D. E. MacLaughlin, O. O. Bernal, Lei Shu, Jun Ishikawa, Yosuke Matsumoto, J. -J. Wen, M. Mourigal, C. Stock, G. Ehlers, C. L. Broholm, Yo Machida, Kenta Kimura, Satoru Nakatsuji, Yasuyuki Shimura, Toshiro Sakakibara
PHYSICAL REVIEW B, 92(5) 054432, Aug, 2015 Peer-reviewed
Specific heat, elastic neutron scattering, and muon spin rotation (mu SR) experiments have been carried out on a well-characterized sample of "stuffed" (Pr-rich) Pr2+xIr2-xO7-delta. Elastic neutron scattering shows the onset of long-range spin-ice "2-in/2-out" magnetic order at T-M = 0.93 K, with an ordered moment of 1.7(1)mu(B)/Pr ion at low temperatures. Approximate lower bounds on the correlation length and correlation time in the ordered state are 170 angstrom and 0.7 ns, respectively. mu SR experiments yield an upper bound 2.6(7) mT on the local field B-loc(4f) at the muon site, which is nearly two orders of magnitude smaller than the expected dipolar field for long-range spin-ice ordering of 1.7 mu(B) moments (120-270 mT, depending on muon site). This shortfall is due in part to splitting of the non-Kramers crystal-field ground-state doublets of near-neighbor Pr3+ ions by the mu(+)-induced lattice distortion. For this to be the only effect, however, similar to 160 Pr moments out to a distance of similar to 14 angstrom must be suppressed. An alternative scenario, which is consistent with the observed reduced nuclear hyperfine Schottky anomaly in the specific heat, invokes slow correlated Pr-moment fluctuations in the ordered state that average B-loc(4f) on the mu SR time scale (similar to 10(-7) s), but are static on the time scale of the elastic neutron scattering experiments (similar to 10(-9) s). In this picture, the dynamic muon relaxation suggests a Pr3+ 4f correlation time of a few nanoseconds, which should be observable in a neutron spin echo experiment.