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    Probing the charge density wave transition in semimetallic 1T−TiSe2−δ by temperature-dependent Raman spectroscopy

    Huynh Phuong Anh1, Nguyen Van Thanh1, Kalingarayanpalayam Matheswaran Arun Kumar1, Paphawee Paukatong1, Xiang-Lin Huang2, Guo-Jiun Shu3, Riichiro Saito1,4, Nguyen Tuan Hung5,*,†, and Hsiang-Lin Liu1,‡

    • *Present address: Frontier Research Institute for Interdisciplinary Sciences, Tohoku University, Sendai 980-8578, Japan.
    • †Contact author: nguyen.tuan.hung.e4@tohoku.ac.jp
    • ‡Contact author: hliu@ntnu.edu.tw

    Phys. Rev. Materials 10, 104001 – Published 1 October, 2026

    DOI: https://doi.org/10.1103/2qjd-mc12

    Abstract

    We present temperature-dependent Raman spectra of semimetallic 1T−TiSe2−δ single crystals from 10 to 300 K using a 532 nm excitation laser, probing the charge density wave (CDW) transition at 170 K. The first-order Eg and A1g phonon modes exhibit asymmetric lineshapes above 170 K, which are described by the Breit–Wigner–Fano (BWF) function and become Lorentzian below 134 K. The Bose–Einstein anharmonic model reveals anomalies in the Eg phonon peak position near the CDW transition, whereas the A1g mode follows conventional anharmonic behavior. Moreover, we observe six low-frequency Raman peaks between 84 and 123cm−1, as well as one Raman peak at 295cm−1. By comparing these features with the one-phonon and two-phonon density of states obtained from the first-principles calculations, we assign the low-frequency modes to defect-induced double-resonance Raman peaks and the 295cm−1 mode to a two-phonon double-resonance Raman peak. The first-principles calculations also indicate phonon softening near the M and L points in the Brillouin zone, suggesting the lattice instability associated with the CDW transition. Our results provide Raman fingerprints of the CDW transition and highlight the role of electron–phonon interactions in semimetallic 1T−TiSe2−δ.

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