Polarized double-resonance Raman spectra of black phosphorus

doi:10.1016/j.jmst.2025.09.079

Abstract

Abstract: Black phosphorus (BP) exhibits a broad spectrum of double-resonance Raman (DRR) peaks from 500 to 1000 cm^-1, which provide valuable information on symmetry and phonon. However, previous assignments of phonons associated with the DRR peaks have not yielded consistent results because most optical phonon branches are densely located in the small frequency region of 350-500 cm^-1. In this study, we calculate the DRR spectra using a first-principles approach that accounts for both the electron-photon and electron-phonon matrix elements. Based on the calculated Raman tensor, we present polarized Raman spectra of each DRR peak, which reproduce the experimental polarized Raman spectra. We find that most of the DRR peaks originate from a specific phonon wavevector in the Brillouin zone. A_g-like linearly and circularly polarized DRR spectra are observed and calculated, which can be ascribed to the phase difference between diagonal elements of the Raman tensor. Our assignments, combined with group-theory analysis, have provided a grounded origin of the DRR peaks of BP.

Key words: Polarized Raman spectra, Double-resonance Raman modes, Black phosphorus, First-principles calculation

Ye Zhang, Renhui Liu, Jianqi Huang, Xingzhi Wang, Wenlai Mu, Nguyen Tuan Hung, Riichiro Saito, Huaihong Guo, Teng Yang, Zhidong Zhang. Polarized double-resonance Raman spectra of black phosphorus[J]. J. Mater. Sci. Technol., 2026, 262: 244-251.

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