Observation of higher order NMR larmor lines by SQUID in solids at low magnetic field

We describe an apparatus allowing the observation of the NMR static longitudinal component of nuclear magnetizationM _z by a SQUID at low magnetic fields and atT=4.2 K in Plexiglas, Teflon, and CaF₂. The higher order NMR Larmor lines at 2f ₀, 3f ₀, and 4f ₀, wheref ₀ is the Larmor frequency of the allowed NMR line, were measured. These lines correspond to a flip of two, three, and four spins, respectively, by one photon. The amplitudes of 2f ₀ and 3f ₀ lines and their field dependences show that the common assertion that the forbidden lines at 2f ₀ and 3f ₀ appear in the same order of perturbation theory and that their intensity decreases with static magnetic fieldB ₀ asB ₀ ^–2 is wrong. In fact, the third Larmor line 3f ₀ appears at higher order than the second Larmor line 2f ₀ and its intensity decreases asB ₀ ^–4 . This is also shown by a theoretical calculation of its intensity. For the first time the NMR SQUID technique allowed the detection of the 4f ₀ line, corresponding to the simultaneous flip of four spins by one photon.