Magnetic Properties of a Quantum Ferrimagnet: NiCu(pba)(D_2O)_3 . 2D_2O

We report the results of magnetic measurements on a powder sample of NiCu(pba)(D_2O)_3 \cdot 2D_2O$(pba=1,3-propylenebis(oxamato)) which is one of the prototypical examples of an$S$=1/2 and 1 ferrimagnetic chain. Susceptibility($\chi$) shows a monotonous increase with decreasing temperature (T) and reaches a maximum at about 7 K. In the plot of$\chi T$versus$T$, the experimental data exhibit a broad minimum and are fit to the$\chi T$curve calculated for the ferrimagnetic Heisenberg chain composed of S=1/2 and 1. From this fit, we have evaluated the nearest-neighbor exchange constant$J/k_B=121 K$, the g-values of Ni$^{2+}$and Cu$^{2+}$,$g_{Ni}$=2.22 and$g_{Cu}$=2.09, respectively. Applied external field dependence of$\chi T$ at low temperatures is reproduced fairly well by the calculation for the same ferrimagnetic model.Comment: 7pages, 4 postscript figures, usues REVTEX. appear in J. Phys. Soc. Jpn vol 67 No.7 (1998

Ground State Property of an Alternating Spin Ladder Involving Two Kinds of Inter-Chain Interactions

The ground state property of the alternating spin ladder is studied in the case that the system involves an antiferromagnetic intra-chain interaction as well as two kinds of inter-chain interactions; one is between spins of the same magnitude and the other is between spins with different magnitudes. The calculation has been carried out by the exact diagonalization method. As a consequence of the competition among interactions, the system is revealed to show an interesting variety of phases in the ground state property. Its phase diagram is exhibited in the parameter space of the system. We find that, however small the total amount of the inter-chain interactions is, the ferrimagnetic ground state becomes unstable in a certain region. In this case, which of the ferrimagnetic and the singlet ground state to appear is determined only by the ratio between the inter-chain interactions regardless of their total amount. The nature of two phases appearing in the singlet region of the phase diagram and the type of the phase transition between them are also discussed. The results are ensured by comparing with those of obtained in other models which are contained in our model as special limiting cases.Comment: 12 pages, 9 PostScript figure

A DMRG Study of Low-Energy Excitations and Low-Temperature Properties of Alternating Spin Systems

We use the density matrix renormalization group (DMRG) method to study the ground and low-lying excited states of three kinds of uniform and dimerized alternating spin chains. The DMRG procedure is also employed to obtain low-temperature thermodynamic properties of these systems. We consider a 2N site system with spins $s_1$ and $s_2$ alternating from site to site and interacting via a Heisenberg antiferromagnetic exchange. The three systems studied correspond to $(s_1 ,s_2 )$ being equal to $(1,1/2),(3/2,1/2)$ and $(3/2,1)$; all of them have very similar properties. The ground state is found to be ferrimagnetic with total spin $s_G =N(s_1 - s_2)$. We find that there is a gapless excitation to a state with spin $s_G -1$, and a gapped excitation to a state with spin $s_G +1$. Surprisingly, the correlation length in the ground state is found to be very small for this gapless system. The DMRG analysis shows that the chain is susceptible to a conditional spin-Peierls instability. Furthermore, our studies of the magnetization, magnetic susceptibility $\chi$ and specific heat show strong magnetic-field dependences. The product $\chi T$ shows a minimum as a function of temperature T at low magnetic fields; the minimum vanishes at high magnetic fields. This low-field behavior is in agreement with earlier experimental observations. The specific heat shows a maximum as a function of temperature, and the height of the maximum increases sharply at high magnetic fields. Although all the three systems show qualitatively similar behavior, there are some notable quantitative differences between the systems in which the site spin difference, $|s_1 - s_2|$, is large and small respectively.Comment: 16 LaTeX pages, 13 postscript figure

Modified spin-wave theory of nuclear magnetic relaxation in one-dimensional quantum ferrimagnets: Three-magnon versus Raman processes

Nuclear spin-lattice relaxation in one-dimensional Heisenberg ferrimagnets is studied by means of a modified spin-wave theory. Calculating beyond the first-order mechanism, where a nuclear spin directly interacts with spin waves through the hyperfine coupling, we demonstrate that the exchange-scattering-enhanced three-magnon nuclear relaxation may generally predominate over the Raman one with increasing temperature and decreasing field. Recent proton spin-lattice relaxation-time (T_1_) measurements on the ferrimagnetic chain compound NiCu(C_7_H_6_N_2_O_6_)(H_2_O)_3_2H_2_O suggest that the major contribution to 1/T_1_ be made by the three-magnon scattering.Comment: 8 pages, 5 figure

Intrinsic double-peak structure of the specific heat in low-dimensional quantum ferrimagnets

Motivated by recent magnetic measurements on A3Cu3(PO4)4 (A=Ca,Sr) and Cu(3-Clpy)2(N3)2 (3-Clpy=3-Chloropyridine), both of which behave like one-dimensional ferrimagnets, we extensively investigate the ferrimagnetic specific heat with particular emphasis on its double-peak structure. Developing a modified spin-wave theory, we reveal that ferromagnetic and antiferromagnetic dual features of ferrimagnets may potentially induce an extra low-temperature peak as well as a Schottky-type peak at mid temperatures in the specific heat.Comment: 5 pages, 6 figures embedded, Phys. Rev. B 65, 214418 (2002

Low-Temperature Properties of Quasi-One-Dimensional Molecule-Based Ferromagnets

Quantum and thermal behaviors of low-dimensional mixed-spin systems are investigated with particular emphasis on the design of molecule-based ferromagnets. One can obtain a molecular ferromagnet by assembling molecular bricks so as to construct a low-dimensional system with a magnetic ground state and then coupling the chains or the layers again in a ferromagnetic fashion. Two of thus-constructed quasi-one-dimensional bimetallic compounds are qualitatively viewed within the spin-wave treatment, one of which successfully grows into a bulk magnet, while the other of which ends in a singlet ground state. Then, concentrating on the ferrimagnetic arrangement on a two-leg ladder which is well indicative of general coupled-chain ferrimagnets, we develop the spin-wave theory and fully reveal its low-energy structure. We inquire further into the ferromagnetic aspect of the ferrimagnetic ladder numerically calculating the sublattice magnetization and the magnetic susceptibility. There exists a moderate coupling strength between the chains in order to obtain the most ferromagnetic ferrimagnet.Comment: 10 pages, 7 figures embedded, to be published in J. Phys. Soc. Jpn. Vol.70, No.5 (2001

Low-Lying Excited States and Low-Temperature Properties of an Alternating Spin-1 / Spin-1/2 Chain : A DMRG study

We report spin wave and DMRG studies of the ground and low-lying excited states of uniform and dimerized alternating spin chains. The DMRG procedure is also employed to obtain low-temperature thermodynamic properties of the system. The ground state of a 2N spin system with spin-1 and spin-1/2 alternating from site to site and interacting via an antiferromagnetic exchange is found to be ferrimagnetic with total spin $s_G=N/2$ from both DMRG and spin wave analysis. Both the studies also show that there is a gapless excitation to a state with spin $s_G-1$ and a gapped excitation to a state with spin $s_G+1$. Surprisingly, the correlation length in the ground state is found to be very small from both the studies for this gapless system. For this very reason, we show that the ground state can be described by a variational ``ansatz'' of the product type. DMRG analysis shows that the chain is susceptible to a conditional spin-Peierls' instability. The DMRG studies of magnetization, magnetic susceptibility ($\chi$) and specific heat show strong magnetic-field dependence. The product $\chi T$ shows a minimum as a function of temperature($T$) at low-magnetic fields and the minimum vanishes at high-magnetic fields. This low-field behaviour is in agreement with earlier experimental observations. The specific heat shows a maximum as a function of temperature and the height of the maximum increases sharply at high magnetic fields. It is hoped that these studies will motivate experimental studies at high-magnetic fields.Comment: 22 pages in latex; 16 eps figures available upon reques

Magnetic Properties of Quantum Ferrimagnetic Spin Chains

Magnetic susceptibilities of spin-$(S,s)$ ferrimagnetic Heisenberg chains are numerically investigated. It is argued how the ferromagnetic and antiferromagnetic features of quantum ferrimagnets are exhibited as functions of $(S,s)$. Spin-$(S,s)$ ferrimagnetic chains behave like combinations of spin-$(S-s)$ ferromagnetic and spin-$(2s)$ antiferromagnetic chains provided $S=2s$.Comment: 4 pages, 7 PS figures, to appear in Phys. Rev. B: Rapid Commu

Simulated nuclear spin-lattice relaxation in Heisenberg ferrimagnets: Indirect observation of quadratic dispersion relations

In response to recent proton spin relaxation-time measurements on NiCu(pba)(H$_2$O)$_3$$\cdot$2H$_2$O with ${pba}=1,3{-propylenebis(oxamato)}$, which is an excellent one-dimensional ferrimagnetic Heisenberg model system of spin-$(1,{1/2})$, we study the Raman relaxation process in spin-$(S,s)$ quantum ferrimagnets on the assumption of predominantly dipolar hyperfine interactions between protons and magnetic ions. The relaxation time $T_1$ is formulated within the spin-wave theory and is estimated as a function of temperature and an applied field $H$ by a quantum Monte Carlo method. The low-temperature behavior of the relaxation rate $T_1^{-1}$ qualitatively varies with $(S,s)$, while $T_1^{-1}$ is almost proportional to $H^{-1/2}$ due to the characteristic dispersion relations.Comment: 5 pages, 3 figures embedded, to appear in Phys. Rev. B Rapid Commu

Combination of Ferromagnetic and Antiferromagnetic Features in Heisenberg Ferrimagnets

We investigate the thermodynamic properties of Heisenberg ferrimagnetic mixed-spin chains both numerically and analytically with particular emphasis on the combination of ferromagnetic and antiferromagnetic features. Employing a new density-matrix renormalization-group technique as well as a quantum Monte Carlo method, we reveal the overall thermal behavior: At very low temperatures, the specific heat and the magnetic susceptibility times temperature behave like $T^{1/2}$ and $T^{-1}$, respectively, whereas at intermediate temperatures, they exhibit a Schottky-like peak and a minimum, respectively. Developing the modified spin-wave theory, we complement the numerical findings and give a precise estimate of the low-temperature behavior.Comment: 9 pages, 9 postscript figures, RevTe