Nonradiative Dynamics Induced by Vacancies in Wide-Gap III-Nitrides: Ab Initio Time-Domain Analysis

Yuxin Yang; Zhiming Shi; Shoufeng Zhang; Xiaobao Ma; Jiangxiao Bai; Dashuo Fan; Hang Zang; Xiaojuan Sun; Dabing Li

doi:10.1021/acs.jpclett.3c01515

Nonradiative Dynamics Induced by Vacancies in Wide-Gap III-Nitrides: Ab Initio Time-Domain Analysis

J Phys Chem Lett. 2023 Jul 27;14(29):6719-6725. doi: 10.1021/acs.jpclett.3c01515. Epub 2023 Jul 20.

Authors

Yuxin Yang^{1

2}, Zhiming Shi¹, Shoufeng Zhang³, Xiaobao Ma^{1

2}, Jiangxiao Bai^{1

2}, Dashuo Fan^{1

2}, Hang Zang¹, Xiaojuan Sun¹, Dabing Li^{1

2}

Affiliations

¹ State Key Laboratory of Luminescence and Applications, Changchun Institute of Optics, Fine Mechanics and Physics, Chinese Academy of Sciences, Changchun 130033, China.
² Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China.
³ Department of Electronic Engineering, Guangxi University of Science and Technology, Liuzhou 545006, China.

PMID: 37470335
DOI: 10.1021/acs.jpclett.3c01515

Abstract

Insightful understanding of defect properties and prevention of defect damage are among the biggest issues in the development of photoelectronic devices based on wide-gap III-nitride semiconductors. Here, we have investigated the vacancy-induced carrier nonradiative dynamics in wide-gap III-nitrides (GaN, AlN, and Al_xGa_1-xN) by ab initio molecular dynamics and nonadiabatic (NA) quantum dynamics simulations since the considerable defect density in epitaxy samples. E-h recombination is hardly affected by V_cation, which created shallow states near the VBM. Our findings demonstrate that V_N in AlN creates defect-assisted nonradiative recombination centers and shortens the recombination time (τ) as in the Shockley-Read-Hall (SRH) model. In GaN, V_N improves the NA coupling between the CBM and the VBM. Additionally, increasing x in the Al_xGa_1-xN alloys accelerates nonradiative recombination, which may be an important issue in further improving the IQE of high Al-content Al_xGa_1-xN alloys. These findings have significant implications for the improvement of wide-gap III-nitrides-based photoelectronic devices.