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Journal of Applied Physics

Thermodynamic properties of Cu3(CO3)2(OH)2 and the spin-1/2 distorted diamond Heisenberg chain

Yanchao Li

Published Dec 1, 2007• 17 citations
Publisher

Abstract

The thermodynamic properties of the spin-1/2 diamond quantum Heisenberg chain model have been investigated by means of the transfer matrix renormalization group (TMRG) method. Considering different crystal structures, by changing the interactions among different spins and the external magnetic fields, we first investigate the magnetic susceptibility, magnetization, and specific heat of the distorted diamond chain as a model of ferrimagnetic spin systems. The susceptibility and the specific heat show different features for different ferromagnetic (F) and antiferromagnetic (AF) interactions and different magnetic fields. A 1/3 magnetization plateau is observed at low temperature in a magnetization curve. Then, we discuss the theoretical mechanism of the double-peak structure of the magnetic susceptibility and the three-peak structure of the specific heat of the compound Cu3(CO3)2(OH)2, on which an elegant measurement was performed by Kikuchi et al. [Phys. Rev. Lett. 94, 227201 (2005)]. Our computed results are consistent with the main characteristics of the experimental data. Meanwhile, we find that the double-peak structure of susceptibility can be found in several different kinds of spin interactions in the diamond chain. Moreover, a three-peak behavior is observed in the TMRG results of magnetic susceptibility. In addition, we perform calculations relevant for some experiments and explain the characteristics of these materials.

DOI
10.1063/1.2817645

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The thermodynamic properties of the spin-1/2 diamond quantum Heisenberg chain model have been investigated by means of the transfer matrix renormalization group (TMRG) method. Considering different crystal structures, by changing the interactions among different spins and the external magnetic fields, we first investigate the magnetic susceptibility, magnetization, and specific heat of the distorted diamond chain as a model of ferrimagnetic spin systems. The susceptibility and the specific heat show different features for different ferromagnetic (F) and antiferromagnetic (AF) interactions and different magnetic fields. A 1/3 magnetization plateau is observed at low temperature in a magnetization curve. Then, we discuss the theoretical mechanism of the double-peak structure of the magnetic susceptibility and the three-peak structure of the specific heat of the compound Cu3(CO3)2(OH)2, on which an elegant measurement was performed by Kikuchi et al. [Phys. Rev. Lett. 94, 227201 (2005)]. Our computed results are consistent with the main characteristics of the experimental data. Meanwhile, we find that the double-peak structure of susceptibility can be found in several different kinds of spin interactions in the diamond chain. Moreover, a three-peak behavior is observed in the TMRG results of magnetic susceptibility. In addition, we perform calculations relevant for some experiments and explain the characteristics of these materials.
The magnetic and thermodynamic properties of spin-1∕21∕21∕2 Heisenberg diamond chains are investigated in three different cases: (a) J1{J}_{1}J1​, J2{J}_{2}J2​, J3>0{J}_{3}>0J3​>0 (frustrated), (b) J1{J}_{1}J1​, J3<0{J}_{3}<0J3​<0, J2>0{J}_{2}>0J2​>0 (frustrated), and (c) J1{J}_{1}J1​, J2>0{J}_{2}>0J2​>0, J3<0{J}_{3}<0J3​<0 (nonfrustrated), where the bond coupling Ji{J}_{i}Ji​ (i=1,2,3)>0(i=1,2,3)>0(i=1,2,3)>0 stands for an antiferromagnetic (AF) interaction, and <0<0<0 for a ferromagnetic (F) interaction. The density-matrix renormalization-group (DMRG) technique is invoked to study the properties of the system in the ground state, while the transfer-matrix renormalization-group (TMRG) technique is applied to explore the thermodynamic properties. The local magnetic moments, spin-correlation functions, and static structure factors are discussed in the ground state for the three cases. It is shown that the static structure factor S(q)S(q)S(q) shows peaks at wave vectors $q=a\ensuremath{\pi}∕3$ (a=0,1,2,3,4,5)(a=0,1,2,3,4,5)(a=0,1,2,3,4,5) for different couplings in a zero magnetic field, which, however, in the magnetic fields where the magnetization plateau with m=1∕6m=1∕6m=1∕6 pertains, exhibits the peaks only at q=0q=0q=0, $2\ensuremath{\pi}∕3$, and $4\ensuremath{\pi}∕3$, which are found to be couplings independent. The DMRG results of the zero-field static structure factor can be nicely fitted by a linear superposition of six modes, where two fitting equations are proposed. It is observed that the six modes are closely related to the low-lying excitations of the system. At finite temperatures, the magnetization, susceptibility, and specific heat show various behaviors for different couplings. The double-peak structures of the susceptibility, and specific heat against temperature are obtained, where the peak positions and heights are found to depend on the competition of the couplings. It is also uncovered that the XXZXXZXXZ anisotropy of F and AF couplings leads the system of case (c) to display quite different behaviors. In addition, the experimental data of the susceptibility, specific heat, and magnetization for the compound Cu3(CO3)2(OH)2{\mathrm{Cu}}_{3}{(\mathrm{C}{\mathrm{O}}_{3})}_{2}{(\mathrm{O}\mathrm{H})}_{2}Cu3​(CO3​)2​(OH)2​ are fairly compared with our TMRG results.
The low-dimensional quantum spin systems have been extensively studied in the past three decades due to the novel ground states and rich magnetic behaviors,especially the quantum spin chain with diamond topology structure. Motivated by recent experimental success in Cu3(CO3)2(OH)2 compound,which is regarded as a model material of spin-1/2 diamond chain,researchers have paid a lot of attention to various variants of diamond spin chains.In this paper,we mainly examine the magnetic properties of an antisymmetric spin-1/2 Ising-Heisenberg diamond chain with the secondneighbor interaction between nodal spins.By using exact diagonalization and transfer-matrix methods,the ground-state phase diagram,magnetization behavior and macroscopic thermodynamics are exactly solved for the particular case that all magnetic bonds yield antiferromagnetic couplings,which usually shows the most interesting magnetic features closely related to a striking interplay between geometric frustration and quantum fluctuations.To clearly illustrate the effect of second-neighbor interaction item,we consider a highly frustrated situation that all Ising-Heisenberg bonds and Heisenberg bonds possess the same interaction strength.The calculation results indicate that the second-neighbor interaction item will enrich ground states and magnetization plateaus.A classical ferrimagnetic phase FRI1 corresponding to a novel two-thirds of intermediate plateau with translationally broken symmetry is introduced,manifesting itself as up-up-up-down-up-up spin configuration at a ground-state.In addition,there are other four distinct ground states which can be identified from the phase diagram,i.e.,one saturated paramagnetic phase SP,one classical ferrimagnetic phase FRI2,one quantum ferrimagnetic phase QFI and the unique quantum antiferromagnetic phase QAF.The classical phase FRI2 and quantum phase QFI both generate one-third of magnetization plateau.It is worth mentioning that all the values of these magnetization plateaus satisfy the Oshikawa-Yamanaka-Affleck condition.Besides,the results also have shown a rich variety of temperature dependence of total magnetization and specific heat.The magnetization displays the remarkable thermal-induced changes as the external field is sufficiently close to critical value where two or more than two different ground states coexist.At the critical field relevant to a coexistence of two different states,the total magnetization displays a monotonic decrease trend.The thermal dependence of zero-field specific heat displays relative complex variations for different second-neighbor interactions between nodal spins.At first,the specific heat presents only a single rounded Schottky-type maximum.Using the second-neighbor interaction,another sharp peak arises at low-temperature and is superimposed on this round maximum,and the specific heat exhibits a double-peak structure. On further strengthening,the low-temperature one keeps its height shifting towards high temperature,while the hightemperature round peak suffers great enhancement and moves in an opposite direction.Finally,the low temperature peak entirely merges with the Schottky-type peak at a certain value of second-neighbor interaction,and above this value, the specific curve recovers its single peak structure.The observed double-peak specific heat curves mainly originate from thermal excitations between the ground-state spin configuration QAF and the ones close enough in energy to the ground state.
The magnetization process, the susceptibility, and the specific heat of the spin-1∕21∕21∕2 antiferromagnet (AF)-AF-ferromagnet (F) and F-F-AF trimerized quantum Heisenberg chains have been investigated by means of the transfer matrix renormalization group (TMRG) technique as well as the modified spin-wave (MSW) theory. A magnetization plateau at m=1∕6m=1∕6m=1∕6 for both trimerized chains is observed at low temperature. The susceptibility and the specific heat show various behaviors for different ferromagnetic and antiferromagnetic interactions and in different magnetic fields. The TMRG results of susceptibility and the specific heat can be nicely fitted by a linear superposition of double two-level systems, where two fitting equations are proposed. Three branch excitations, one gapless excitation and two gapful excitations, for both systems are found within the MSW theory. It is observed that the MSW theory captures the main characteristics of the thermodynamic behaviors at low temperatures. The TMRG results are also compared with the possible experimental data.
The exact solution of the distorted Ising-Hubbard model for a diamond chain is obtained by means of transfer matrix method. Based on this solution the magnetic, thermal and concurrence properties of the system are studied. We discuss in detail the ground state varying values of Ising and Hubbard interaction couplings, hopping amplitude, magnetic field, chemical potential and get paramagnetic, ferromagnetic, antiferromagnetic and ferrimagnetic phases of the system. Plateaus in magnetization curves and several-peak structures of the specific heat curve for different values of Hamiltonian parameters are obtained. The dependence of concurrence in Hubbard dimers from chain parameters, external magnetic field and temperature are studied.
Thermodynamic properties of a tetrameric bond-alternating Heisenberg spin chain with ferromagnetic-ferromagnetic-antiferromagnetic-antiferromagnetic exchange interactions are studied using the transfer-matrix renormalization group and compared to experimental measurements. The temperature dependence of the uniform susceptibility exhibits typical ferrimagnetic features. Both the uniform and staggered magnetic susceptibilities diverge in the limit $T\ensuremath{\rightarrow}0$, indicating that the ground state has both ferromagnetic and antiferromagnetic long-range orders. A double-peak structure appears in the temperature dependence of the specific heat. Our numerical calculation gives a good account for the temperature and field dependence of the susceptibility, the magnetization, and the specific heat for $\mathrm{Cu}{(3\text{\ensuremath{-}}\mathrm{Clpy})}_{2}{({\mathrm{N}}_{3})}_{2}$ $(3\text{\ensuremath{-}}\mathrm{Clpy}=3\text{\ensuremath{-}}\text{Chloroyridine})$.
The thermodynamic properties of a spin S=1/2S=1/2S=1/2 tetrameric Heisenberg antiferromagnetic chain with alternating interactions AF1-AF2-AF1-F{\text{AF}}_{1}{\text{-AF}}_{2}{\text{-AF}}_{1}\text{-F}AF1​-AF2​-AF1​-F (AF and F denote the antiferromagnetic and ferromagnetic couplings, respectively) are studied by means of the transfer-matrix renormalization-group method and Jordan-Wigner transformation. It is found that in the absence of magnetic field, the thermodynamic behaviors are closely related to the gapped low-lying excitations, and a novel structure with three peaks in the temperature dependence of specific heat is unveiled. In a magnetic field, a phase diagram in the temperature-field plane for the couplings satisfying JAF1=JAF2=JF{J}_{{\text{AF}}_{1}}={J}_{{\text{AF}}_{2}}={J}_{\text{F}}JAF1​​=JAF2​​=JF​ is obtained, in which various phases are identified. The temperature dependence of thermodynamic quantities including the magnetization, susceptibility, and specific heat are studied to characterize the corresponding phases. It is disclosed that the magnetization has a crossover behavior at low temperature in the Luttinger liquid phase, which is shown falling into the same class as that in the S=1S=1S=1 Haldane chain. In the plateau regime, the thermodynamic behaviors alter at a certain field, which results from the crossing of two excitation spectra. By means of the fermion mapping, it is uncovered that the system has four spectra from fermion and hole excitations that are responsible for the observed thermodynamic behaviors.