We performed17 O nuclear magnetic resonance measurements on superconducting (SC) Sr2RuO4 under in-plane magnetic fields. We found that no new signal appears in the SC state and that the 17 O Knight shifts obtained from the double-site measurements remain constant across the first-order phase-transition line, as well as across the second-order phase-transition line as already reported. The present results indicate that the SC spin susceptibility does not decrease in the high-field region, although a magnetization jump in the SC state was reported at low temperatures. Because the spin susceptibility is unchanged in the SC state in Sr2RuO4, we suggest that the first-order phase transition across the upper critical field should be interpreted as a depairing mechanism other than the conventional Pauli-paramagnetic effect.The layered perovskite Sr 2 RuO 4 has attracted special attention, because it has been suggested that Sr 2 RuO 4 may be a chiral p-wave spin-triplet superconductor.1 The chiral state is shown from the broken time-reversal symmetry probed by µSR 2 and Kerr-effect 3 measurements. The existence of spin-triplet equal-spin pairing is based on experimental results that show the spin susceptibility is unchanged on passing through the superconducting (SC) transition temperature T c , as revealed by nuclear magnetic resonance (NMR) Knight-shift measurements at the Ru and O sites 4-8 and polarized neutron scattering measurements.9 The chiral p-wave spin-triplet state would be an SC state analogous to the superfluid 3 He A-phase with two dimensionality.However, several recent experimental results are difficult to interpret with the above SC state. The firstorder (FO) SC-normal (S-N) transition 10 accompanied by a clear magnetization jump 11 is observed in a lowtemperature region near the upper critical field H c2 for fields parallel to the ab plane. This abrupt S-N transition suggests that Sr 2 RuO 4 is a spin-singlet superconductor, because this cannot be interpreted by the conventional orbital depairing effect but seems to be explained consistently by the conventional Pauli-paramagnetic effect. Indeed, the experimental µ 0 H c2 for T → 0 nearly matches the Pauli-limiting field µ 0 H Pauli estimated using the well-1/2 ∼ 1.4 T with χ sc = 0, where E cond is the SC condensation energy and χ n and χ sc are the spin susceptibilities in the normal and SC states, respectively. Here, χ sc = 0 means that the spin susceptibility totally vanishes in the SC state, which contradicts the above spin-susceptibility results showing χ n = χ sc .Recently, we performed 99 Ru Knight-shift ( 99 K) measurements again to re-examine the previous results, and found a new phenomenon that the spin susceptibility slightly increases in the SC state at lower magnetic fields.12 We reported that this experimental result further suggests the spin-triplet equal-spin pairing state.
13Because the hyperfine coupling constant A hf at the 99 Ru site is largest among the nuclei that are feasible for NMR in Sr 2 RuO 4 ( 99 A hf ∼ −25 T/µ B ), 6 the s...