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Sulfur Passivation Engineering of Carbon Defects in N-Surface GaN - Suppressing Nonadiabatic Carrier Recombination Via Self-Compensated SN-CN Complexes

MetadataDetails
Publication Date2025-06-06
JournalThe Journal of Physical Chemistry Letters
AuthorsFuwei Kang, Shuai-Shuai Liu, Jinfeng Kang, Ze Peng, Shaoqiang Guo
InstitutionsInner Mongolia University

In gallium nitride (GaN), the carbon-on-nitrogen substitutional defect (C<sub>N</sub>) has been extensively investigated as a prototypical deep acceptor center, particularly for its well-characterized yellow luminescence associated with the (-/0) transition. However, the carrier dynamics involving its secondary (0/+) transition remains poorly understood. Combining first-principles calculations and nonadiabatic molecular dynamics simulations, we systematically investigate the nonradiative carrier capture processes mediated by the C<sub>N</sub> defects on nitrogen-terminated GaN surfaces, along with their sulfur-based passivation mechanisms. Our results demonstrate that the neutral C<sub>N</sub> defect serves as a critical nonradiative recombination center, exhibiting an ultrafast hole capture rate (Ļ„ ā‰ˆ 10<sup>-12</sup> s). Notably, sulfur atoms can migrate with a low energy barrier (0.64 eV) to occupy adjacent nitrogen vacancies on the N surface, forming S<sub>N</sub>-C<sub>N</sub> complex defects through a self-compensation mechanism. This structural modification induces a significant charge redistribution, shifting the defect level from deep within the bandgap to near the valence band maximum. Such electronic structure modulation effectively suppresses nonadiabatic transitions between defect states and the valence band. This work provides the first atomistic visualization of sulfur passivation mechanisms for C<sub>N</sub> defects in GaN, establishing a quantitative relationship between defect configuration engineering and carrier recombination dynamics.