We report comprehensive Cu NMR studies on single crystals of
Sr14-xCaxCu24O41, which
contain simple CuO2 chains and two-leg
Cu2O3 ladders. From measurements of the
63Cu NMR shift, it is clear that the spin gap in the ladders
decreases with isovalent Ca substitution from Δ=550+/-30 K for
Sr14Cu24O41 (Sr14) to 350+/-30 K,
280+/-30 K, and 270+/-30 K for x=6 (Ca6), x=9 (Ca9), and x=11.5
(Ca11.5), respectively. The exponential decrease of the nuclear
spin-lattice relaxation rate 1/T1 below ~130 K is consistent
with the presence of the spin gap in the spin excitation spectrum. In
the T range higher than ~200 K, we observed the following dependences:
1/T1=const and the square of Gaussian spin-echo decay time,
T22G~T which are consistent with the scaling
theory for the S=1/2 one-dimensional (1D) Heisenberg model. The value of
T2G/T1T is compatible with the theoretical
prediction of an exchange constant along the leg J∥~1800
K for Ca6 and J∥~1500 K for Ca9 and Ca11.5. A notable
finding is that the magnitude of the spin gap remains nearly constant
and characteristics of novel 1D-like spin dynamics are maintained in the
content varying from Ca9 to Ca11.5. On the other hand, the charge
transport changes with increasing Ca content so that the more conductive
Ca11.5 exhibits pressure-induced superconductivity exceeding 3.5 GPa. We
have found that T22G, which is proportional to the
inverse spin correlation length ξ-1, deviates from a
linear T dependence upon cooling and is described by A+BT
exp(-Δ/T), regardless of the Ca substitution. We point out that
the value of T22G(T=0)=A is proportional to the
finite value of ξ-10=Δ/c1D,
where c1D=(π/2)J∥ is the spin-wave
velocity. From the result that the values of
A-1~ξeff for Ca6, Ca9, and Ca11.5 are
significantly reduced compared to that for Sr14, it is suggested that
ξeff is dominated at low T by an average distance d among
mobile holes obeying the relation ξeff~d=ξh.
From an estimate of ξ0/a~ 5.2 for Sr14, where a is the
Cu-Cu distance along the leg, ξh/a is obtained as ~3.5,
2.3, and 2.0, and hole content x as ~0.14, 0.22, and 0.25 per
Cu2O3 ladder for Ca6, Ca9, and Ca11.5,
respectively. These values were consistent with x= 0.14, 0.2, and 0.22
for Ca6, Ca9, and Ca11 estimated from the optical conductivity
experiment by Osafune et al. [Phys. Rev. Lett. 78, 1980 (1997)]. The
Sr14-xCaxCu24O41 compounds
are thus hole-doped two-leg spin-ladder systems which reveal the
metallic behavior dominated by the 1D-like spin dynamics at high T and
accompanied by the spin gap formation at low T. For Ca11.5, as the spin
gap is formed upon cooling below ~180 K, the resistivity increases in
the direction perpendicular to the ladder, whereas the conductivity
along the ladder remains metallic, followed by the localization of
mobile holes in both directions below TL~60 K. We point out
that preformed pairs are confined in each ladder and localized below ~60
K at an ambient pressure.