We report $^{123}$Sb nuclear quadrupole resonance (NQR) measurements of the filled skutterudite heavy-fermion superconductor PrOs$_4$Sb$_{12}$ under high pressure. The temperature dependence of NQR frequency and the spin-lattice relaxation rate $1/T_1$ indicate that the crystal-electric-field splitting $Δ_{\rm CEF}$ between the ground state $Γ_1$ singlet and the first excited state $Γ_4^{(2)}$ triplet decreases with increasing pressure. Ac-susceptibility measurements indicate that the superconducting transition temperature ($T_{\rm c}$) also decreases with increasing pressure. However, above $P$ $\sim$ 2 GPa, both $Δ_{\rm CEF}$ and $T_{\rm c}$ do not depend on external pressure up to $P$ = 3.82 GPa. These pressure dependences of $Δ_{\rm CEF}$ and $T_{\rm c}$ suggest an intimate relationship between quadrupole excitations associated with the $Γ_4^{(2)}$ level and unconventional superconductivity in PrOs$_4$Sb$_{12}$. In the superconducting state, 1/$T_1$ below $T_{\rm c}$ = 1.55 and 1.57 K at $P$ = 1.91 and 2.63 GPa shows a power-law temperature variations and are proportional to $T^5$ at temperatures considerably below $T_{\rm c}$. These data can be well fitted by the gap model $Δ(θ) = Δ_0\sinθ$ with $Δ_0$ = 3.08 $k_{\rm B}T_{\rm c}$ and 3.04 $k_{\rm B}T_{\rm c}$ for $P$ = 1.91 and 2.63 GPa, respectively. The results indicate there exists point nodes in the gap function.
We report $^{123}$Sb nuclear quadrupole resonance (NQR) measurements of the filled skutterudite heavy-fermion superconductor PrOs$_4$Sb$_{12}$ under high pressures of 1.91 and 2.34 GPa. The temperature dependence of NQR frequency and the spin-lattice relaxation rate $1/T_1$ indicate that the crystal-electric-field splitting $Δ_{\rm CEF}$ between the ground state $Γ_1$ singlet and the first excited state $Γ_4^{(2)}$ triplet decreases with increasing pressure. The 1/$T_1$ below $T_c$ = 1.55 K at $P$ = 1.91 GPa shows a power-law temperature variation and is proportional to $T^5$ at temperatures c…
Motivated by the recent observation of ferromagnetic spin correlations in the filled skutterudite SrFe$_4$As$_{12}$ [Ding et al., Phys. Rev. B 98, 155149 (2018)], we have carried out $^{75}$As nuclear magnetic resonance (NMR) and nuclear quadrupole resonance (NQR) measurements to investigate the role of magnetic fluctuations in a newly discovered isostructural superconductor SrOs$_4$As$_{12}$ with a superconducting transition temperature of $T_{\rm c}$ $\sim$ 4.8 K. Knight shift $K$ determined by the NQR spectrum under a small magnetic field ($\le$ 0.5 T) is nearly independent of temperature, …
We have carried out nuclear quadrupole resonance (NQR) measurements in the filled skutterudite compounds Pr(Os$_{1-x}$Ru$_x$)$_4$Sb$_{12}$ ($x=0.1, 0.2$), in order to gain insights into the symmetry of the superconducting gap function. Upon replacing Os with Ru, the spin-lattice relaxation rate $1/T_1$ becomes proportional to temperature ($T$) at low $T$ far below $T_c$, and the magnitude of $(1/T_1T)_{low-T}$ increases with increasing Ru content. These results indicate that a finite density of states is induced at the Fermi level by the impurity, and thus suggest that there exist nodes in the…
We report the electronic and superconducting properties in the Pr-based filled-skutterudite superconductor PrRu$_4$Sb$_{12}$ with $T_c = 1.3$ K via the measurements of nuclear-quadrupole-resonance (NQR) frequency $ν_Q$ and nuclear-spin-lattice-relaxation time $T_1$ of Sb nuclei. The temperature dependence of $ν_Q$ has revealed the energy scheme of Pr$^{3+}$ crystal electric field (CEF) that is consistent with an energy separation $Δ_{CEF}\sim 70$K between the ground state and the first-excited state. In the normal state, the Korringa relation of $(1/T_1T)_{Pr}$=const. is valid, with [$(1/T_{1}…
We report on Sb nuclear-quadrupole-resonance (NQR) study in filled-skutterudite compounds (Pr_1-xLa_x)Os_4Sb_12. The Sb-NQR spectra have split into two sets, arising from different Sb_12 cages containing either Pr or La, which enables us to measure two kinds of nuclear spin-lattice relaxation time T_1^Pr and T_1^La. In the normal state, the temperature (T) dependence of 1/T^Pr_1T showed almost the same behavior as that for PrOs_4Sb_12 regardless of. In contrast, 1/T^La_1T markedly decreases with increasing La concentration. In the superconducting state for x=0.05 and 0.2, 1/T_1^Pr exponentiall…
We present a novel phase diagram for the antiferromagnetism and superconductivity in Ce$_2$RhIn$_8$ probed by In-NQR studies under pressure ($P$). The quasi-2D character of antiferromagnetic spin fluctuations in the paramagnetic state at $P$ = 0 evolves into a 3D character because of the suppression of antiferromagnetic order for $P > P_{\rm QCP}\sim$ 1.36 GPa (QCP: antiferromagnetic quantum critical point). Nuclear-spin-lattice-relaxation rate $1/T_1$ measurements revealed that the superconducting order occurs in the $P$ range 1.36 -- 1.84 GPa, with maximum $T_c\sim$ 0.9 K around $P_{\rm QCP}…
We report Cu nuclear-quadrupole-resonance results under pressure on a homogeneous CeCu2Si2 (Tc = 0.65 K) that revealed critical magnetic fluctuations at the border to an antiferromagnetic phase. This exotic superconducting phase evolves into the typical heavy-fermion superconducting phase at minute pressures exceeding Pc ~ 0.2 GPa. The nuclear spin-lattice relaxation data in a pressure range 0.85 - 2.58 GPa are shown to be accountable by the SCR theory based on the nearly antiferromagnetic Fermi-liquid model. In 0 < P < Pc ~ 0.2 GPa, by contrast, we conclude that the exotic superconducting pha…
We report a pressure ($P$) effect on CeCu$_2$(Si$_{0.98}$Ge$_{0.02}$)$_2$ where an antiferromagnetic (AFM) order at $T_N \sim$ 0.75 K coexists with superconductivity below $T_c \sim$ 0.4 K\@. At pressures exceeding $P = 0.19$ GPa, the AFM order is suppressed, which demonstrates that the sudden emergence of AFM order due to the Ge doping is ascribed to the intrinsic lattice expansion. The exotic superconductivity at $P = 0$ GPa is found to evolve into a typical heavy-fermion one with a line-node gap above $P = 0.91$ GPa\@. We highlight that the anomalous enhancement in nuclear spin-lattice rela…
We report $^{121,123}$Sb nuclear quadrupole resonance (NQR) measurements in the filled-skutterudite superconductor PrOs$_4$Sb$_{12}$ in the temperature range of 0.05-30 K. The electric field gradients (EFG), $V_{zz}$ and $V_{xx}-V_{yy}$, at the Sb site exhibit unusual temperature dependence below 30 K. To explain these features, we discuss the coupling between the Sb nuclear quadrupole moment and Pr $4f^2$-derived multipole moments. The observed $T$ dependence of EFG is well explained by the CEF quasi-quartet consisted of $Γ_1$ singlet and $Γ_4^{(2)}$ triplet states in the cubic point group $T…
We report $^{115}$In nuclear-quadrupole-resonance (NQR) measurements of the pressure($P$)-induced superconductor CeRhIn$_5$ in the antiferromagnetic (AF) and superconducting (SC) states. In the AF region, the internal field $H_{int}$ at the In site is substantially reduced from $H_{int}=1.75$ kOe at P=0 to 0.39 kOe at $P=1.23$ GPa, while the Néel temperature slightly changes with increasing $P$. This suggests that either the size in the ordered moment $M_{Q}(P)$ or the angle $θ(P)$ between the direction of $M_{Q}(P)$ and the tetragonal $c$ axis is extrapolated to zero at $P^*=1.6 \pm 0.1$ GPa …
We report evidence for unconventional superconductivity in CeIn_3 at a pressure P = 2.65 GPa above critical pressure (P_c ~ 2.5 GPa) revealed by the measurements of nuclear-spin-lattice-relaxation time (T_1) and ac-susceptibility (ac-chi). Both the measurements of T_1 and ac-chi have pointed to a superconducting transition at T_c = 95 mK, which is much lower than an onset temperature T_{onset} = 0.15 K at zero resistance. The temperature dependence of 1/T_1 shows no coherence peak just below T_c, indicative of an unconventional nature for the superconductivity induced in CeIn_3.
We report Sb-NQR results which evidence a heavy-fermion (HF) behavior and an unconventional superconducting (SC) property in the filled-skutterudite compound PrOs_4Sb_12 revealing a SC transition temperature T_c=1.85 K. The temperature (T) dependence of nuclear-spin-lattice-relaxation rate 1/T_1 and NQR frequency unravel a low-lying crystal-electric-field splitting below T_0~10 K, associated with Pr^3+ (4f^2)-derived ground state. The emergence of T_1T=const. behavior below T_F~4 K points to the formation of heavy-quasiparticle state. In the SC state, 1/T_1 shows neither a coherence peak nor a…
We report on the itinerant ferromagnetic superconductor UGe_2 through ^73Ge-NQR measurements under pressure (P). The P dependence of the NQR spectrum signals a first-order transition from the low-temperature (T) and low-P ferromagnetic phase (FM2) to high-T and high-P one (FM1) around a critical pressure of P_x ~ 1.2 GPa. The superconductivity exhibiting a maximum value of T_sc=0.7 K at P_x ~ 1.2 GPa, was found to take place in connection with the P-induced first-order transition. The nuclear spin-lattice relaxation rate 1/T_1 has probed the ferromagnetic transition, exhibiting a peak at the C…
We report the novel pressure($P$) - temperature($T$) phase diagram of antiferromagnetism and superconductivity in CeRhIn$_5$ and CeIn$_3$ revealed by the $^{115}$In nuclear-spin-lattice-relaxation ($T_1$) measurement. In the itinerant magnet CeRhIn$_5$, we found that the Néel temperature $T_N$ is reduced at $P \geq$ 1.23 GPa with an emergent pseudogap behavior. In CeIn$_3$, the localized magnetic character is robust against the application of pressure up to $P \sim$ 1.9 GPa, beyond which the system evolves into an itinerant regime in which the resistive superconducting phase emerges. We discus…
We report on a novel pressure ($P$)-induced evolution of magnetism and superconductivity (SC) in a helical magnet CeRhIn$_5$ with an incommensurate wave vector $Q_i=({1/2},{1/2},0.297)$ through the $^{115}$In nuclear quadrupole resonance (NQR) measurements under $P$. Systematic measurements of the $^{115}$In-NQR spectrum reveal that the commensurate antiferromagnetism (AFM) with $Q_c=({1/2},{1/2},{1/2})$ is realized above $P_m \sim$ 1.7 GPa. An important finding is that the size of SC gap and $T_c$ increase as the magnitude of the AFM moment decreases in the $P$ region, where SC uniformly coex…
We report the discovery of exotic superconductivity (SC) and novel magnetism in heavy-fermion (HF) compounds, CeCu$_2$Si$_2$, CeRhIn$_5$ and CeIn$_3$ through nuclear-quadrupole-resonance (NQR) measurements under pressure ($P$). The exotic SC in a homogeneous CeCu$_2$Si$_2$ revealed antiferromagnetic critical fluctuations at the border to antiferromagnetism (AFM) or marginal AFM. The uniform mixed phase of SC and AFM in CeCu$_2$(Si$_{1-x}$Ge$_x$)$_2$ emerges on a microscopic level, once a tiny amount of 1%Ge($x=0.01$) is substituted for Si to expand its lattice. The application of minute pressu…
We report on the pressure-induced unconventional superconductivity in the heavy-fermion antiferromagnet CeIn3 by means of nuclear-quadrupole-resonance (NQR) studies conducted under a high pressure. The temperature and pressure dependences of the NQR spectra have revealed a first-order quantum-phase transition (QPT) from an AFM to PM at a critical pressure Pc=2.46 GPa. Despite the lack of an AFM quantum critical point in the P-T phase diagram, we highlight the fact that the unconventional SC occurs in both phases of the AFM and PM. The nuclear spin-lattice relaxation rate 1/T1 in the AFM phase …
The Ca10(PtnAs8)(Fe2As2)5 (n=3,4) compounds are a new type of iron pnictide superconductors whose structures consist of stacking Ca-PtnAs8-Ca-Fe2As2 layers in a unit cell. When n=3 (the 10-3-8 phase), the undoped compound is an antiferromagnetic (AFM) semiconductor, while, when n=4 (the 10-4-8 phase), the undoped compound is a superconductor with the transition temperature of 26K. Here we report the results of high-pressure studies on the 10-3-8 compound obtained through a combination of in-situ resistance, magnetic susceptibility, and Hall coefficient measurements. We find that its AFM order …
We report on two fold increase in superconducting transition temperature of La3Co4Sn13 by substituting indium at the tin site. The transition temperature of this skutterudite is observed to increase from 2.5 K to 5.1 K for 10 % indium substituted sample. The band structure and density of states calculations also indicate such a possibility. The compounds exhibit type - II superconductivity and the values of lower critical field (Hc1), upper critical field (Hc2), Ginzburg - Landau coherence length , penetration depth and GL parameter are estimated to be 0.0028 T, 0.68 T, 21.6 nm, 33.2 nm and 1.…
We report systematic measurements of ac-susceptibility, nuclear-quadrupole-resonance spectrum, and nuclear-spin-lattice-relaxation time ($T_1$) on the pressure ($P$)- induced heavy-fermion (HF) superconductor CeRhIn$_5$. The temperature ($T$) dependence of $1/T_1$ at $P$ = 1.6 GPa has revealed that antiferromagnetism (AFM) and superconductivity (SC) coexist microscopically, exhibiting the respective transition at $T_N = 2.8$ K and $T^{MF}_c$ = 0.9 K. It is demonstrated that SC does not yield any trace of gap opening in low-lying excitations below $T_c^{onset} = 2$ K, but $T_c^{MF} = 0.9$ K, fo…
We report on a pressure-induced evolution of exotic superconductivity and spin correlations in CeIr(In$_{1-x}$Cd$_{x}$)$_5$ by means of In-Nuclear-Quadrupole-Resonance (NQR) studies. Measurements of an NQR spectrum and nuclear-spin-lattice-relaxation rate $1/T_1$ have revealed that antiferromagnetism induced by the Cd-doping emerges locally around Cd dopants, but superconductivity is suddenly induced at $T_c$ = 0.7 and 0.9 K at 2.34 and 2.75 GPa, respectively. The unique superconducting characteristics with a large fraction of the residual density of state at the Fermi level that increases wit…
We present the results of $^{75}$As nuclear magnetic resonance (NMR), nuclear quadrupole resonance (NQR), and resistivity measurements in KFe$_2$As$_2$ under pressure ($p$). The temperature dependence of the NMR shift, nuclear spin-lattice relaxation time ($T_1$) and resistivity show a crossover between a high-temperature incoherent, local-moment behavior and a low-temperature coherent behavior at a crossover temperature ($T^*$). $T^*$ is found to increase monotonically with pressure, consistent with increasing hybridization between localized $3d$ orbital-derived bands with the itinerant elect…
We report magnetic neutron-diffraction and electrical resistivity studies on single crystals of the heavy-fermion antiferromagnet CeRhIn$_{5}$ at pressures up to 2.3 GPa. These experiments show that the staggered moment of Ce and the incommensurate magnetic structure change weakly with applied pressure up to 1.63 GPa, where resistivity, specific heat and NQR measurements confirm the presence of bulk superconductivity. This work places new constraints on an interpretation of the relationship between antiferromagnetism and unconventional superconductivity in CeRhIn$_{5}$.
Pressure-induced superconductivity was studied for a spin-ladder cuprate Sr$_2$Ca$_{12}$Cu$_{24}$O$_{41}$ using nuclear magnetic resonance (NMR) under pressures up to the optimal pressure 3.8 GPa. Pressure application leads to a transitional change from a spin-gapped state to a Fermi-liquid state at temperatures higher than $T_c$. The relaxation rate $1/T_1$ shows activated-type behavior at an onset pressure, whereas Korringa-like behavior becomes predominant at the optimal pressure, suggesting that an increase in the density of states (DOS) at the Fermi energy leads to enhancement of $T_c$. N…
A fundamental problem posed from the study of correlated electron compounds, of which heavy-fermion systems are prototypes, is the need to understand the physics of states near a quantum critical point (QCP). At a QCP, magnetic order is suppressed continuously to zero temperature and unconventional superconductivity often appears. Here, we report pressure ($P$) -dependent $^{115}$In nuclear quadrupole resonance (NQR) measurements on heavy-fermion antiferromagnet CeRh$_{0.5}$Ir$_{0.5}$In$_5$. These experiments reveal an antiferromagnetic (AF) QCP at $P_{\rm c}^{\rm AF}$ = 1.2 GPa where a dome o…
We report T_c and ^{59}Co nuclear quadrupole resonance (NQR) measurements on the cobalt oxide superconductor Na_{x}CoO_{2}\cdot 1.3H_{2}O (T_c=4.8 K) under hydrostatic pressure (P) up to 2.36 GPa. T_c decreases with increasing pressure at an average rate of -0.49\pm0.09 K/GPa. At low pressures P\leq0.49 GPa, the decrease of T_c is accompanied by a weakening of the spin correlations at a finite wave vector and a reduction of the density of states (DOS) at the Fermi level. At high pressures above 1.93 GPa, however, the decrease of T_c is mainly due to a reduction of the DOS. These results indica…
We performed $^{185/187}$Re nuclear quadrupole resonance (NQR) measurements under pressure to investigate the superconducting properties of noncentrosymmetric superconductor Cd$_{2}$Re$_{2}$O$_{7}$ under various crystal structures. The pressure dependence of superconducting transition temperature $T_{\rm c}$ determined through ac susceptibility measurements is consistent with the results of previous resistivity measurements [T. C. Kobayashi $et al$., J. Phys. Soc. Jpn. 80, 023715 (2011).]. Below 2.2 GPa, in the nuclear spin-lattice relaxation rate $1/T_{1}$, a clear coherence peak was observed…
We report the novel pressure(P)-temperature(T) phase diagrams of antiferromagnetism (AF) and superconductivity (SC) in CeRhIn$_5$, CeIn$_3$ and CeCu$_2$Si$_2$ revealed by the NQR measurement. In the itinerant helical magnet CeRhIn$_5$, we found that the Néel temperature $T_N$ is reduced at $P \geq$ 1.23 GPa with an emergent pseudogap behavior. The coexistence of AF and SC is found in a narrow P range of 1.63 - 1.75 GPa, followed by the onset of SC with line-node gap over a wide P window 2.1 - 5 GPa. In CeIn$_3$, the localized magnetic character is robust against the application of pressure up …
We report a study on the interplay between antiferromagnetism (AFM) and superconductivity (SC) in a heavy-fermion compound CeRhIn$_5$ under pressure $P=1.75$ GPa. The onset of the magnetic order is evidenced from a clear split of $^{115}$In-NQR spectrum due to the spontaneous internal field below the Néel temperature $T_N=2.5$ K. Simultaneously, bulk SC below $T_c=2.0$ K is demonstrated by the observation of the Meissner diamagnetism signal whose size is the same as in the exclusively superconducting phase. These results indicate that the AFM coexists homogeneously with the SC at a microscopic…
Pressure evolution of the normal- and superconducting-state properties of the line-nodal material CaSb$_2$ revealed by $^{123}$Sb nuclear quadrupole resonance
