Polarization of photoluminescence by optically driven orbital reconstruction in magnetically ordered CrCl3

In this paper, we show that photoluminescence from CrCl3 bulk crystal exhibits a preferential polarization direction when films are magnetically ordered or strained. We verify the magnetization as responsible for the polarization by measuring the signal as a function of the temperature in Voigt configuration while applying the in-plane magnetic field. We show that phonon coupling contributing to vibronic transitions depolarizes the signal compared with zero phonon lines. We explain the data using DFT calculations, which reveal a magnetization-selective occupation of the low energy d-orbital triplet state of Cr3+ upon photon absorption. In addition, the calculations find that the excitation of one electron results in the excited state acquiring out-of-plane components of spin and very large orbital magnetic moments, in addition to a lattice deformation.