Nuclear Spin Relaxation in Hole Doped Two-Leg Ladders

The nuclear spin-lattice relaxation rate ($1/T_{1}$) has been measured in the single crystals of hole doped two-leg ladder compounds Sr$_{14-x}$Ca$_{x}$Cu$_{24}$O$_{41}$ and in the undoped parent material La$_6$Ca$_8$Cu$_{24}$O$_{41}$. Comparison of $1/T_{1}$ at the Cu and the two distinct oxygen sites revealed that the major spectral weight of low frequency spin fluctuations is located near $q \sim (\pi, \pi)$ for most of the temperature and doping ranges investigated. Remarkable difference in the temperature dependence of $1/T_1$ for the two oxygen sites in the heavily doped $x$=12 sample revealed reduction of singlet correlations between two legs in place of growing antiferromagnetic correlations along the leg direction with increasing temperature. Such behavior is most likely caused by the dissociation of bound hole pairs.