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中国物理学会期刊

石墨烯狄拉克等离激元调控的第一性原理研究

CSTR: 32037.14.aps.74.20250913

First-principles study of modulation of graphene Dirac plasmons

CSTR: 32037.14.aps.74.20250913
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  • 石墨烯等离激元在红外-太赫兹波段具有高度局域化和动态可调性, 但其精准调控机制仍需深入探索. 本文基于国产第一性原理计算软件ABACUS, 采用线性响应含时密度泛函理论方法, 结合截断库仑势消除层间耦合效应, 系统研究了石墨烯狄拉克等离激元的三类调控机制. 研究结果表明, 无论采用何种调控手段, 石墨烯狄拉克等离激元的色散关系均呈现出典型的双区域特征: 在长波区域, 其色散关系遵循\sqrtq的形式; 在短波区域, 则逐渐过渡为准线性行为. 此外, 随着载流子浓度的增加, 等离激元的激发能量呈现系统性增强, 并遵循\omega \propto n^1/4的标度律; 施加双轴应变时, 等离激元激发能量随晶格常数的增大而线性降低; 引入六方氮化硼(hBN)作为基底时, 对原始结果影响较小, 仅导致整体能量发生轻微红移. 进一步地, 深入揭示了上述三种调控机制的物理起源. 这些结果为基于石墨烯/hBN异质结构的高性能动态光电器件设计提供了坚实的理论支撑.

     

    Graphene Dirac plasmons, which are collective oscillations of charge carriers behaving as massless Dirac fermions, have emerged as a transformative platform for nanophotonics due to their exceptional capability for deep subwavelength light confinement in the infrared-to-terahertz spectral region and their unique dynamic tunability. Although external controls such as electrostatic doping, mechanical strain, and substrate engineering are empirically known to be able to modulate plasmonic responses, a comprehensive and quantitative theoretical framework from first principles is essential to reveal the distinct efficiency and fundamental mechanisms of each tuning strategy. To address this issue, we conduct a systematic first-principles study of three primary modulation pathways—carrier density, biaxial strain, and substrate integration—by using linear-response time-dependent density functional theory in the random-phase approximation (LR-TDDFT-RPA) as implemented in the computational code ABACUS. A truncated Coulomb potential is adopted in order to accurately model the isolated two-dimensional system, while structural and electronic properties are computed using the PBE functional with SG15 norm-conserving pseudopotentials and van der Waals corrections for heterostructures. Our research results indicate that modulating carrier concentration can cause the plasmon dispersion to follow the characteristic \omega \propto n^1/4 scaling law, thereby tuning within a wide range from 0.45 eV to 1.38 eV at the Landau damping threshold—a 207% change for the carrier density varying from 0.005 to 0.1 electrons/unit cell, although efficiency decreases at higher concentrations due to the sublinear nature of the scaling law. Biaxial strain linearly changes the plasmon energy by modifying the Fermi velocity (v_\mathrmF) near the Dirac point, yielding a 30.4% tuning range (0.78–1.12 eV) under \pm 10\text% strain. Introducing an hBN substrate induces a small band gap (~43 meV) and causes a general redshift in plasmon energy due to band renormalization, while remarkably preserving the linear strain-tuning capability in a 30.1\text% energy range (0.72–1.03 eV) in the heterostructure, demonstrating robust compatibility between strain engineering and substrate integration. These results quantitatively elucidate the different physical mechanisms—Fermi level shifting, Fermi velocity modification, and substrate-induced symmetry breaking and hybridization—underpinning each strategy, thereby providing a solid theoretical foundation for designing dynamically tunable optoelectronic devices based on graphene and its van der Waals heterostructures.

     

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