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Anomalies in G and 2D Raman modes of twisted bilayer graphene near the magic angle

Darshit Solanki1, Kenji Watanabe2, Takashi Taniguchi2, A. K. Sood1,*, and Anindya Das1,†

  • *Contact author: asood@iisc.ac.in
  • †Contact author: anindya@iisc.ac.in

Phys. Rev. B 112, 045412 – Published 11 July, 2025

DOI: https://doi.org/10.1103/9xym-n83q

Abstract

The role of twist angle (θt) in tailoring the physical properties of heterostructures is emerging as a new paradigm in two-dimensional materials. The influence of flat electronic bands near the magic angle (∼1.1∘) on the phononic properties of twisted bilayer graphene (t-BLG) is not well understood. In this work, we systematically investigate the G and 2D Raman modes of t-BLG samples with twist angles ranging from ∼0.3∘ to ∼3∘ using micro-Raman spectroscopy. A key finding of our work is the splitting of the G mode near the magic angle due to moiré potential induced phonon hybridization. The linewidth of the low-frequency component of the G mode (G−), as well as the main component of the 2D mode, exhibits enhanced broadening near the magic angle due to increased electron-phonon coupling, driven by the emergence of flat electronic bands. Additionally, temperature-dependent Raman measurements (6–300 K) of a magic-angle twisted bilayer graphene sample (θt∼1∘) reveal an almost tenfold increase in phonon anharmonicity induced temperature variation in both components of the split G mode, as compared to a Bernal-stacked bilayer graphene sample, further emphasizing the role of phonon hybridization in this system. These studies could be important for understanding the thermal properties of the twisted bilayer graphene systems.

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