Theory of Dipolar Lineshifts in Free-Radical Crystals

Abstract
The spin absorption spectrum of a free‐radical crystal containing several inequivalent radicals per unit cell is obtained in the high temperature and the large magnetic field limit. A direct, approximate solution of the total (Zeeman+dipolar) Hamiltonian is used rather than a moment calculation. The spectrum is found for arbitrary ωd / Δω where ωd is the dipolar coupling between radicals whose Larmor frequencies differ by Δω . For both small and large ωd / Δω , the dipolar lineshifts agree with results based on the moment method.