Mn掺杂SnO_2中铁磁耦合机理研究
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摘要
稀磁半导体由于在自旋电子学领域具有潜在的应用价值,受到人们广泛地关注。而稀磁半导体中铁磁性的来源一直是困扰人们的问题,其中晶体缺陷及载流子是影响稀磁半导体铁磁性的两个主要因素。本论文主要研究了载流子对Mn掺杂SnO_2稀磁半导体铁磁性的影响,主要工作概括如下:
利用固相反应法制备了Sn_(1-x)Mn_xO_2 (x = 0.01, 0.03, 0.05),Sn_(1-x-y)Mn_xSb_yO_2 (x = 0.01, 0.03; y = 0, 0.005, 0.02, 0.04)和Sn_(1-x-z)Mn_xCu_zO_2 (x = 0.01, 0.03, 0.05; z = 0.005, 0.02)多晶样品。利用X射线衍射仪(XRD)、X射线光电子能谱(XPS)和物理性质测试系统(PPMS)对样品的结构、价态、电输运性质和磁性质进行了系统的研究。
多晶Sn_(1-x-y)Mn_xSb_yO_2系列样品呈现出单一金红石结构,没有杂相生成,随着Sb含量的增加,晶胞体积增大,铁磁性减弱。对于x = 0.03的样品,居里温度由未掺杂Sb (y = 0)时的27 K减小到26.5 K (y = 0.005),当掺杂量y≥0.02时,样品表现出顺磁性。而Sb的掺杂量为y = 0.04时,由于样品中Sb~(5+)离子代替SnO_2中Sn~(4+)离子而产生大量电子,导致样品导电性显著增强。
为进一步研究空穴在铁磁耦合中的作用,我们在Sn_(1-x)Mn_xO_2中共掺杂Cu元素。电输运测量表明所有Sn_(1-x-z)Mn_xCu_zO_2样品在室温均为绝缘体,而随着Cu含量的增加样品的铁磁性呈现出增强趋势:对于x = 0.03系列样品,少量Cu掺杂(z = 0.005)时居里温度上升到30.5 K;随着Cu含量进一步增加到2 %时,居里温度增加到40.0 K。
上述Sb和Cu掺杂Sn_(1-x)Mn_xO_2中的磁性可以用束缚磁极化子模型解释:在Sn_(1-x)Mn_xO_2样品中,Mn~(3+)代替样品中Sn~(4+)离子产生局域化的空穴,周围的Mn~(3+)以局域化的空穴为中心形成束缚磁极化子,极化子间有效半径发生交叠产生铁磁相互作用。当体系中掺入Sb后,Sb~(5+)代替Sn~(4+)产生自由电子补偿掉样品中局域化的空穴,减少了样品中束缚磁极化子数目,导致铁磁性减弱。而当体系中掺入Cu后,Cu~(2+)代替SnO_2晶格中Sn~(4+)产生新的局域化空穴,增多的空穴与邻近的Mn~(3+)离子形成新的束缚磁极化子,从而使样品的铁磁性增强。
Diluted magnetic semiconductors (DMSs) have become a focus of considerable interests in recent years due to their potential application in the new field of research and application known as spintronics. However, the origin of the ferromagnetism challenges the researcher’s understanding of magnetic order in solids. In this thesis, we have investigated the influence of charge carrier on the structural, magnetic and electrical properties of Sb and Cu doped Sn_(1-x)Mn_xO_2. The main results are generalized as follows.
Sn_(1-x)Mn_xO_2 (x = 0.01, 0.03, 0.05), Sn_(1-x-y)Mn_xSb_yO_2 (x = 0.01, 0.03; y = 0, 0.005, 0.02, 0.04), Sn_(1-x-z)Mn_xCu_zO_2 (x = 0.01, 0.03, 0.05; z = 0.005, 0.02) polycrystalline samples were prepared by a solid-state reaction method. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and physical property measurement system (PPMS) were used to measure the crystal structure, the chemical binding state, the electrical properties and the magnetic properties, respectively.
It is found that all Sn_(1-x-y)Mn_xSb_yO_2 samples are crystallized in single phase with a rutile structure which is the characteristic of SnO_2. The lattice expansion and reducing ferromagnetism are observed with increasing Sb concentration. In particular, at a fixed Mn composition of x = 0.03, it is found that the ferromagnetic behaviors observed in undoped Sn0.97Mn0.03O_2 are suppressed due to the antimony doping; and the resistivity decreased drastically with Sb concentration up to 0.04 in Sn0.97-yMn0.03SbyO_2. Combined with all the results, we conclude that the ferromagnetic interaction between Mn~(3+) ions is destroyed by the mobile charge electrons which are introduced by Sb~(5+) substitution for Sn~(4+).
To investigate the role of hole in ferromagnetism, Cu is co-doped into the Sn_(1-x)Mn_xO_2. It is found that the doping of copper, which acts as Cu~(2+) in SnO_2, brings significant enhancement of the ferromagnetism in Sn_(1-x)Mn_xO_2, while the samples remain electrical insulating. In particular, at a fixed Mn composition of x = 0.03, Curie temperature (TC) increases up to 40.0 K at Cu concentration z = 0.02 from TC = 27.0 K at undoped Sn0.97Mn0.03O_2.
The observed ferromagnetism in Mn-doped SnO_2 is discussed on the basis of the formation of bound magnetic polarons (BMP): a BMP consists of a localized hole and many Mn~(3+) ions around the localized center, the overlapping and interaction of neighboring BMPs produce long-range ferromagnetic coupling. In Sn_(1-x-y)Mn_xSb_yO_2, the localized holes will be compensated by the electrons introduced by the Sb doping, which will induce a decrease of the concentration of BMPs and suppression of the ferromagnetism. For the Cu doped Sn0.97Mn0.03O_2, the concentration of localized hole will be increased by substituting Cu~(2+) for Sn~(4+), which would introduce more BMPs with the proximate Mn, hence the ferromagnetism are enhanced.
利用固相反应法制备了Sn_(1-x)Mn_xO_2 (x = 0.01, 0.03, 0.05),Sn_(1-x-y)Mn_xSb_yO_2 (x = 0.01, 0.03; y = 0, 0.005, 0.02, 0.04)和Sn_(1-x-z)Mn_xCu_zO_2 (x = 0.01, 0.03, 0.05; z = 0.005, 0.02)多晶样品。利用X射线衍射仪(XRD)、X射线光电子能谱(XPS)和物理性质测试系统(PPMS)对样品的结构、价态、电输运性质和磁性质进行了系统的研究。
多晶Sn_(1-x-y)Mn_xSb_yO_2系列样品呈现出单一金红石结构,没有杂相生成,随着Sb含量的增加,晶胞体积增大,铁磁性减弱。对于x = 0.03的样品,居里温度由未掺杂Sb (y = 0)时的27 K减小到26.5 K (y = 0.005),当掺杂量y≥0.02时,样品表现出顺磁性。而Sb的掺杂量为y = 0.04时,由于样品中Sb~(5+)离子代替SnO_2中Sn~(4+)离子而产生大量电子,导致样品导电性显著增强。
为进一步研究空穴在铁磁耦合中的作用,我们在Sn_(1-x)Mn_xO_2中共掺杂Cu元素。电输运测量表明所有Sn_(1-x-z)Mn_xCu_zO_2样品在室温均为绝缘体,而随着Cu含量的增加样品的铁磁性呈现出增强趋势:对于x = 0.03系列样品,少量Cu掺杂(z = 0.005)时居里温度上升到30.5 K;随着Cu含量进一步增加到2 %时,居里温度增加到40.0 K。
上述Sb和Cu掺杂Sn_(1-x)Mn_xO_2中的磁性可以用束缚磁极化子模型解释:在Sn_(1-x)Mn_xO_2样品中,Mn~(3+)代替样品中Sn~(4+)离子产生局域化的空穴,周围的Mn~(3+)以局域化的空穴为中心形成束缚磁极化子,极化子间有效半径发生交叠产生铁磁相互作用。当体系中掺入Sb后,Sb~(5+)代替Sn~(4+)产生自由电子补偿掉样品中局域化的空穴,减少了样品中束缚磁极化子数目,导致铁磁性减弱。而当体系中掺入Cu后,Cu~(2+)代替SnO_2晶格中Sn~(4+)产生新的局域化空穴,增多的空穴与邻近的Mn~(3+)离子形成新的束缚磁极化子,从而使样品的铁磁性增强。
Diluted magnetic semiconductors (DMSs) have become a focus of considerable interests in recent years due to their potential application in the new field of research and application known as spintronics. However, the origin of the ferromagnetism challenges the researcher’s understanding of magnetic order in solids. In this thesis, we have investigated the influence of charge carrier on the structural, magnetic and electrical properties of Sb and Cu doped Sn_(1-x)Mn_xO_2. The main results are generalized as follows.
Sn_(1-x)Mn_xO_2 (x = 0.01, 0.03, 0.05), Sn_(1-x-y)Mn_xSb_yO_2 (x = 0.01, 0.03; y = 0, 0.005, 0.02, 0.04), Sn_(1-x-z)Mn_xCu_zO_2 (x = 0.01, 0.03, 0.05; z = 0.005, 0.02) polycrystalline samples were prepared by a solid-state reaction method. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and physical property measurement system (PPMS) were used to measure the crystal structure, the chemical binding state, the electrical properties and the magnetic properties, respectively.
It is found that all Sn_(1-x-y)Mn_xSb_yO_2 samples are crystallized in single phase with a rutile structure which is the characteristic of SnO_2. The lattice expansion and reducing ferromagnetism are observed with increasing Sb concentration. In particular, at a fixed Mn composition of x = 0.03, it is found that the ferromagnetic behaviors observed in undoped Sn0.97Mn0.03O_2 are suppressed due to the antimony doping; and the resistivity decreased drastically with Sb concentration up to 0.04 in Sn0.97-yMn0.03SbyO_2. Combined with all the results, we conclude that the ferromagnetic interaction between Mn~(3+) ions is destroyed by the mobile charge electrons which are introduced by Sb~(5+) substitution for Sn~(4+).
To investigate the role of hole in ferromagnetism, Cu is co-doped into the Sn_(1-x)Mn_xO_2. It is found that the doping of copper, which acts as Cu~(2+) in SnO_2, brings significant enhancement of the ferromagnetism in Sn_(1-x)Mn_xO_2, while the samples remain electrical insulating. In particular, at a fixed Mn composition of x = 0.03, Curie temperature (TC) increases up to 40.0 K at Cu concentration z = 0.02 from TC = 27.0 K at undoped Sn0.97Mn0.03O_2.
The observed ferromagnetism in Mn-doped SnO_2 is discussed on the basis of the formation of bound magnetic polarons (BMP): a BMP consists of a localized hole and many Mn~(3+) ions around the localized center, the overlapping and interaction of neighboring BMPs produce long-range ferromagnetic coupling. In Sn_(1-x-y)Mn_xSb_yO_2, the localized holes will be compensated by the electrons introduced by the Sb doping, which will induce a decrease of the concentration of BMPs and suppression of the ferromagnetism. For the Cu doped Sn0.97Mn0.03O_2, the concentration of localized hole will be increased by substituting Cu~(2+) for Sn~(4+), which would introduce more BMPs with the proximate Mn, hence the ferromagnetism are enhanced.
引文
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