Structural stability, phase transformations and band-tuning of actinide and rare earth based intermetallics under high pressure: a perspective

When a solid is subjected to external pressure, it can undergo either structural transformation or remain stable in its parent structure. The sequence of structural transformations, when mapped for similar materials, viz., isostructural, isoelectronic and so on, can be used to create a map showing the evolution of structures under pressure for such materials. Such maps are useful in predicting high pressure phases. The structural transitions and the stability of materials as a function of pressure are intricately connected to their electronic structure. Many a times it is advantageous to know the stability of the material under pressure just by calculating its electronic structure. This can be accomplished only if several homologues materials are studied and the stability criteria arrived at by correlating their electronic structure with their structural stability under pressure. Further, as a function of pressure, the electronic structure changes can lead to enhancement in certain desired electronic, physical or mechanical properties. Several examples are known, wherein, pressure tuning of the band structure leads to improved properties. In this paper, we have discussed the above mentioned areas and presented a perspective of the above using the results of our own studies on f-electron based intermetallics (f-IMCs).     

Revealing the Pressure-Induced Softening/Weakening Mechanism in Representative Covalent Materials

Diamond, cubic boron nitride(c-BN), silicon(Si), and germanium(Ge), as examples of typical strong covalent materials, have been extensively investigated in recent decades, owing to their fundamental importance in material science and industry. However, an in-depth analysis of the character of these materials' mechanical behaviors under harsh service environments, such as high pressure, has yet to be conducted. Based on several mechanical criteria, the effect of pressure on the mechanical properties of these materials is comprehensively investigated.It is demonstrated that, with respect to their intrinsic brittleness/ductile nature, all these materials exhibit ubiquitous pressure-enhanced ductility. By analyzing the strength variation under uniform deformation, together with the corresponding electronic structures, we reveal for the first time that the pressure-induced mechanical softening/weakening exhibits distinct characteristics between diamond and c-BN, owing to the differences in their abnormal charge-depletion evolution under applied strain, whereas a monotonous weakening phenomenon is observed in Si and Ge. Further investigation into dislocation-mediated plastic resistance indicates that the pressure-induced shuffle-set plane softening in diamond(c-BN), and weakening in Si(Ge), can be attributed to the reduction of antibonding states below the Fermi level, and an enhanced metallization, corresponding to the weakening of the bonds around the slipped plane with increasing pressure, respectively. These findings not only reveal the physical mechanism of pressure-induced softening/weakening in covalent materials, but also highlights the necessity of exploring strain-tunable electronic structures to emphasize the mechanical response in such covalent materials.     

波导等离子体限幅器中气体的选择与触发条件计算

 为保护电子设备不受高功率微波损坏,在矩形波导中嵌入等离子体限幅器。计算了不同气体的微波击穿场强随气体压强以及微波频率的变化规律。在高气压条件下（1 333~133 320 Pa）,气体击穿场强随气压增大而增大,在计算的4种气体中Ne的击穿场强最小;低气压条件下（1.333 2~133.32 Pa）,气体击穿场强随气压增大而减小,且Xe具有最小击穿场强。高气压条件下气体的击穿场强明显高于低气压下的击穿场强。计算结果表明：当填充133.32 Pa的Xe时,限幅器能够在约30 km范围内,有效地防护10 GW级高功率微波对电子设备的损坏。     

Controllable synthesis of fullerene nano/microcrystals and their structural transformation induced by high pressure

Fullerene molecules are interesting materials because of their unique structures and properties in mechanical, electrical, magnetic, and optical aspects. Current research is focusing on the construction of well-defined fullerene nano/microcrystals that possess desirable structures and morphologies. Further tuning the intermolecular interaction of the fullerene nano/microcrystals by use of pressure is an efficient way to modify their structures and properties, such as creation of nanoscale polymer structures and new hybrid materials, which expands the potential of such nanoscale materials for di- rect device components. In this paper, we review our recent progress in the construction of fullerene nanostructures and their structural transformation induced by high pressure. Fullerene nano/microcrystals with controllable size, morphology and structure have been synthesized through the self-assembly of fullerene molecules by a solvent-assisted method. By virtue of high pressure, the structures, components, and intermolecular interactions of the assemblied fullerene nano/microcrystals can be finely tuned, thereby modifying the optical and electronic properties of the nanostructures. Several examples on high pressure induced novel structural phase transition in typical fullerene nanocrystals with C60 or C70 cage serving as build- ing blocks are presented, including high pressure induced amorphization of the nanocrystals and their bulk moduli, high pressure and high temperature （HPHT） induced polymerization in C60 nanocrystals, pressure tuned reversible polymeriza- tion in ferrocene-doped C60/C70 single crystal, as well as unique long-range ordered crystal with amorphous nanoclusters serving as building blocks in solvated C60 crystals, which brings new physical insight into the understanding of order and disorder concept and new approaches to the design of superhard carbon materials. The nanosize and morphology effects on the transformations of fullerene nanocrystals have also been discussed. These results provide the foundation for the fabrication of pre-designed and controllable geometries, which is critical in fullerenes and relevant materials for designing nanometer-scale electronic, optical, and other devices.     

Structures and physical properties of R_2TX_3 compounds

Rare-earth compounds have been an attractive subject based on the unique electronic structures of the rare-earth elements. Novel ternary intermetallic compounds R2TX3 (R = rare-earth element or U, T = transition-metal element, X = Si, Ge, Ga, In) are a significant branch of this research field due to their complex and intriguing physical properties, such as magnetic order at low temperature, spin-glass behavior, Kondo effect, heavy fermion behavior, and so on. The unique physical properties of R2TX3 compounds are related to distinctive electronic structures, crystal structures, micro-interaction, and external environment. Most R2TX3 compounds crystallize in AlB2-type or derived AlB2-type structures and exhibit many similar properties. This paper gives a concise review of the structures and physical properties of these compounds. Spin glass, magnetic susceptibility, resistivity, and specific heat of R2TX3 compounds are discussed.     

Application of accelerated-convergence technique to modified Lanczos calculations

Summary The use of modified Lanczos procedure to obtain the ground-state eigenvalue and eigenvector of the Hamiltonians of physical systems and its subsequent modification for the determination of excited states has been revealed a very efficient and powerful procedure. Nevertheless, when implementing the method, one notices that the convergence of the algorithm is very slow, so that the calculation may become heavy from a computational point of view. The aim of this paper is the proposal of an accelerated-convergence technique (which has already been successfully used in density-of-states calculations), that allows to obtain a faster convergence of the modified Lanczos eigenvalues to the exact ones. The advantages of such a technique are shown through the discussion of some examples.     

High pressure electronic properties in the light of inelastic X-ray scattering From magnetic collapse to quantum criticality

The properties of solids are strongly modified at high pressure. Not only their structure is affected as a direct consequence of the compressed lattice, but also their electronic and magnetic properties as pressure alters significantly the electron density and orbital overlap, thus the electronic localization and hybridization. We present here high pressure experiments using resonant inelastic x-ray scattering. RIXS in the high energy range (≥5keV) has appeared as a powerful probe of the electronic properties under extreme conditions. It is chemically and orbitally selective while showing an intrinsic resolving power spectacularly larger than standard spectroscopic probes. Results will be briefly presented in 3d metals and f-electron systems. The behavior of 3d electrons under pressure will be explored in the light of magnetic collapse transitions; We will comment on f-electron delocalization, especially when approaching a Kondo anomaly or a quantum critical point; Pressure dedicated setups are also discussed.     

统计物理和复杂系统专题编者按

从20世纪中叶至今,复杂系统研究迅速发展,成为了引人注目并具有广泛应用的新领域.复杂系统要么具有结构的复杂性,要么具有演化的复杂性,在多数情况下二者兼具.不同于传统物理学通常处理的规则介质,许多复杂系统具有复杂结构,近年来受到极大关注的复杂网络结构就是其中最典型的代表.同时复杂系统也可表现为演化行为的多样性和复杂性.即便系统结构并不复杂,系统中的非线性相互作用可能产生复杂的演化行为,包括:形形色色的不稳定性;丰富的斑图动力学;各种各样的自组织、涌现及进化行为等等.物理学从一开始就深深进入了复杂系统研究领域,其中统计物理无疑是研究和理解复杂系统最主要的工具.     

Quantum phase transitions in electronic systems

Quantum phase transitions occur at zero temperature when some non‐thermal control‐parameter like pressure or chemical composition is changed. They are driven by quantum rather than thermal fluctuations. In this review we first give a pedagogical introduction to quantum phase transitions and quantum critical behavior emphasizing similarities with and differences to classical thermal phase transitions. We then illustrate the general concepts by discussing a few examples of quantum phase transitions occurring in electronic systems. The ferromagnetic transition of itinerant electrons shows a very rich behavior since the magnetization couples to additional electronic soft modes which generates an effective long‐range interaction between the spin fluctuations. We then consider the influence of rare regions on quantum phase transitions in systems with quenched disorder, taking the antiferromagnetic transitions of itinerant electrons as a primary example. Finally we discuss some aspects of the metal‐insulator transition in the presence of quenched disorder and interactions.     

Magnetic behavior in UFe?Zn?? and URu?Zn?? single crystals

The magnetic, electrical transport and thermodynamic properties of the compounds UFe?Zn?? and URu?Zn?? were studied on single-crystalline specimens over wide ranges of temperature and magnetic field. The results indicate that the two ternaries are paramagnetic moderately enhanced heavy fermion systems. Their physical behavior is governed predominantly by the hybridization of uranium 5f orbitals with electronic states of ligands, which brings about considerable delocalization of the 5f states.     

重费米子化合物 CemMnIn3m+2n(m = 1, 2, 3; n = 0, 1, 2; M = Co,Rh,Ir,Pt 及Pd) 的角分辨光电子能谱研究

重费米子材料以其新奇多变的宏观性质,复杂而难以理解的微观物理过程而受到广泛的关注,长期是凝聚态物理研究的重点。角分辨光电子能谱作为一种能够直接探测材料电子结构的实验手段,随着近年来实验技术的高度发展,能量和动量分辨率得到了极大的提高,能够有力地探测到强关联材料中更加精细的电子结构。使用角分辨光电子能谱探测重费米子材料的电子结构,为理解其各种物理过程提供强有力的实验证据,进而推进重费米子理论的发展。本文回顾 Ce 基重费米子材料 CemMnIn3m+2n (m = 1; 2; 3;n = 0; 1; 2;M =Co, Rh, Ir, Pt, Pd) 系列化合物的角分辨光电子能谱研究,包括电子结构的维度、近藤共振、f 电子与导带电子的杂化和电子结构随温度的变化等。     

Analysis of semiconductor surface phonons by Raman spectroscopy

Only recently Raman spectroscopy (RS) has advanced into the study of surface phonons from clean and adsorbate-covered semiconductor surfaces. RS allows the determination of eigenfrequencies as well as symmetry selection rules of surface phonons, by k-conservation limited to the Brillouin zone-center, and offers a significantly higher spectral resolution than standard surface science techniques such as high-resolution electron energy loss spectroscopy. Moreover, surface electronic states become accessible via electron–phonon coupling. In this article the fundamentals of Raman scattering from surface phonons are discussed and its potential illustrated by considering two examples, namely Sb-monolayer-terminated and clean InP(110) surfaces. Both are very well understood with respect to their atomic and electronic structure and thus may be regarded as model systems for heteroterminated and clean semiconductor surfaces. In both cases, localized surface phonons as well as surface resonances are detected by Raman spectroscopy. The experimental results are compared with surface modes predicted by theoretical calculations. On InP(110), due to the high spectral resolution of Raman spectroscopy, several surface modes predicted by theory can be experimentally verified. Surface electronic transitions are detected by changing the energy of the exciting laser light indicating resonances in the RS cross section. Received: 7 April 1999 / Accepted: 25 June 1999 / Published online: 16 September 1999     

Kohn-Sham theory for ground-state ensembles

An electron density distribution n(r) which can be represented by that of a single-determinant ground state of noninteracting electrons in an external potential v(r) is called pure-state v-representable (P-VR). Most physical electronic systems are P-VR. Systems which require a weighted sum of several such determinants to represent their density are called ensemble v-representable (E-VR). This paper develops formal Kohn-Sham equations for E-VR physical systems, using the appropriate coupling constant integration. It also derives local density- and generalized gradient approximations, and conditions and corrections specific to ensembles.     

Spin and spin-orbit coupling effects in nickel-based superalloys: A first-principles study on Ni3Al doped with Ta/W/Re

Heavy elements(X=Ta/W/Re)play an important role in the performance of superalloys,which enhance the strength,anti-oxidation,creep resistance,and anti-corrosiveness of alloy materials in a high-temperature environment.In the present research,the heavy element doping effects in FCC-Ni(γ)and Ni₃Al(γ')systems are investigated in terms of their thermodynamic and mechanical properties,as well as electronic structures.The lattice constant,bulk modulus,elastic constant,and dopant formation energy in non-spin,spin polarized,and spin-orbit coupling(SOC)calculations are compared.The results show that the SOC effects are important in accurate electronic structure calculations for alloys with heavy elements.We find that including spin for bothγandγ'phases is necessary and sufficient for most cases,but the dopant formation energy is sensitive to different spin effects,for instance,in the absence of SOC,even spin-polarized calculations give 1%to 9%variance in the dopant formation energy in our model.Electronic structures calculations indicate that spin polarization causes a split in the metal d states,and SOC introduces a variance in the spin-up and spin-down states of the d states of heavy metals and reduces the magnetic moment of the system.     

Electronic structure calculations and strong correlations: A model study

Metals with strong correlations are a major challenge for realistic electronic structure calculations. The complexity of the systems under consideration precludes a direct fully microscopic treatment by means of the theoretical and computational methods available at present. The present paper analyzes the applicability and restrictions of common approximation schemes by comparing their predictions for a model pertinent to heavy fermion metals to the exact solution. The criteria chosen for the assessment are the density distribution in the ground state as well as the energy scale for low-lying excitations.     

Linearization of Systems of Nonlinear Diffusion Equations

We investigate the linearization of systems of n-component nonlinear diffusion equations; such systems have physical applications in soil science, mathematical biology and invariant curve flows. Equivalence transformations of their auxiliary systems are used to identify the systems that can be linearized. We also provide several examples of systems with two-component equations, and show how to linearize them by nonlocal mappings.     

Electronic-enthalpy functional for finite systems under pressure

We introduce the notion of electronic enthalpy for first-principles structural and dynamical calculations of finite systems under pressure. An external pressure field is allowed to act directly on the electronic structure of the system studied via the ground-state minimization of the functional E+PV(q), where V(q) is the quantum volume enclosed by a charge isosurface. The Hellmann-Feynman theorem applies, and assures that the ionic equations of motion follow an isoenthalpic dynamics. No pressurizing medium is explicitly required, while coatings of environmental ions or ligands can be introduced if chemically relevant. We apply this novel approach to the study of group-IV nanoparticles during a shock wave, highlighting the significant differences in the plastic or elastic response of the diamond cage under load, and their potential use as novel nanostructured impact-absorbing materials.     

Condensation effects of excitons

The theory of the electronic excitations in a highly excited semiconductor is presented. The relaxation processes, the formation of excitons and excitonic molecules, the interaction among the various forms of electronic excitations, as well as their optical and thermodynamical properties are analyzed. At low temperatures one expects condensations into the quantum statistically degenerate phases of the excitonic molecules and of the electron-hole plasma. The physical properties of these low temperature phases are investigated. Possibilities and previous attempts to observe the Bose-Einstein condensation in excitonic systems are discussed critically. The experimental observations of the electron-hole liquid phase transition are reviewed.     

Anomalous electronic state in CaCrO3 and SrCrO3

Comprehensive measurements of electrical transport properties under pressure, thermal conductivity, magnetic susceptibility, and room-temperature compressibility have been used to characterize SrCrO3 and CaCrO3 perovskites synthesized under high pressure. Comparison with other narrow-band perovskite oxides suggests that their anomalous physical properties are correlated with bond-length instabilities caused by the crossover from localized to itinerant electronic behavior.