Carbon ( IF 10.5 ) Pub Date : 2021-09-18 , DOI: 10.1016/j.carbon.2021.09.017 X. Chen 1, 2 , M.-L. Lin 1 , X. Cong 1, 2 , Y.-C. Leng 1, 2 , X. Zhang 1 , P.-H. Tan 1, 2
The temperature-dependent (T-dependent) linewidth (ΓG) and frequency shift (ΔωG) of the G mode provide valuable information on the phonon anharmonicity of graphene-based materials. In contrast to the negligible contribution from electron-phonon coupling (EPC) to the linewidth of a Raman mode in semiconductors, ΓG in pristine graphene is dominated by EPC contribution at room temperature due to its semimetallic characteristics. This leads to difficulty in resolving intrinsic contribution from phonon anharmonicity to ΓG. Here, we probed the intrinsic phonon anharmonicity of heavily-doped graphene by T-dependent Raman spectra based on FeCl3-based stage-1 graphite intercalation compound (GIC), in which the EPC contribution is negligible due to the large Fermi level (EF) shift. The ΔωG and ΓG exhibit a nonlinear decrease and noticeable broadening with increasing temperature, respectively, which are both dominated by phonon anharmonicity processes. The contribution of phonon anharmonicity to ΓG of heavily-doped graphene decreases as the EF approaches to the Dirac point. However, the T dependence of ΔωG is almost independent on EF and qualitatively agrees with the theoretical result of pristine graphene. These results provide a deeper understanding of the role of phonon anharmonicity on the Raman spectra of heavily doped graphene.
中文翻译:
拉曼光谱探测重掺杂石墨烯中的固有声子非谐性
G 模式的温度相关(T相关)线宽 (Γ G ) 和频移 (Δ ω G ) 提供了有关石墨烯基材料声子非谐性的宝贵信息。与电子-声子耦合 (EPC) 对半导体中拉曼模式线宽的贡献可忽略不计相比,由于其半金属特性,原始石墨烯中的Γ G在室温下由 EPC 贡献主导。这导致难以解决声子非谐性对Γ G 的内在贡献。在这里,我们通过基于 FeCl 3 的T依赖拉曼光谱探测了重掺杂石墨烯的固有声子非谐性基于阶段1石墨层间化合物(GIC),其中,所述EPC贡献是可忽略的,由于大费米能级(Ë ˚F)移位。Δ ω G和Γ G分别随着温度的升高表现出非线性减小和显着的展宽,这两者都由声子非谐过程控制。随着E F接近狄拉克点,声子非谐性对重掺杂石墨烯的Γ G的贡献降低。然而,Δω G的T依赖性几乎与E F无关并定性地与原始石墨烯的理论结果一致。这些结果提供了对声子非谐性对重掺杂石墨烯拉曼光谱的作用的更深入理解。