Abstract
On-site excitations of the Gd3+ ion in lanthanum ethylsulphate have recently been shown to produce a spin-correlated crystal field which results in zero-field splittings of the same sign as those from experiment but, approximately, two time too large. In this paper intersite one-electron excitations have been invoked to produce additional contributions to the spin-correlated crystal field, which compensate the zero-field splittings from on-site contributions alone to produced zero-field splittings in good agreement with experiment. The resultant zero-field splittings are thus a delicate balance between a number of on-site mechanisms, i.e. a contribution from the paramagnetic Gd3+ ion itself and one from the host in which it is embedded.
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