A new method is given for obtaining low temperatures in paramagnetic crystals in the presence of a large magnetic field by utilizing anisotropic hyper fine structure coupling. The method consists essentially of reduction of h.f.s. splittings by rotation of a magnetic field under adiabatic conditions. A discussion of the requirements on the properties of the usable paramagnetic ions is given. The usefulness of the method was demonstrated with crystals of CoCs 2(SO 4) 2.6D 2O in which 54Mn was incorporated in order to serve as a thermometer. The ratio between initial and final temperature was 4 to 5, resulting in a lowest temperature of 0.006°K, which could be maintained for at least one hour. In high magnetic fields establishment of thermal equilibrium between the 54Mn and stable 59Co nuclei could not be obtained, indicating extremely long relaxation times in the interaction of nuclear spins of unlike paramagnetic ions. However, for medium field strengths relaxation time measurements could be carried out as a function of field strength, of the direction of the field and of the temperature. It was found that the relaxation time was very strongly dependent on the field strength when the field was in a fixed direction, but was approximately constant for a fixed value of the sum of electronic Zeeman splittings of Mn and Co-ions, when varying both the direction and magnitude of the field. Gamma ray intensity measurements of 54Mn at a very high degree of nuclear polarization (> 97%) resulted in the establishment of an upper limit to the possible disturbance of the 54Mn nuclear polarization due to K-capture or to its after-effects. The rotational cooling procedure was further investigated by measurements of anisotropies of 60Co gamma radiations; the main features of the experimental results, obtained for various field directions, were in agreement with theoretical predictions. However, at the lowest temperatures significant deviations were found. 137Cs-nuclei were oriented by electric h.f.s. coupling; peculiar relaxation phenomena were observed which led to the conclusion that 137mBa has a negative sign for its nuclear electric quadrupole moment. The magnitude of the crystalline electric field gradient was found to be at least a factor of 30 larger than that found by Kiddle et Proctor by means of nuclear quadrupole resonance at room temperature. The relaxation time for establishment of thermal equilibrium between Cs and Co-nuclei was found to be a few orders of magnitude shorter than that between Co- and Mn-nuclear spins. Negative results concerning attempts to orient 134Cs, 86Rb are reported.
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