale, tens of picoseconds, and captures the majority of free electrons available to directly recombine with free holes while inhibiting the recombination of free electrons and holes, delaying the recombination by a factor of 1.5. However, the positive interstitial iodine easily converts to a neutral iodine defect by capturing an electron, giving rise to a singly occupied state above the valence band maximum and acting as a hole trap. The photoexcitation valence band hole becomes trapped by the hole trap state very rapidly, followed by acceleration of recombination with the conduction band free electron by a factor of 1.6. Surprisingly, molecular oxygen interacting with interstitial iodine anion forms a stable IO3 -1 species, which inhibits ion migration, stabilizes perovskites, and suppresses the electron-hole recombination by a factor of 2.7. Our simulations reveal the microscopic effects of the oxidation state of interstitial iodine defects and oxygen passivation in perovskites, suggesting an effective way to improve perovskite photovoltaic and optoelectronic devices.

Dataset Information

Ab Initio Time-Domain Study of Charge Relaxation and Recombination in N-Doped Cu₂O.

Publications

Ab Initio Time-Domain Study of Charge Relaxation and Recombination in N-Doped Cu<sub>2</sub>O.

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Ab Initio Time-Domain Study of Charge Relaxation and Recombination in N-Doped Cu2O.

Publications

Ab Initio Time-Domain Study of Charge Relaxation and Recombination in N-Doped Cu<sub>2</sub>O.

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OmicsDI is part of the ELIXIR infrastructure

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Ab Initio Time-Domain Study of Charge Relaxation and Recombination in N-Doped Cu₂O.