Absolute frequency measurements on the 2S ! 3S transition of lithium-6,7

The frequencies of the 2S–3S two-photon transition for the stable lithium isotopes were measured by cavity-enhanced Doppler-free laser excitation that was controlled by a femtosecond frequency comb. The resulting values of 815 618 181.57(18) and 815 606 727.59(18) MHz, respectively, for 7Li and 6Li are in agreement with previous measurements but are more accurate by an order of magnitude. There is still a discrepancy of about 11.6 and 10.6 MHz from the latest theoretical values. This is comparable to the uncertainty in the theoretical calculations, while uncertainty in our experimental values is more than a hundred-fold smaller. More accurate theoretical calculation of the transition frequencies would allow extraction of the absolute charge radii for these stable isotopes, which in turn could improve nuclear charge radii values for the unstable lithium isotopes.