Resonant Raman scattering of few layers CrBr3

Abstract

We investigate the vibrational and magnetic properties of thin layers of chromium tribromide (CrBr₃) with a thickness ranging from three to twenty layers (3–20 L) revealed by the Raman scattering (RS) technique. Systematic dependence of the RS process efficiency on the energy of the laser excitation is explored for four different excitation energies: 1.96 eV, 2.21 eV, 2.41 eV, and 3.06 eV. Our characterization demonstrates that for 12 L CrBr₃, 3.06 eV excitation could be considered resonant with interband electronic transitions due to the enhanced intensity of the Raman-active scattering resonances and the qualitative change in the Raman spectra. Polarization-resolved RS measurements for 12 L CrBr₃ and first-principles calculations allow us to identify five observable phonon modes characterized by distinct symmetries, classified as the A$_{\text{g}}^{}$ and E$_{\text{g}}^{}$ modes. The evolution of phonon modes with temperature for a 16 L CrBr₃ encapsulated in hexagonal boron nitride flakes demonstrates alterations of phonon energies and/or linewidths of resonances indicative of a transition between the paramagnetic and ferromagnetic state at Curie temperature ($T_{\text{C}}\approx 50$ K). The exploration of the effects of thickness on the phonon energies demonstrated small variations pronounces exclusively for the thinnest layers in the vicinity of 3–5 L. We propose that this observation can be due to the strong localization in the real space of interband electronic excitations, limiting the effects of confinement for resonantly excited Raman modes to atomically thin layers.