两种化合物的相变及磁性研究
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摘要
具有庞磁电阻(CMR)效应的Mn基钙钛矿氧化物所表现出的独特物理性质蕴藏着潜在的应用前景,而且,对庞磁电阻物理本质的认识涉及强关联物理中很多基础性问题,因此,这类氧化物一直是人们研究的热点。本论文主要目的是探讨Mn基钙钛矿氧化物中绝缘体一金属(I—M)转变和CMR效应可能的物理起因。虽然目前提出了很多不同的理论和模型,但是都不能对已有实验观察给予合理的解释。
在本文中,简单综述了钙钛矿结构Mn基氧化物的基本电特征和磁特征,并介绍了目前在一定程度上被人们所接受的用来解释Mn基氧化物中I—M转变和CMR效应起因的理论和模型,如基于双交换机理的唯象模型,电荷局域化模型,自旋—极化子模型以及基于相分离提出的二相唯象模型等。在文章中用渗流模型来计算Mn基钙钛矿氧化物中绝缘体—金属(I—M)转变温度T__(C,H)。关于渗流主要讨论了渗流的基本概念,渗流临界指数以及其中两个重要参数,渗流阈值和渗流几率的求取。详细介绍了随机阻抗网络模型的建立及求解方法,并用其模拟了两相系统的导电行为,并对这一结果用渗流理论求转变温度。作为模型中的参数,网格大小N和随机矩阵的生成方法,它们的改变对模型计算结果的影响也给予了详细的讨论。在对实验数据进行综合分析的基础上,提出Mn基钙钛矿氧化物在T_C附近发生动力学相分离的可能性,进而用蒙特卡罗方法生成了由PMI和FMM随机分布的阻抗网络。以此为基础提出的模型定性分析了Mn基钙钛矿氧化物中的主要实验特征,如高温顺磁绝缘体行为、低温铁磁金属性行为以及在居里温度T_C处发生的绝缘体到金属的转变。利用所建立的模型,对外加磁场下的电子输运行为也进行了模拟。结果表明,外加磁场使得I-M转变移向高温且转变附近电阻大幅度下降,从而导致T_(C,H)附近出现CMR现象。并且,随着外加磁场的增加,转变温度T_(C,H)呈线性增加。
自从诸如poly-BIPO,m-PDPC,p-NPNN等有机铁磁性聚合物的发现,基于低维纯有机聚合物或高分子的磁性材料引起了人们的广泛关注。聚合物,如m-PDPC等,在过去的研究中,已采用Kondo-Hubbard哈密顿量模型来描述该磁性系统,并且通过平均场近似和量子蒙特卡罗方法研究发现,该磁性系统的基态呈现铁磁磁有序。在本学位论文中,我们将选择有机聚合物poly-BIPO作为研究对象,并将其描述为准一维的Ising-Heisenberg型的“之”字型自旋链模型,并且采用有限温度的量子转移矩阵方法,对其热力学性质进行较系统的研究。由数值结果,我们发现:当侧自由基和主链间没有磁性耦合作用时,且主链内都为反铁磁相互作用,磁性系统的热容量随温度的变化表现为一个圆形的比热峰结构:但是,当主链的磁性耦合作用为铁磁一反铁磁交错耦合时,系统的热容量随温度的变化曲线表现为双峰结构,该行为的出现是来源于系统内铁磁激发和反铁磁激发之间的竞争。同时,在考虑侧基与主链间的相互作用时,如果主链内,以及主链和侧自由基的磁性相互作用都为反铁磁相互作用时,该系统的热容量仍然只表现为一个圆形的比热峰;但如果,主链的磁性耦合作用为反铁磁相互作用,而侧基与主链间的磁性耦合为铁磁相互作用,该磁性系统将表现为清晰的比热双峰结构,其仍然来源于系统铁磁和反铁磁激发之间的竞争,同时,比热双峰的出现意味系统的亚铁磁磁有序的存在。
Colossal magnetoresistive (CMR) materials such as rare-earth manganites is still a hot topic up to now. For one thing, scientists are looking forward to potential applications for their CMR effect; for another, the essence of the CMR is related to the basic issues in strongly correlated physics. The main purpose of this paper is to study in details the possible origin of insulator-metal (I-M) transition and CMR effect found in manganese perovskite. Up to now, there are many different theories and models trying to explain this phenomenon but no one can provide a feasible explanation.
In this paper, the electrical and magnetic characters of manganese perovskite have been briefly summarized. Some theories and models introduced here also include phenomenon model based on double exchange theory, charge ordering model, spin-polarons model and 2-phase phenomenon model based on phase separation.The I-M transition temperature T_(c,h) in different magnetic fields has been obtained in the paper. The content about percolation includes the concept of percolation, critical percolation exponent and percolation probability about random resistor network model. The method of constructing model and calculating model resistance is presented here in details. The simulated result of the system through percolation theory is also discussed. Clearly, with the different parameters, just like the size of network and the generating method of random matrix, the model will give different result. Based on the analysis on experiment data, it is proposed that there is possibility of kinetic PS near T_c in manganese perovskite oxide. Thus, a random resistor network consisted of PMI and FMM is generated through Monte Carlo method. The model qualitatively analyses the main character of manganese perovskite which is PMI at high temperature, FMM at low temperature and insulator transiting to metal near Curie temperature. The model also simulates electrical transport behavior of sample when applied magnetic field and the result shows that I-M transition moves to high temperature and resistance near T_c falls sharply because of field. It is found there is linear dependence of the critical temperature on the magnetic field, provided the magnetic field is not too strong. The theoretical predications coincide well with the result of experiments.
In addition, low-dimensional magnetism in organic polymers or molecules has attracted considerable interest from scientists since the discovery of ferromagnetism in organic polymer, such as poly-BIPO, m-PDPC, p-NPNN. The polymer chain, m-PDPC, is described by the Kondo-Hubbard Hamiltonian, which exhibits the ferromagnetic order by means of the mean-field theory and the quantum Monte Carlo simulation. In the present paper, we choose poly-BIPO and describe it as a simplified quasi-one- dimensional Ising-Heisenberg zig-zag spin chain model, and then we apply the quantum transfer-matrix method to study the specific heat of which. From the calculated results, we can find that, in the absence of the exchange interactions between side radicals and the main chain, the curves of specific heat show a round peak due to the antiferromagnetic excitations for the all antiferromagnetic interactions along the polymer chain, and considering the exchange interactions between the side radicals and the main chain, the curves of the specific heat show double-peak structure for ferromagnetic interactions between the radicals and main chain, indicating a competition between ferromagnetic and antiferromagnetic interactions and the possibility of the occurrence of the stable ferrimagnetic state along the polymer chain.
在本文中,简单综述了钙钛矿结构Mn基氧化物的基本电特征和磁特征,并介绍了目前在一定程度上被人们所接受的用来解释Mn基氧化物中I—M转变和CMR效应起因的理论和模型,如基于双交换机理的唯象模型,电荷局域化模型,自旋—极化子模型以及基于相分离提出的二相唯象模型等。在文章中用渗流模型来计算Mn基钙钛矿氧化物中绝缘体—金属(I—M)转变温度T__(C,H)。关于渗流主要讨论了渗流的基本概念,渗流临界指数以及其中两个重要参数,渗流阈值和渗流几率的求取。详细介绍了随机阻抗网络模型的建立及求解方法,并用其模拟了两相系统的导电行为,并对这一结果用渗流理论求转变温度。作为模型中的参数,网格大小N和随机矩阵的生成方法,它们的改变对模型计算结果的影响也给予了详细的讨论。在对实验数据进行综合分析的基础上,提出Mn基钙钛矿氧化物在T_C附近发生动力学相分离的可能性,进而用蒙特卡罗方法生成了由PMI和FMM随机分布的阻抗网络。以此为基础提出的模型定性分析了Mn基钙钛矿氧化物中的主要实验特征,如高温顺磁绝缘体行为、低温铁磁金属性行为以及在居里温度T_C处发生的绝缘体到金属的转变。利用所建立的模型,对外加磁场下的电子输运行为也进行了模拟。结果表明,外加磁场使得I-M转变移向高温且转变附近电阻大幅度下降,从而导致T_(C,H)附近出现CMR现象。并且,随着外加磁场的增加,转变温度T_(C,H)呈线性增加。
自从诸如poly-BIPO,m-PDPC,p-NPNN等有机铁磁性聚合物的发现,基于低维纯有机聚合物或高分子的磁性材料引起了人们的广泛关注。聚合物,如m-PDPC等,在过去的研究中,已采用Kondo-Hubbard哈密顿量模型来描述该磁性系统,并且通过平均场近似和量子蒙特卡罗方法研究发现,该磁性系统的基态呈现铁磁磁有序。在本学位论文中,我们将选择有机聚合物poly-BIPO作为研究对象,并将其描述为准一维的Ising-Heisenberg型的“之”字型自旋链模型,并且采用有限温度的量子转移矩阵方法,对其热力学性质进行较系统的研究。由数值结果,我们发现:当侧自由基和主链间没有磁性耦合作用时,且主链内都为反铁磁相互作用,磁性系统的热容量随温度的变化表现为一个圆形的比热峰结构:但是,当主链的磁性耦合作用为铁磁一反铁磁交错耦合时,系统的热容量随温度的变化曲线表现为双峰结构,该行为的出现是来源于系统内铁磁激发和反铁磁激发之间的竞争。同时,在考虑侧基与主链间的相互作用时,如果主链内,以及主链和侧自由基的磁性相互作用都为反铁磁相互作用时,该系统的热容量仍然只表现为一个圆形的比热峰;但如果,主链的磁性耦合作用为反铁磁相互作用,而侧基与主链间的磁性耦合为铁磁相互作用,该磁性系统将表现为清晰的比热双峰结构,其仍然来源于系统铁磁和反铁磁激发之间的竞争,同时,比热双峰的出现意味系统的亚铁磁磁有序的存在。
Colossal magnetoresistive (CMR) materials such as rare-earth manganites is still a hot topic up to now. For one thing, scientists are looking forward to potential applications for their CMR effect; for another, the essence of the CMR is related to the basic issues in strongly correlated physics. The main purpose of this paper is to study in details the possible origin of insulator-metal (I-M) transition and CMR effect found in manganese perovskite. Up to now, there are many different theories and models trying to explain this phenomenon but no one can provide a feasible explanation.
In this paper, the electrical and magnetic characters of manganese perovskite have been briefly summarized. Some theories and models introduced here also include phenomenon model based on double exchange theory, charge ordering model, spin-polarons model and 2-phase phenomenon model based on phase separation.The I-M transition temperature T_(c,h) in different magnetic fields has been obtained in the paper. The content about percolation includes the concept of percolation, critical percolation exponent and percolation probability about random resistor network model. The method of constructing model and calculating model resistance is presented here in details. The simulated result of the system through percolation theory is also discussed. Clearly, with the different parameters, just like the size of network and the generating method of random matrix, the model will give different result. Based on the analysis on experiment data, it is proposed that there is possibility of kinetic PS near T_c in manganese perovskite oxide. Thus, a random resistor network consisted of PMI and FMM is generated through Monte Carlo method. The model qualitatively analyses the main character of manganese perovskite which is PMI at high temperature, FMM at low temperature and insulator transiting to metal near Curie temperature. The model also simulates electrical transport behavior of sample when applied magnetic field and the result shows that I-M transition moves to high temperature and resistance near T_c falls sharply because of field. It is found there is linear dependence of the critical temperature on the magnetic field, provided the magnetic field is not too strong. The theoretical predications coincide well with the result of experiments.
In addition, low-dimensional magnetism in organic polymers or molecules has attracted considerable interest from scientists since the discovery of ferromagnetism in organic polymer, such as poly-BIPO, m-PDPC, p-NPNN. The polymer chain, m-PDPC, is described by the Kondo-Hubbard Hamiltonian, which exhibits the ferromagnetic order by means of the mean-field theory and the quantum Monte Carlo simulation. In the present paper, we choose poly-BIPO and describe it as a simplified quasi-one- dimensional Ising-Heisenberg zig-zag spin chain model, and then we apply the quantum transfer-matrix method to study the specific heat of which. From the calculated results, we can find that, in the absence of the exchange interactions between side radicals and the main chain, the curves of specific heat show a round peak due to the antiferromagnetic excitations for the all antiferromagnetic interactions along the polymer chain, and considering the exchange interactions between the side radicals and the main chain, the curves of the specific heat show double-peak structure for ferromagnetic interactions between the radicals and main chain, indicating a competition between ferromagnetic and antiferromagnetic interactions and the possibility of the occurrence of the stable ferrimagnetic state along the polymer chain.
引文
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