Ultra-slow electron spin-lattice relaxation in a low magnetic field enables massive optical spin polarization in the 4A2 ground state of Cr3+ in ruby* *This paper is dedicated to my late friend and mentor Dr Alex Szabo, the originator of transient spectral hole-burning and fluorescence line narrowing in the solid state, whose knowledge of the spectroscopy of ruby is unsurpassed.

Abstract

Ruby (α-Al2O3 doped with Cr3+) has been an archetypal material in the development of optical spectroscopy of the solid state for the last 150 years and was the first material that was demonstrated to lase. Notwithstanding the vast literature on ruby, one effect was somehow missed: in a magnetic field B ∥c ∼ 235 mT, the spin-lattice relaxation time T 1 for the |+3/2⟩ level in the 4A2 ground state is massively lengthened to ∼12 s at 1.4 K as demonstrated in this study. This very long relaxation time enables optical pumping of the |+3/2⟩ level via the R 1(±1/2) lines and a considerable +3/2 spin polarization of ∼95% is readily achieved. The observed magnetic field dependence can be quantitatively described using the one-phonon relaxation process.