Li Ning, Bao Tianqi, Zhao Yang, Zhang Fan, Zhang Junfeng, Jiang Xue, Cherenda Nikolai, Gao Weiwei, Zhao Jijun, Su Yan
Key Laboratory of Materials Modification by Laser, Ion and Electron Beams (Dalian University of Technology), Ministry of Education, Dalian, 116024, China.
College of Physics and Electronic Engineering, Hainan Normal University, Haikou, 571158, China.
Phys Chem Chem Phys. 2025 Jun 18;27(24):12848-12857. doi: 10.1039/d5cp01203a.
Two-dimensional (2D) fullerene monolayer materials exhibit a wide range of unique properties, including pronounced excitonic effects with significant potential for optoelectronic applications. Here, we perform a comprehensive investigation of the quasiparticle (QP) and excitonic properties of the C-2D monolayer using density functional theory (DFT) and many-body perturbation theory (MBPT) based on the GW approximation and Bethe-Salpeter equation (GW-BSE). Our calculations reveal substantial excitonic effects in the C-2D monolayer, with an impressive exciton binding energy of 1.58 eV, a notable breakthrough compared to the 0.8 eV reported for the C monolayer. Embedding magnesium (Mg) into the C-2D monolayer induces polarization effects and enhances dielectric screening, driving a transition of the lowest-energy excitons from the Frenkel to the Wannier type. This transition is accompanied by significant changes in both the intensity and range of optical absorption. These findings reveal the tunability of fullerene materials through embedding, offering insights for the development of next-generation optoelectronic devices.
二维（2D）富勒烯单层材料展现出广泛的独特性质，包括显著的激子效应，在光电子应用方面具有巨大潜力。在此，我们基于GW近似和贝叶斯 - 萨尔皮特方程（GW - BSE），使用密度泛函理论（DFT）和多体微扰理论（MBPT），对C - 2D单层的准粒子（QP）和激子性质进行了全面研究。我们的计算揭示了C - 2D单层中存在显著的激子效应，其激子结合能高达1.58 eV，与报道的C单层的0.8 eV相比，这是一个显著的突破。将镁（Mg）嵌入C - 2D单层会引发极化效应并增强介电屏蔽，促使最低能量激子从弗伦克尔型向万尼尔型转变。这种转变伴随着光吸收强度和范围的显著变化。这些发现揭示了通过嵌入来调控富勒烯材料的可能性，为下一代光电器件的开发提供了思路。
