外延应变和铁电极化双重调控LaMnO3/BaTiO3超晶格的磁性

对钙钛矿锰氧化物的磁性进行调控在科学上具有重要意义,在自旋电子学领域更是有紧迫需求.利用外延应变和铁电极化双重调控超晶格材料的磁性不但更加接近体系的真实状态,而且能诱导出丰富的物理性质.本文采用第一性原理计算,系统地研究了外延应变和铁电极化对LaMnO₃/BaTiO₃超晶格磁性的鲁棒控制.通过精确调控Mn原子磁矩的大小和方向,实现了铁磁?反铁磁?亚铁磁之间的可逆转变,同时产生了强烈的磁电耦合效应.除此之外,本文在超晶格中实现了铁电极化和金属性共存.通过分析Jahn-Teller效应,氧八面体旋转、倾斜以及体系内部电子转移对磁性的影响,揭示了磁性调控的物理机制.研究结果不但对系统地了解LaMnO₃体系的磁性变化具有重要意义,而且可以为设计基于钙钛矿锰氧化物的自旋电子器件提供理论指导.     

B,P掺杂β-Si3N4的电子结构和光学性质研究

运用第一性原理方法, 计算了B, P两种元素单掺杂和共掺杂的β -Si₃N₄材料的电子结构和光学性质. 结果表明: B掺杂体系的稳定性更高, 而P掺杂体系的离子性更强; 单掺和共掺杂均窄化带隙, 且共掺在禁带中引入深能级, 使局域态增强; 单掺杂体系介电函数虚部、吸收谱和能量损失谱各峰均发生红移、幅值减小, 而共掺后介电函数虚部主峰出现蓝移、能量损失峰展宽、高能区电子跃迁大大增强, 且控制共掺杂的B, P比例可获得较低的带电缺陷浓度.     

新型钙钛矿铜氧材料Sr8 CaRe3 Cu4 O24的亚铁磁和轨道有序性质

用密度泛函理论和格林函数方法研究了新型钙钛矿铜氧材料Sr8CaRe3Cu44O24的电子结构和磁性性质.所得结果与实验符合得很好,表明这种材料是绝缘体,每个元胞有1.0μB的磁矩.磁矩主要在Cu原子上,相邻Cu原子上的磁矩反平行排列.非磁的Re原子使得Cu上的d轨道有序排列,这导致这种材料有很高的居里温度(TC≈440K).基于密度泛函的结果,用海森伯模型描述了材料的电子自旋自由度,并用格林函数方法研究了材料有限温度下的磁性行为,所得结果和实验一致,表明自旋为1和自旋为1/2磁矩交错排列的海森伯模型可很好地描述这种材料的磁性性质.     

Fe:LiNbO3和(Fe,Tb):LiNbO3晶体中入射光强

用一种新的测量方法在不同入射光强下同时观测了Fe:LiNbO3和(Fe,Tb):LiNbO3晶体中光致折射率变化Δns、吸收系数α和光电导σph与入射光强I的依赖关系, 并从理论上对观测结果给予了初步解释。     

磁性形状记忆合金Mn2NiGa band Jahn-Teller效应的第一性原理研究

运用第一性原理的方法,研究了磁性形状记忆合金Mn₂NiGa在马氏体相变中晶格结构、磁结构、Mn原子d电子结构的变化.研究表明,伴随Mn₂NiGa马氏体相变的发生,形成了一个由两根长键及四根短键组成的拉长八面体结构,即产生了沿z轴拉长的Jahn-Teller畸变;在相变时,位于八面体中心的Mn原子的磁矩发生显著的变化,而作为配体的Ni、Ga原子的磁矩变化很微小;Jahn-Teller畸变的发生,是由于晶体的畸变使配住场产生变化,导致Mn原子d电子态密度重新分布,从而使e_g和t_2g能级分裂所致.     

Heusler合金Mn2NiGe马氏体相变的带Jahn-Teller效应研究

运用第一性原理的方法,计算磁性形状记忆合金Mn₂NiGe的晶体结构、磁结构、电子结构在马氏体相变中的变化.结果表明:Mn₂NiGe在发生马氏体相变时,产生了c轴拉长而a和b轴缩短的Jahn-Teller畸变,形成一个由两根长键和四根短键组成的拉长的八面体;伴随Jahn-Teller畸变,处于八面体中心的Mn离子的磁矩发生了显著的变化,而作为配体的Ni和Ge离子的磁矩基本不变;Jahn-Teller效应中Mn离子的e_g和t_2g能级的分裂,源自于晶体畸变所产生的配位场的改变,导致Mn离子d电子态密度的重新分布,从而在费米能级两侧打开一个赝能隙.     

La0.2Ca0.8MnO3材料电荷有序转变附近弹性模量的研究

通过超声与低频切变模量测量,得到多晶锰氧化物La0.2Ca0.8MnO3材料纵向模量与切变模量随温度变化关系曲线,发现在电荷有序转变温度附近,纵向模量与切变模量都出现最小值.运用合作Jahn-Teller效应理论对实验数据进行了拟合,发现理论与实验曲线符合较好,表明Jahn-Teller效应是发生电荷有序状态转变的主要机制之一.     

用SiCl4/H2气源沉积多晶硅薄膜光照稳定性的研究

对以SiH₄/H₂及SiCl₄/H₂为源气体、采用 等离子体增强化学气相沉积技术制备的非晶硅薄膜和多晶硅薄膜进行了光照稳定性的研究.实验表明，制备的多晶硅薄膜并没有出现 非晶硅中的光致衰减现象，其光电导、暗电导在光照过程中没有下降反而有所上升且电导率 变化快慢受氢稀释度的制约.多晶硅薄膜的光照稳定性可能来源于高的晶化度及Cl元素的存在. 关键词： 多晶硅薄膜 稳恒光电导效应 晶界 光致衰退效应     

Fe3GeTe2/h-BN/石墨烯二维异质结器件中的高效率自旋注入

最近,二维铁磁材料的发现加速了自旋电子学在超低功耗电子器件方面的应用.其中, Fe₃GeTe₂通过实验调控,比如界面层间耦合和离子液体调控,可以使其居里温度达到室温,具有广泛的应用前景.本文基于密度泛函理论与非平衡格林函数方法,研究了Fe₃GeTe₂/石墨烯二维异质结在有无氮化硼作隧穿层情况下的输运性质.结果表明:当Fe₃GeTe₂/石墨烯之间为透明接触时,由于电子轨道杂化,在±0.1 V偏压下可以实现有效的自旋注入.通过加入氮化硼作为隧穿层,则可以在更宽偏压范围[–0.3 V, 0.3 V]内实现高效自旋隧穿注入;并且,由于Fe₃GeTe₂与石墨烯电子态在布里渊区的空间匹配程度取决于电子自旋方向,相应出现的自旋过滤效应导致了接近100%的自旋极化率.这些研究结果有望推动二维全自旋逻辑以及相关超低功耗自旋电子器件的发展.     

应变和电场对Ga2SeTe/In2Se3异质结电子结构和光学性质的影响

异质结构的构筑与堆垛是新型二维材料物性调控及应用的有效策略.基于密度泛函理论的第一性原理计算,本文研究了4种不同堆叠构型的新型二维Janus Ga₂SeTe/In₂Se₃范德瓦耳斯异质结的电子结构和光学性质. 4种异质结构型均为Ⅱ型能带结构的间接带隙半导体,光致电子的供体和受体材料由二维In₂Se₃的极化方向决定.光吸收度在可见光区域高达25%,有利于太阳可见光的有效利用.双轴应变可诱导直接-间接带隙转变,外加电场能有效调控异质结构带隙,使AA2叠加构型的带隙从0.195 eV单调增大到0.714 eV,AB2叠加构型的带隙从0.859 eV单调减小到0.058 eV,两种调控作用下异质结的能带始终保持Ⅱ型结构.压缩应变作用下的异质结在波长较短的可见光区域表现出更优异的光吸收能力.这些研究结果揭示了Janus Ga₂SeTe/In₂Se₃范德瓦耳斯异质结电子结构的调控机理,为新型光电器件的设计提供理论指导.     

Roles of Electron Hopping on Orbital Ordering for Vanadium Spinels

We investigate the orbital ordering quantitatively for the spinel systems RV 2 O 4(R=Mg,Zn,Cd) in the viewpoint of single-ion physics through the method of diagonalization.Through the quantitative calculation,it is found that the spin-orbit(SO)coupling and the Jahn-Teller(JT) effect enable the orbital ordering under the conditions of negligible electron hopping among different V 3+ sites.For the systems RV 2 O 4,the electron hopping is implied to be observable from the energy gap in conductivity,so the orbital ordering of RV 2 O 4 cannot be induced by the SO coupling and JT effect at definite temperature,which is on contrary to the conclusions in [Phys.Rev.Lett.93(2004) 157206].     

Roles of Electron Hopping on Orbital Ordering for Vanadium Spinels

We investigate the orbital ordering quantitatively for the spinel systems RV₂O₄ (R=Mg, Zn, Cd) in the viewpoint of single-ion physics through the method of diagonalization. Through the quantitative calculation, it is found that the spin-orbit (SO)coupling and the Jahn-Teller (JT) effect enable the orbital ordering under the conditions of negligible electron hopping among different V³⁺ sites. For the systems RV₂O₄, the electron hopping is implied to be observable from the energy gap in conductivity, so the orbital ordering of RV₂O₄ cannot be induced by the SO coupling and JT effect at definite temperature, which is on contrary to the conclusions in [Phys. Rev. Lett. 93 (2004) 157206].     

Tuning charge and orbital ordering in DyNiO3 by biaxial strain

The first-principles calculations were used to explore the tunable electronic structure in DyNiO₃ (DNO) under the effects of the biaxial compressive and tensile strains. We explored how the biaxial strain tunes the orbital hybridization and influences the charge and orbital ordering states. We found that breathing mode and Jahn-Teller distortion play a primary role in charge ordering state and orbital ordering state, respectively. Additionally, the calculated results revealed that the biaxial strain has the ability to manipulate the phase competition between the two states. A phase transition point has been found under tensile train. If the biaxial train is larger than the point, the system favors orbital ordering state. If the strain is smaller than the point, the system is in charge ordering state favorably.     

Different effects of Ce-doping on orbital and spin ordering in perovskite vanadate Sm_(1-χ)Ce_χ VO_3

The effects of Ce-doping on the phase transition of the orbital/spin ordering (OO/SO) are studied through the structural, magnetic, and electrical transport measurements of perovskite vanadate Sm1 x Ce x VO 3 . The measurements of structure show that the cell volume decreases as x≤ 0.05, and then increases as Ce-doping level increases further. The OO state exists but is suppressed progressively in the sample with x≤0.2 and disappears as x0.2. The temperature at which the C-type SO transition is present increases monotonically with Ce-doping level increasing. The temperature dependence of resistivity for each of the samples shows a semiconducting transport behavior and the transport can be well described by the thermal activation model. The activation energy first decreases as x ≤0.2, and then increases for further doping. The obtained results are discussed in terms of the mixed-valent state of the doped-Ce ions.     

Ba0.5Sr0.5TiO3电子结构和光学性质的第一性原理研究

利用第一性原理研究了Ba_0.5Sr_0.5TiO₃的能带结构和光学性质.结果表明,导带和价带都来源于钛原子3d轨道和氧原子2p轨道的杂化.导带主要由钛原子的3d轨道贡献,价带主要由氧原子的2p轨道贡献.吸收系数为10⁵ cm^-1量级,且吸收主要集中在低能区.折射率为n（0）=2.1,结果与实验符合. 关键词： 第一性原理 能带结构 光学性质     

轨道序对半掺杂锰氧化物光学性质的影响

在两轨道双交换模型基础上，讨论了电子关联作用对半掺杂锰氧化物轨道序的影响，推导出能计算各个相的光电导公式.结果显示，光吸收与轨道序之间存在关联现象.对于铁磁相，当格点库仑相互作用(U)从无到有逐渐增加时，铁磁相会从无轨道序过渡到有轨道序，相变前 后非相干光吸收有一个从无能隙到有能隙的明显变化.对于层状反铁磁的A相，U的增加会使 轨道序更明显，非相干光吸收部分的能隙随之也增大. 关键词： 轨道序 光电导 锰氧化物 库仑相互作用     

Magnetic order driven by orbital ordering in the semiconducting KFe1.5Se2

The two-orbital Hubbard model is studied numerically by using the Hartree-Fock approximation in both real space and momentum space, and the ground-state properties of the alkali metal iron selenide semiconducting KFe_1.5Se₂ are investigated. A rhombus-type Fe vacancy order with stripetype antiferromagnetic (AFM) order is found, as was observed in neutron scattering experiments [J. Zhao, et al., Phys. Rev. Lett. 109, 267003 (2012)]. Hopping parameters are obtained by fitting the experimentally observed stripe AFM phase in real space. These hopping parameters are then used to study the ground-state properties of the semiconductor in momentum space. It is found to be a strongly correlated system with a large on-site Coulomb repulsion U, similar to the AFM Mott insulator — the parent compound of copper oxide superconductors. We also find that the electronic occupation numbers and magnetizations in the d_xz and d_yz orbitals become different simultaneously when U>U_c (～3.4 eV), indicating orbital ordering. These results imply that the rotational symmetry between the two orbitals is broken by orbital ordering and thus drives the strong anisotropy of the magnetic coupling that has been observed by experiments and that the stripe-type AFM order in this compound may be caused by orbital ordering together with the observed large anisotropy.     

Charge ordering characteristics in Y0.5Ca0.5MnO3 manganite

The charge ordering characteristics in Y_0.5Ca_0.5MnO₃ manganite, prepared by sol–gel process, have been investigated experimentally. It is found that the superlattice diffractions appear in the electron diffraction patterns recorded at low temperatures, while only basic Brag diffraction spots can be observed when temperature is higher than 300 K. This provides direct evidence for the existence of charge ordering in Y_0.5Ca_0.5MnO₃. The magnetization and specific heat measurements indicate the charge ordering temperature of Y_0.5Ca_0.5MnO₃ is 290 K, around which both the magnetization and specific heat reveal anomalous behaviors. We also observed that the MnO bond length changed remarkably and the effective number of carriers reduced prominently with decreasing temperature around charge ordering temperature through transform infrared spectra measurements.     

Sr掺杂对La_(1-x)Sr_xMnO_3/LaAlO_3/SrTiO_3界面电子结构的影响

采用基于密度泛函理论的第一性原理计算方法,系统地研究了La_(1-x)Sr_xMnO_3层中Sr的掺杂方式和掺杂量对4La_(1-x)Sr_xMnO_3/3LaAlO_3/4SrTiO_3(LSMO/LAO/STO)异质结构原子和电子结构的影响.结果表明:对于相同的Sr掺杂量,掺杂方式的差异对体系电子结构的影响微弱,不会导致体系发生金属-绝缘体转变;掺杂量的不同对体系电子结构有着显著的影响,当Sr的掺杂量较少时,LAO/STO界面处存在着准二维电子气,当Sr的掺杂量高于1/3时,LAO/STO界面处准二维电子气消失.我们相信,Sr的引入以及通过Sr掺杂量的改变可以对LSMO覆盖层极化进行调控,这也是导致体系LAO/STO界面处金属-绝缘体转变的可能原因,进一步为极化灾变机制导致的界面处电子重构提供了证据.     

正交相Fe2(MoO4)3的制备与表征及其负膨胀行为的第一性原理研究

采用水热合成法制备出Fe₂(MoO₄)₃样品, 并用高温X-射线衍射、热重和差示扫描量热同步热分析仪对其进行表征, 发现样品在510 ℃附近发生低温单斜相和高温正交相之间的可逆相变, 且正交相表现出负膨胀特征. 采用第一性原理计算了正交相Fe₂(MoO₄)₃ 的原子、电子结构以及声子谱、声子态密度, 并和可获得的实验结果进行了系统的比较. 结果显示正交相Fe₂(MoO₄)₃中MoO₄四面体较之FeO₆八面体具有更强的刚性. 发现最低频的光学支处具有最负的格林乃森(Grüneisen)系数, MoO₄四面体和FeO₆ 八面体相连的桥氧原子的横向振动、FeO₆八面体柔性扭曲转动以及MoO₄四面体的刚性翻转共同导致了Fe₂(MoO₄)₃负膨胀现象的发生.