Circularly
polarized light carries light spin angular momentum,
which may lead helicity-resolved Raman scattering to be sensitive
to the electronic spin configuration in magnetic materials. Here,
we demonstrate that all Raman modes in the 2D ferromagnet VI3 show different scattering intensities to left and right circularly
polarized light at low temperatures, which gives direct evidence of
the time-reversal symmetry breaking. By measuring the circular polarization
of the dominant Raman mode with respect to the temperature and magnetic
field, the ferromagnetic (FM) phase transition and hysteresis behavior
can be clearly resolved. Besides the lattice excitations, quasielastic
scattering is detected in the paramagnetic phase, and it gradually
evolves into the acoustic magnon mode at 18.5 cm–1 in the FM state, which gives the spin wave gap that results from
large magnetic anisotropy. Our findings demonstrate that helicity-resolved
Raman spectroscopy is an effective tool to directly probe the ferromagnetism
in 2D magnets.