The magnetic susceptibility and high-field magnetization process of NH 4 CuCl 3 with double chains of CuCl 3 have been measured using single crystals. No anomaly indicative of the threedimensional ordering is observed in susceptibility data above 1.7 K. It is found, by magnetization measurement down to 0.5 K, that in contrast to KCuCl 3 and TlCuCl 3 , NH 4 CuCl 3 has a gapless magnetic ground state at zero field. It is observed that the magnetization curve has two plateaus at one-quarter and three-quarters of the saturation magnetization, irrespective of the external field direction. The origin of the plateaus is attributed not to the magnetic anisotropy, but to the quantum effect. The relation between the plateaus and the period of the spin state is discussed in terms of a recent theory presented by Oshikawa et al. [Phys. Rev. Lett. 78 (1997) 1984.KEYWORDS: NH 4 CuCl 3 , double chain, high field, magnetization process, magnetization plateausThe magnetization processes of low-dimensional quantum spin systems with spatial structures such as spin ladders and exchange-alternating chains, are new problems in magnetism. In particular, magnetization plateaus are of great interest, because the magnetization is quantized at the plateaus. In a spin-1/2 Heisenberg chain with ferromagnetic (J F )-ferromagnetic (J F )-antiferromagnetic (J AF ) interactions, the magnetization curve has a plateau at 1/3 of the saturation magnetization M s , when J F /J AF < 5 ∼ 6.1, 2) For a spin-1/2 antiferromagnetic alternating Heisenberg chain with the next-nearestneighbor interaction, a plateau can appear at (1/2)M s in an appropriate parameter region. 3,4) In this case the next-nearest-neighbor interaction is essential for the existence of the plateau. The period of the spin state at the plateau is twice as large as the period of the Hamiltonian.4) Thus the plateau is caused by the quantum manybody effect. For a spin-1 antiferromagnetic Heisenberg chain, a plateau exists at (1/2)M s as long as the exchange interaction alternates.5, 6) The 1/2-plateau has been observed experimentally in the nickel compound8) investigated general Heisenberg chains in a magnetic field. They showed that the magnetization can have plateaus, and that it is quantized at the plateaus aswhere n is the period of the spin state, S the magnitude of spin and m the magnetization per site in the unit of gμ B . All of the above-mentioned plateaus satisfy this quantization condition. * Author to whom correspondence should be addressed. E-mail: tanaka@lee.cme.phys.titech.ac.jp
1548In this letter we report the magnetization plateaus observed in NH 4 CuCl 3 . At room temperature, NH 4 CuCl 3 is isostructural with KCuCl 3 which belongs to the monoclinic space group P 2 1 /c. 9, 10) The crystal structure is composed of double chains of edge-sharing CuCl 6 octahedra along the a-axis. The double chains are located at the corners and center of the unit cell in the bc-plane, and are separated by NH 4+ ions. There are three kinds of nearest-neighbor-interactions, J 1 , J 2 and J 3...