Abstract

We have performed magnetic susceptibility $(\ensuremath{\chi})$, heat capacity $({C}_{p})$, and nuclear magnetic resonance (NMR) measurements on the layered compound ${\mathrm{Na}}_{2}{\mathrm{Mn}}_{3}{\mathrm{O}}_{7}$ in which the magnetic ${\mathrm{Mn}}^{4+}$ ions constitute a maple-leaf lattice. At high temperature, $\ensuremath{\chi}$ follows the Curie-Weiss (CW) law with CW temperature as high as 152 K and ${\mathrm{Mn}}^{4+}$ ions are found to be in the high-spin state $(S=\frac{3}{2})$. With decreasing temperature, $\ensuremath{\chi}$ passes through a broad maximum at 115 K and decreases rapidly at low temperature. A similar broad peak appears at around 62 K in the magnetic contribution to heat capacity $({C}_{m})$. The temperature dependence of $\ensuremath{\chi}$ and ${C}_{m}$ are the characteristics of an one-dimensional Heisenberg antiferromagnetic spin chain with a nonmagnetic ground state. The obtained values of spin-gap energy $({\mathrm{\ensuremath{\Delta}}}_{s})$ and nearest-neighbor antiferromagnetic exchange coupling $(J)$ are 28 and 27 K, respectively. There is no evidence of a long-range magnetic ordering down to 2 K in heat capacity data, in agreement with spin-singlet ground state. These observations are further corroborated by $^{23}\mathrm{Na}$ NMR studies through measurements of both the NMR shift and the spin-lattice relaxation rate.

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