Abstract
Solid solutions grown from the ternary system NH4Cl–MnCl2–H2O with Mn2+ concentrations up to 8% by weight show a change of structure from cubic to tetragonal in the vicinity of 4% Mn2+. Electron spin resonance at X band shows an extraordinarily complex spectrum for the series, and a change in hyperfine structure intensity with change of structure. Previous workers have shown by x‐ray diffraction that the tetragonal phase, which occurs at high concentrations of manganese, is due to ordered arrangement of NH4Cl double cells in which the manganese ion is interstitial. It is deduced from the electron spin resonance results that the double cell structure also holds at low concentrations, the bcc phase shown by x‐ray diffraction being due to a lack of order among such double cells. A Q‐band spectrum yields an exceptionally large axial parameter D=0.150 cm—1, and a small cubic parameter a=2.8×10—4 cm—1 in the spin Hamiltonian.

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