Optical line narrowing by nuclear spin decoupling in Pr3+: LaF3

We have applied the technique of nuclear spin decoupling to the optical regime. In these experiments we selectively eliminated the role of ¹⁹F spin fluctuations as the dominant source of dephasing in the 5925A (¹D₂ / ³H₄)Pr³⁺ optical transition in 0.05% Pr³⁺: LaF₃ at 2K. The homogeneous optical linewidth (FWHM), measured by photon echoes, was reduced from 56 kHz to 6 kHz by on-resonance nutation of ¹⁹F in an external magnetic field of 375G. Further reduction of the linewidth to 4.1 kHz was observed by off-resonance irradiation of the fluorines such that their effective field in the rotating frame was at the ‘magic angle’ ($\text{cos}{}^{-1}\text{1}\text{3}$) with respect to the external field.