Citation: Hongqin Chu, Liyang Li, Fan Yang, Shujuan Li, Jiayao Wang, Shulai Lei, Jinbo Sun, Ke Xu, Xinyue Xiong, Zhenpeng Hu. Characterization of intrinsic defects and their effects on carrier lifetime in CdTeSe: First principles and non-adiabatic molecular dynamics simulations[J]. Chinese Chemical Letters, ;2026, 37(9): 111490. doi: 10.1016/j.cclet.2025.111490 shu

Characterization of intrinsic defects and their effects on carrier lifetime in CdTeSe: First principles and non-adiabatic molecular dynamics simulations

Hongqin Chu ^a ,
Liyang Li ^a ,
Fan Yang ^a ,
Shujuan Li ^b ,
Jiayao Wang ^b ,
Shulai Lei ^{b, c, *,} ,
Jinbo Sun ^b ,
Ke Xu ^b ,
Xinyue Xiong ^b ,
Zhenpeng Hu ^{a, *,}

a.
School of Physics, Nankai University, Tianjin 300071, China
b.
School of Physics and Electronic Engineering, Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices, Hubei University of Arts and Science, Xiangyang 441053, China
c.
Hubei Longzhong Laboratory, Xiangyang 441053, China

sllei@hbuas.edu.cn

zphu@nankai.edu.cn

Received Date: 14 March 2025
Revised Date: 16 June 2025
Accepted Date: 18 June 2025
Available Online: 20 June 2025

Figures(7)

With the rapid advancement of solar cell and radiation detector technology, understanding and controlling intrinsic defects in semiconductor materials is crucial for improving photovoltaic device performance. This study employs density functional theory (DFT) and non-adiabatic molecular dynamics (NAMD) methods to investigate the ground-state properties of intrinsic defects in CdTeSe (CTS) material and their impact on carrier dynamics. The results demonstrate that defect formation is strongly influenced by the chemical environment: acceptor defects are favored in Te-rich conditions, donor defects are promoted in Cd-rich conditions, while Se substitution at the Te site (Se_Te) and Te substitution at the Se site (Te_Se) defects are readily formed under various conditions due to their low formation energies. Carrier lifetime is significantly affected by various defects, as shown by their modulation of electron-phonon coupling interactions in electron-hole recombination dynamics. Se_Cd and Te_Cd defects are characterized by strong coupling between local vibrational modes and band-edge states, which enhances non-adiabatic coupling (NAC) strength and reduces recombination times to 9.44 ns and 30.95 ns, respectively. In contrast, Se_Te and Te_Se defects suppress the NAC by markedly reducing coupling, thereby extending the recombination times to 198.04 ns and 239.5 ns. Fourier transform analysis further indicates that the low-frequency phonon modes associated with Se_Te and Te_Se defects enhance carrier dynamics by optimizing phonon-assisted processes. Finally, it is found that variations in carrier concentration have a significant impact on carrier recombination, especially at high non-equilibrium carrier concentrations, which notably shorten the carrier lifetime. This study offers a theoretical framework for the performance optimization and defect engineering of CTS material in high-efficiency solar cell applications.
- First-principles calculation,
- Intrinsic defects,
- Non-adiabatic molecular dynamics,
- Electron-hole recombination,
- Non-adiabatic coupling
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