Dy在Nd2Fe14B晶格中的占位及其对Fe原子磁矩影响的第一性原理计算

基于第一性原理投影缀加波和梯度矫正局域密度近似(PAW-GGA), 研究了Nd₂Fe₁₄B和Dy₂Fe₁₄B的基态晶格属性, 进而对Dy在Nd₂Fe₁₄B晶格中的掺杂进行了研究, 并采用GGA+U的方式进行了原子磁矩计算, 并与自旋轨道耦合 (SOI) 计算结果进行了对照. 置换计算表明, Dy原子倾向于置换Nd₂Fe₁₄B晶格中4f位的稀土原子. 磁矩计算表明, 在R₂Fe₁₄B (R: 稀土元素) 晶格中, 4f位的稀土元素与Fe原子作用更强, 对磁性能的影响更大. 稀土原子与Fe的作用与距离呈正相关. 关键词： 2Fe₁₄B')" href="#">Nd₂Fe₁₄B 晶格占位 形成能 原子磁矩     

Investigating material trends and lattice relaxation effects for understanding electron transfer phenomena in rare-earth-doped optical materials

Rare-earth-doped insulators and semiconductors play an important role in a wide range of modern optical technologies. Knowledge of the relative energies of rare-earth ions’ localized electronic states and the band states of the host crystal is important for understanding the properties of these materials and for determining the potential material performance in specific applications such as lasers, phosphors, and optical signal processing. Current understanding of the systematic variations of electron binding energies in these materials is reviewed with analysis of how lattice relaxation affects the results obtained from different experimental techniques. Detailed examples are presented for rare-earth-doped YAG and LaF₃ material systems. A method for predicting the chemical shift of the 4f electrons of rare-earth impurities from the host crystal’s photoemission spectrum is also demonstrated. Furthermore, a simple model is presented that predicts host-dependent trends in the binding energies of the rare-earth ion states in materials ranging from the elemental metals to the ionic fluorides. By understanding the systematic changes in the relative energies for different states, different ions, and different host materials, insight is gained into electron transfer transitions, valence stability, and luminescence quenching that can accelerate the development of materials for optical applications.     

Bethe ansatz results for the 4f-electron spectra of a degenerate Anderson model

We show that the density of states for localized 4f electrons coupled to a conduction band calculated in the framework of Bethe ansatz solution for the degenerate Anderson model qualitatively disagree with the well-known results obtained for the same model but using a variational approach. The scales of parameters used in our Bethe ansatz calculations to fit the experiments disagree with the commonly accepted values from other studies. This implies narrower conduction bands hybridized with 4f orbitals or questions the applicability of the Bethe ansatz for a degenerate Anderson model for the high-energy characteristics of some rare-earth systems.     

Direct observation of antiferroquadrupolar ordering: resonant X-Ray scattering study of DyB2C2

Antiferroquadrupolar (AFQ) ordering has been conjectured in several rare-earth compounds to explain their anomalous magnetic properties. No direct evidence for AFQ ordering, however, has been reported. Using the resonant x-ray scattering technique near the Dy L(III) absorption edge, we have succeeded in observing the AFQ order parameter in DyB2C2 and analyzing the energy and polarization dependence. The much weaker coupling between the orbital degrees of freedom and the lattice in 4f electron systems than in 3d compounds makes them an ideal platform to study orbital interactions originating from electronic mechanisms.     

First principles study on magnetic and electronic properties with rare-earth atoms doped SWCNTs

The adsorptions of rare-earth (RE) atoms on (6, 0) and (8, 0) single-walled carbon nanotubes (SWCNTs) have been investigated by using the first-principles pseudopotential plane wave method within density functional theory (DFT). The binding energy, Mulliken charge, magnetic properties, band structure and DOS were calculated and analyzed. Most of RE atoms including Nd, Sm and Eu have a magnetic ground state with a significant magnetic moment. Some electrons transfer between RE-5d, 6s and C-2p orbitals. Owing to the curvature effect, the values of binding energy for RE atoms doped (6, 0) SWCNT are lower than those of the same atoms on (8, 0) SWCNT. The pictures of DOS show that hybridizations between RE-5d, 6s states and C-2p orbitals and between RE-4f and C-2p orbitals appear near the Fermi level. Results indicate that the properties of SWCNTs can be modified by the adsorptions of RE atoms.     

利用光电离技术研究奇宇称的Sm原子光谱

采用一台频率可扫描的染料激光器将Sm原子从4f66s2 7FJ(J=1,2)态分别激发到具有不同电子组态的若干原子态上,然后利用光电离技术对处于上述状态的Sm原子进行高灵敏探测.通过波长固定在355nm的紫外激光器,我们对一系列具有4f66s6p或者4f55d6s2电子组态的原子状态进行了精密的光谱测量.本实验研究不但确定了这些态的能级位置,还给出了它们的相对光谱强度.通过理论方法对光谱数据详细的分析,我们不但确认了文献中Sm原子的部分奇字称能级的位置和光谱标识,还同时给出了许多新的跃迁及其光谱特性.     

Theory of core-level spectroscopy of rare-earth oxides

A review is presented of the recent development in theoretical studies of X-ray photoemission spectra (XPS) and X-ray absorption spectra (XAS) for rare-earth sesquioxides (R₂O₃) and rare-earth dioxides (RO₂). From the analysis of 3d XPS for R₂O₃ (R = La, Ce,..., Yb) and RO₂ (R = Ce, Pr, Tb) with the impurity Anderson model (without the multiplet coupling effect), we estimate the strength of the covalency hybridization between rare-earth 4f and oxygen 2p states, the charge transfer energy and other physical quantities, and discuss their systematic variation with the change in rare-earth elements. Two possible mechanisms for the splitting of the 3d XPS are pointed out for R₂O₃. One is the initial-state hybridization for R = La, Ce, Pr and Nd; the other is the final-state hybridization for R = Eu and Yb. For RO₂ (R = Ce, Pr, Tb), both of the initial- and final-state hybridizations are essential in explaining the 3d XPS spectra. Then, we study the effect of the intraatomic multiplet coupling on 3d and 4d XPS for La₂O₃, Ce₂O₃, Pr₂O₃, Nd₂O₃, Yb₂O₃ and CeO₂. The multiplet coupling effect is not very important for the 3d XPS, causing only an additional spectral broadening and some minor spectral structures. In the analysis of 4d XPS, however, the interplay between the multiplet coupling and the hybridization plays an essential role. Finally, we study the multiplet structure in 3d and 4d XAS for CeO₂ and PrO₂. It is shown that the original atomic multiplet structure in these XAS is strongly modified by the interatomic hybridization effect, and the experimental multiplet structure is explained consistently with the analysis of 3d and 4d XPS, by the mixed-valence ground state with strong covalency hybridization.     

Eu原子4f~76p_(3/2)ns自电离态的光谱的研究(英文)

采用孤立实激发技术,对铕原子4f~76p_(3/2)ns(n=7,8)自电离态的光谱进行了系统的研究,同时是首次在不同激光偏振组合下进行的研究。首先,用前两束激光分步将铕原子从基态4f~76s~2经中间4f~76s6p态激发至4f~76sns里德堡态,然后再用第三束激光通过离子实4f~76s~+→4f~76p~+_(3/2)的跃迁将其进一步激发至4f~76p_(3/2)7s自电离态或4f~76p_(3/2)8s自电离态。对铕原子4f~76p_(3/2)ns(n=7,8)自电离态复杂的光谱分别给出了详细的解释,从中我们可以获得一些重要的光谱信息,比如自电峰的能级位置和线宽等,同时还可以观察到收敛于不同离子限的自电离系列之间的组态相互作用。最后,通过比较不同激光偏振组合下的自电离光谱,确定了一些自电离态的总角动量的值。     

Ce 基重费米子材料的电子态研究与维度调控

重费米子材料作为一类典型的强关联电子体系,蕴含着非常规超导、奇异金属、量子临界、 磁有序、重电子态、关联拓扑态等新奇的量子态,而4f 电子在其中扮演着重要的作用。随着高分 辨角分辨光电子能谱和薄膜生长技术的发展,精确探测重费米子材料中4f 电子在能量/动量空间 的色散和谱权重成为了可能,这为从微观上理解这类材料中的电子关联效应和新奇量子现象提供 了重要的基础。本论文总结了几个典型的重费米子单晶和薄膜体系的电子态研究,包括Ce-115 体 系、CeCu2Si2、CeRh6Ge4 以及单晶 Ce 膜等。这些结果为理解重费米子体系中重电子态的形成 和温度演化、近藤杂化的能带/动量依赖、重电子能带与超导的关系、近藤效应与磁性和其它量子 态的竞争、4f 电子的维度调控等重要物理问题提供了谱学证据。     

Electronic structure and properties of the actinides

We review the present state of understanding of the electronic structure and physical properties of actinide metals and intermetallic compounds as derived from relativistic APW energy band studies of some of the light (Th, U, Np, and Pu) and heavy (Am, Bk, and Cm) metals, the intermetallics URh₃ and UIr₃ and (NaCl structure compounds such as) UC. Emphasis is placed on the importance of Coulomb correlation and the role of actinide-actinide separation in determining the itinerancy (as in the light metals) or localization (as in the heavy metals) of the 5f electrons and in turn their resulting magnetic and other properties. The UX₃ systems considered are significant because the uranium sites are sufficiently separated to fall in the local moment f orbital range of the Hill superconductivity/magnetism plot but show no magnetic ordering. Comparisons to recent optical, de Haas-van Alphen and other data are given when available. The contrasting cases of the transition and rare-earth systems make it clear that the 5f electrons are a unique species which offer exciting challenges to both experimentalists and theorists.     

Electronic and magnetic properties of SmCrSb3 and GdCrSb3: A first principles study

The density of states (DOS) and the magnetic moments of SmCrSb₃ and GdCrSb₃ have been studied by first principles full-potential linearized augmented plane wave (FP-LAPW) method based on density functional theory (DFT). For the exchange-correlation potential, the local-spin density approximations with correlation energy (LSDA+U) method have been used. Total and partial DOS have been computed using the WIEN2k code. DOS result shows the exchange-splittings of Cr-3d and rare-earth (R) 4f states electrons, which are responsible for the ground state ferromagnetic (FM) behavior of the systems. The FM behavior of these systems is strongly influenced by the average number of Cr-3d and Sm (Gd) 4f-electrons. The effective moment of SmCrSb₃ is found to be 7.07 μ_B while for GdCrSb₃ it is 8.27 μ_B. The Cr atom plays a significant role on the magnetic properties due to the hybridization between Cr-3d and Sb-5p states.     

Unusual spectral renormalization in hexaborides

Employing high resolution photoemission spectroscopy, we studied the evolution of the spectral features in rare earth hexaboride single crystals as a function of temperature and 4f binding energy, where the variation of the 4f binding energy is obtained by changing the rare earth element. High energy resolution helped to reveal the distinct features corresponding to the various photoemission final states. Experimental results of CeB(6), a dense Kondo system, exhibit the growth of the features near the Fermi level with the decrease in temperature relative to the uncompensated local moment contributions. The valence band spectra of the antiferromagnetic compounds, PrB(6) and NdB(6), exhibit multiple features-the 4f ionization peaks (poorly screened features) appear at higher binding energies and the features in the vicinity of the Fermi level possessing significant 4f character are due to the well-screened photoemission final states. These results indicate finite hybridization between the 4f and B 2s2p conduction electronic states. Interestingly, the well-screened features in PrB(6) and NdB(6) exhibit unusual enhancement in intensity at low temperature.     

ELECTRONIC STRUCTURE AND CRYSTALLINE ELECTRIC FIELD IN Rco5(R= Y,La, Ce,Pr, Nd,Sm, Gd,and Tb)

Self consistent charge and spin polarized local spin-density approximation functional theory calculations based on the discrete variational method have been performed for RCo₅(R=Y, La, Ce, Pr, Nd, Sm, Gd, and Tb) compounds. The partial density of states of the Pr atom in the PrCo₆Co₁₂ cluster is established to be strikingly similar to that of the Ce atom in the CeCo₆Co₁₂ cluster, supporting the suggestion that the Pr atom is valence fluctuating. The radii ＜r_4f＞ and ＜r₄f²＞ of the 4f electrons of the R atom from La to Tb, except Ce, show the lanthanide contraction. The crystalline electric field (CEF) parameter A⁰₂ at the R site is calculated using a real charge distribution ρ(R) in the cluster, except for Pr and Nd, and is in agreement with that evalu ated based on the single-ion model. This result shows that the CEF parameter A⁰₂ is mainly determined by the near electronic structure. There exists a hybridization in a certain degree between the light rare-earth R-4f and Co-3d orbitals in some single-electron-molecular-orbitals, which are n ear the Fermi energy level and occupied by electrons. For light rare-earths the R-4f electrons in R Co₆Co₁₂(R=Y, La, Ce, Pr, Nd, and Sm) clu sters are not localized entirely and a small amount of the R-4f electrons have itinerant properties.     

稀土元素(Ce,Pr)掺杂GaN的电子结构和光学性质的理论研究

采用基于密度泛函理论的第一性原理平面波赝势法计算了稀土元素Ce,Pr掺杂GaN的晶格参数、能带、电子态密度和光学性质,使用LSDA +U的方法处理具有强关联作用的稀土4f态,并分析比较计算结果.计算表明:掺入Ce和Pr后的体系相比未掺杂的GaN晶格常数增大,带隙变窄,并分别在禁带中和价带顶附近引入了局域的杂质能级,该能级主要由Ce和Pr的4f电子提供;掺杂后都发生了磁有序化并产生磁矩;最后定性分析了掺杂前后介电函数和光吸收系数的变化,掺Ce的体系在介电函数和吸收系数的低能区出现了峰值,该峰的出现和禁带中的杂质能级到导带底的跃迁有关,而掺Pr的体系由于带隙变窄使介电峰和吸收边发生红移.     

On the electronic structure of thorium metal: Role of the 5 ƒ electrons

Symmetrized Relativistic Augmented Plane Wave calculations for thorium using Kohn-Sham-Gaspár exchange which are found about 5 eV above the Fermi energy metal demonstrate that the 5? states must be considered as band states, unlike the 4? states in the rare-earth metals which are localized states.     

Trapping mechanism in the afterglow process of the rare-earth activated Y2O2S phosphors

Phosphorescence properties are investigated in Y₂O₂S phosphors doped with rare-earth (lanthanoid, Ln) ions. Luminescence afterglow with a decay time of several ten milliseconds is observed at room temperature in the phosphors activated by Nd, Sm, Eu, Dy, Ho, Tm, Er, and Yb. The depths (thermal activation energies) of the traps causing the afterglow are measured with the transient luminescence method.It is concluded that the excited electron and the hole in the conduction and valence bands are trapped separately in the states (impurity levels) located in the vicinity of the Ln³⁺ ion. The trapping depths of the level range from 0.3 to 1.1 eV and are dependent on the electron affinity of the Ln³⁺ ion estimated from the energy difference between the 4fⁿ⁺¹ and the 4fⁿ configurations in the 4f shell of the ion.     

Eu原子4f~76p_(3/2)6d自电离过程的动力学特性

采用孤立实激发技术(isolated-core excitation, ICE)及速度影像技术(velocity-map imaging,VMI),研究了Eu原子4f~76p_(3/2)6d自电离过程的动力学特性.孤立实激发技术用于将Eu原子从基态4f~76s~(2 8)S_(7/2)经中间态4f~76s6p激发到4f~76s6d里德堡态,然后将其进一步激发至4f~76p_(3/2)6d自电离态;速度影像技术用于探测其自电离过程的动力学特性,从而获得自电离衰变的分支比(branch ratio, BR)和弹射电子的角分布(angular distribution, AD).自电离衰变的分支比代表离子的能量分布,从中获得VMI影像的径向信息;而通过各向异性参数描述的弹射电子的角分布揭示了VMI影像的角向信息.此外,讨论了自电离衰变分支比和弹射电子角分布在整个自电离共振能域内的变化情况.基于4f~76s~+和4f~75d~+两个离子态的分支比,讨论了实现Eu离子粒子数反转的可能性.     

Branching ratios of autoionization from Eu 4f~76p_(1/2)6d [J] autoionizing states

The autoionization branching ratios from Eu 4f76p1/26 d [J] autoionizing states to its 4f76s+(9So), 4f76s+(7So), and4f75d+(9Do) final ionic states are investigated with the combination of the three-step laser excitation and the velocity-map imaging technique. These different autoionizing states are excited via 4f76s6d8 DJ [J = 5/2, 7/2, and 9/2] intermediate states, respectively. The experimental photoelectron images are obtained, from which energy distributions of ejected electrons are achieved with the mathematical transformation. Furthermore, the energy dependence of the branching ratio is investigated within the autoionization resonance, by which population inversion is observed as an important characteristic.The J-dependence is also studied systematically. The validity of the well-known isolated core excitation technique used for obtaining the autoionization spectrum is also studied.     

Photon migration at multiple frequencies in YLiF4:Nd crystal

A spatially resolved microluminescence technique was used to measure the spatial distribution of emitted light and photon propagation in Nd³⁺-doped YLiF₄ crystal excited at 514 nm. The spatial distribution of the luminescence was studied and the energy transfer processes among neodymium ions were discussed. We measured the photon diffusion length for specific wavelengths. It was found that re-absorption by ground and excited states plays a crucial role to the propagation. With this information, the microluminescence technique has played a useful role in the investigation of energy transfer processes in rare-earth doped systems.     

Physical Foundations of Formation of Bio-Self-Organization and the Bio-Photon Emission in the Living Systems

According to elementary processes of the biological activities in the living systems with open and non-equilibrium states, which can ever exchange the energy and material and information with the environments, we have established a statistical model formed bio-self-organization, which live on the basis of the negative entropy, by the quantum statistical-theory of non-equilibrium state. From this model we have obtained the peculiar curves of changes of the energy of molecules and found out the distribution function of bio-molecules on quantum energy-levels in the living systems which are completely different from that in inorganic matters. Utilizing the curves of energy obtained we explain well the phenomenon of bio-photon emission of the bio-self-organizations found in the experiments.