Undoped and Cr3+-doped KTiOPO4 (KTP) systems were studied by means of P-31
nuclear-magnetic-resonance measurements. The high-resolution P-31 isotropic
-chemical-shift measurements were employed as a new probe in addition to th
e laboratory and rotating frame spin-lattice relaxation-time measurements.
As a result, two phase-transitional behaviors ascribed to the changes in th
e dominant charge carriers were well characterized. Furthermore, it was fou
nd that the Cr3+ doping of the KTP system results in significant shifts in
the transition temperatures.