Properties of doped and natural impurities in Lithium Niobate single crystals are studied using the Whispering Gallery Mode method at low temperatures as a function of magnetic field. The study reveals considerable coupling of microwave photon modes to the Fe spin ensemble in iron-doped and non-doped crystals. The structure of the Fe impurities demonstrate Zero Field Splittings of and GHz, significant asymmetry of the Zeeman lines and additional lines with anomalous -factors of and . Also, interactions between different transitions of the Fe ion is observed. An additional ion impurity ensemble with a splitting of about GHz is shown to couple to the dominating Fe spins and the effect on -factors of microwave photon modes due to the Fe ion ensemble is also demonstrated. Measurements down to less than one photon level are made with a loss tangent of order determined.

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