Anisotropic Spin Fluctuations and Superconductivity in ‘115’ Heavy Fermion Compounds : 59Co NMR Study in PuCoGa 5 S.-H. Baek et. al. PRL 105,217002(2010) Kazuhiro Nishimoto Kitaoka lab. 1 Contents • Introduction - History of superconductivity - Heavy fermion system - Transuranic HF compounds - Motivation •Measurement - NMR (Nuclear Magnetic Resonance) • Experimental Results (PuCoGa5) • Summary 2 introduction History of Superconductivity Transition temperature (K) 200 metal heavy fermion system high-Tc cuprate 163 iron-based system 150 1911 Hg-Ba-Ca-Cu-O (under high pressure) Discovery of superconducting phenomenon Hg-Ba-Ca-Cu-O Tl-Ba-Ca-Cu-O Bi-Sr-Ca-Cu-O 100 Y-Ba-Cu-O 77 1979 Heavy fermion superconductor 1986 50 MgB2 Pb Hg Nb NbC La-Ba-Cu-O PuCoGa5 NbGe NbN CeCu2Si2 SmO0.9F0.11FeAs LaO0.89F0.11FeAs LaOFeP 0 1900 1920 1940 1960 1980 2000 2020 Year High-Tc cuprate superconductor 2006 Iron-based high-Tc superconductor 3 introduction Heavy Fermion System What does “Heavy” mean? Heavy Fermion system Normal metal + + + f + f + f + + + + f + f f + + c-f hybridization ( c-f 混成) Strong electron correlation makes effective mass large. “Heavy” ⇒ large effective mass 4 introduction Heavy Fermion System Example of heavy fermion superconductor compounds CeCu2Si2 CePd2Si2 CeRh2Si2 CeIn3 CeRhIn5 PrOs4Sb12 lanthanide compounds ⇒some 4f electrons UPt3 UPd2Al3 PuCoGa5 actinide compounds ⇒some 5f electrons All of HF compounds have f-electrons. 5 Transuranic HF Compounds introduction transuranium elements (超ウラン元素) • don’t exist in nature • Handling is difficult because of strong radioactivity example : PuCoGa5 , PuRhGa5 , NpPd5Al2 6 introduction Motivation iso-structural superconductor PuCoGa5 : Pu-115 compounds 5f-electron : 5個 Tc = 18.5 K CeCoIn5 : Ce-115 compounds 4f-electron : 1個 Tc = 2.3 K Amazingly high Tc in HF 115 compounds NMR study (PuCoGa5 in normal state) • Spectra • K (Knight shift) • 1/T1T 7 Introduction measurement NMR spectra I =1/2 m=-1/2 gℏ H0 m=+1/2 NMR Intensity Zeeman splitting 0 ω 8 measurement Δ𝑯 𝑯0 NMR Intensity Knight shift ΔH 𝐼 H electron H res H0 ℋ𝑍𝑒𝑒𝑚𝑎𝑛 = −𝛾ℏ𝑰 ∙ 𝑯0 + Δ𝑯 𝜔 = 𝛾𝑯0 = 𝛾 𝑯𝑟𝑒𝑠 + Δ𝑯 = 𝛾 ∙ 𝑯𝑟𝑒𝑠(1 + 𝐾) Knight shift Δ𝐻 𝐾≡ 𝐻𝑟𝑒𝑠 9 measurement T1~spin-lattice relation time Release the energy Excitation energy I=-1/2 I=+1/2 spin-lattice interaction nuclear spin electronic spin Energytransfer 1/T1 is quite sensitive to spin fluctuations 10 59Co result NMR Spectra at 19 K Co : I =7/2 g = 10.103MHz/T Spectra • Quadrupole Interaction : I >1 (電気四重極相互作用) • νQ = 1.02 MHZ νQ 11 result Knight shifts and 1/T1 ~T3 • Knight shifts show strongly anisotropic behavior. • At Tc both sifts drop sharply , indicating spin-singlet pairing. Spin singlet S=0 • 1/T1⇒d-wave superconductor anisotropic : 異方性 12 result 1/T1T in 115 compounds 5f-electrons PuCoGa5 LuCoGa5 PuCoGa5 LuCoGa5 5個 0個 • LuCoGa5 1/T1T = const conduction electrons ⇒ metallic • PuCoGa5 conduction electrons + 5f-electrons ⇒heavy fermion state Spin fluctuations develop as temperature decrease. Anisotropy (T1T)∥-1 / (T1T)⊥-1 reaches a maximum just above Tc . 13 result Korringa ratio Korringa ratio RK > 1 ⇒ antiferromagnetic RK ~ 1 ⇒Fermi gas RK < 1 ⇒ ferromagnetic From K(T) and 1/T1T , Rk ranges from 5 to 16 Strong AFM fluctuations in PuCoGa5 14 result Anisotropic nature PuCoGa5 : tetragonal structure (a=b≠c) new spin-lattice relaxation rate (1/T1T )H∥c = 2Ra • in-plane component : Ra • out-of-plane component : Rc (1/T1T )H⊥c = Ra+Rc AFM spin fluctuation is strong In XY-plane. 15 result Ratio of spin fluctuation energy : ρ g n A (0) Spin fluctuation energy : 2R ratio : c A c a A a χ″(q=Q,ω) Ra K c (T ) Ra a Rc K a (T ) Rc c Γ Magnetic order ω 115 HF compounds ρ > 1 ⇒ XY-like anisotropy Cuprates : YBa2Cu3O7 ρ ⋍ 1 ⇒ isotropic 16 Tc versus Γa/Γc for 115 HF superconductors result • Reduced dimensionality could enhance Tc . • Anisotropy Γc/Γa is a good parameter for determining Tc . 17 Summary PuCoGa5 : 59CoNMR study in the normal state • Spin fluctuations promote d-wave superconductivity in the iso-structural 115 HF compounds. • Both the Knight shift K and the spin-lattice relaxation rate 1/T1 are strongly anisotropic. • The ratio Γc/Γa (spin fluctuation energy) is a characteristic quantity in 115 HF compounds. This suggest the possibility that anisotropic spin-fluctuations enhance Tc . 18 a: 71Ga NMR spectra in 8T b : The normal-state magnetic shift K tot of the 59Co and 71Ga(1) versus bulk susceptibility x. c : The total magnetic shift K tot of the 59Co and 71Ga(1) versus temperature. 1/T1 温度依存性 ~T0.35 ~T3 Normalized spin susceptibility in the superconducting state. 71Ga 59Co (T 1T )-1/(T 1T )-10 versus T/Tc (T 1T )-10 is given by the value of (T 1T )-1 at 1.25Tc Tc versus the characteristic spin fluctuation energy T0 T0 = ΓqB2/2π 1000 Tl2Ba2Ca2Cu3O10 YBa2Cu3O6+x 100 HgBa2Ca2Cu3O8+ Tc (K) PuCoGa5 10 CeRhIn5 1 La1.85Sr0.15CuO4 CeCoIn5 U6Fe UBe13 UPt3 CeIrIn5 CeCu2Si2 0.1 10 UPd2Al3 URu2Si2 UNi2Al3 100 T0 (K) 1000 10000 c/a ratio of tetragonal structure parameter versus Tc Temperature - pressure phase diagram 電気四重極相互作用 C軸となす角度 H∥c θ=0° H⊥c θ=90° Crystal structure in 115 compounds 遍歴的 局在的 What can we know from Knight shift ? ~Symmetry of Cooper pair~ Cooper pairing state ψ(r1-r2;s1,s2) = Φ(r1-r2) σ (s1,s2) orbital orbital part spin spin part even function (s, d wave) spin-singlet Φ (-(r1-r2)) =Φ (r1-r2) s (s2,s1) = -s (s1,s2) S=0 s-wave odd function (p wave) Φ (-(r1-r2)) = -Φ (r1-r2) spin-triplet s (s2,s1) = s(s1,s2) S=1 d-wave p-wave 1/T1 in various superconductors Conventional type (BCS) NS(E) NS(E) N0 1 e T1 s-wave EF EF +Δ0 k BTc Line nodes N0 1 T3 T1 EF EF +Δ0 NbB2 101 d-wave Tc=5K 1/ T1 ( sec-1 ) unconventional superconductors (non BCS) p-wave MgB2 100 Tc(H) Point nodes ~T 2/kBTc=2.85 10-1 1 T5 T1 ~exp(-/kBT) 2/kBTc=5 10-2 1 10 Temperature ( K ) 100 EF EF +Δ0