The 5f localization/delocalization in square and hexagonal americium monolayers: a FP-LAPW electronic structure study

The electronic and geometrical properties of bulk americium and square and hexagonal americium monolayers have been studied with the full-potential linearized augmented plane wave (FP-LAPW) method. The effects of several common approximations are examined: (1) non-spin polarization (NSP) vs. spin polarization (SP); (2) scalar-relativity (no spin-orbit coupling (NSO)) vs. full-relativity (i.e., with spin-orbit (SO) coupling included); (3) local-density approximation (LDA) vs. generalized-gradient approximation (GGA). Our results indicate that both spin polarization and spin orbit coupling play important roles in determining the geometrical and electronic properties of americium bulk and monolayers. A compression of both americium square and hexagonal monolayers compared to the americium bulk is also observed. In general, the LDA is found to underestimate the equilibrium lattice constant and give a larger total energy compared to the GGA calculations. While spin orbit coupling shows a similar effect on both square and hexagonal monolayer calculations regardless of the model, GGA versus LDA, an unusual spin polarization effect on both square and hexagonal monolayers is found in the LDA results as compared with the GGA results. The 5f delocalization transition of americium is employed to explain our observed unusual spin polarization effect. In addition, our results at the LDA level of theory indicate a possible 5f delocalization could happen in the americium surface within the same Am II (fcc crystal structure) phase, unlike the usually reported americium 5f delocalization which is associated with crystal structure change. The similarities and dissimilarities between the properties of an Am monolayer and a Pu monolayer are discussed in detail.     

Many-body electronic structure of americium metal

We report computer based simulations of energetics, spectroscopy, and electron-phonon interaction of americium using a novel spectral density functional method. This approach gives rise to a new concept of a many-body electronic structure and reveals the unexpected mixed valence regime of Am 5f6 electrons which under pressure acquire the 5f7 valence state. This explains the unique properties of Am and addresses the fundamental issue of how the localization delocalization edge is approached from the localized side in a closed shell system.     

Implementation of LDA+DMFT with the pseudo-potential-plane-wave method

We propose an efficient implementation of combining dynamical mean field theory(DMFT) with electronic structural calculation based on the local density approximation(LDA).The pseudo-potential-plane-wave method is used in the LDA part,which enables it to be applied to large systems.The full loop self consistency of the charge density has been reached in our implementation,which allows us to compute the total energy related properties.The procedure of LDA+DMFT is introduced in detail with a complete flow chart.We have also applied our code to study the electronic structure of several typical strong correlated materials,including cerium,americium and NiO.Our results fit quite well with both the experimental data and previous studies.     

Quantum size effects on the (0001) surface of double hexagonal close packed americium

Electronic structures of double hexagonal close-packed americium and the (0001) surface have been studied via full-potential all-electron density-functional calculations with a mixed APW+lo/LAPW basis. The electronic and geometric properties of bulk dhcp Am as well as quantum size effects in the surface energies and the work functions of the dhcp Am (0001) ultra thin films up to seven layers have been examined at nonmagnetic, ferromagnetic, and antiferromagnetic configurations with and without spin orbit coupling. The anti-ferromagnetic state including spin-orbit coupling is found to be the ground state of dhcp Am with the 5f electrons primarily localized. Our results show that both magnetic configurations and spin-orbit coupling play important roles in determining the equilibrium lattice constant, the bulk modulus as well as the localized feature of 5f electrons for dhcp Am. Our calculated equilibrium lattice constant and bulk modulus at the ground state are in good agreement with the experimental values respectively. The work function of dhcp Am (0001) 7-layer surface at the ground state is predicted to be 2.90 eV. The surface energy for dhcp Am (0001) semi-infinite surface energy at the ground state is predicted to be 0.84 J/m². Quantum size effects are found to be more pronounced in work functions than in surface energies.     

Superconductivity in the americium metal as a function of pressure: probing the Mott transition

High-pressure measurements of the resistivity of americium metal are reported to 27 GPa and down to temperatures of 0.4 K. The unusual dependence of the superconducting temperature (T(c)) on pressure is deduced. The critical field [H(c)(0) extrapolated to T=0] increases dramatically from 0.05 to approximately 1 T as the pressure is increased, suggesting that the type of superconductivity is changing as pressure increases. At pressures of approximately 16 GPa the 5f electrons of Am are changing from localized to itinerant, and the crystal structure also transforms to a complex one. The role of a Mott-type transition in the development of the peak in T(c) above 16 GPa is postulated.     

Two dimensional counterpropagating spatial solitons in photorefractive crystals

We demonstrate experimentally the existence of two transverse-dimensional counterpropagating (CP) incoherent spatial solitons in a 5 x 5 x 23 mm SBN:60Ce photorefractive crystal and investigate their dynamical behavior. We carry out numerical simulations that confirm our experimental findings. Substantially different behavior from the copropagating incoherent solitons is found. A symmetry breaking transition from stable overlapping CP solitons to unstable transversely displaced CP solitons is observed. We perform linear stability analysis that predicts the threshold for the split-up transition, in qualitative agreement with numerical simulations and experimental results.     

Anomalous bond-length behaviors of solid halogens under pressure

The three halogen solids(Cl_2, Br_2, and I_2) have the isostructural diatomic molecular phase I with a space group of Cmca at ambient pressure. At high pressure, they all go through an intermediate phase V with incommensurate structures before eventually dissociating into the monatomic phase II. However, a new structural transition between phase I and V with anomalous bond-length behavior was observed in bromine under pressure, which, so far, has not been confirmed in iodine and chlorine. Here, we perform first-principles calculations for iodine and chlorine. The new structural transition was predicted to be common to all three halogens under pressure. The transition pressures might be systematically underestimated by the imperfect van der Waals correction method, but they follow the order Cl_2 Br_2 I_2, which is consistent with other pressure-induced structural transitions such as metallization and the molecular-to-monatomic transition.     

Charge regulation as a stabilization mechanism for shell-like assemblies of polyoxometalates

We show that the equilibrium size of single-layer shells composed of polyoxometalate macroions is inversely proportional to the dielectric constant of the medium in which they are dispersed. This behavior is consistent with a stabilization mechanism based on Coulomb repulsion combined with charge regulation. We estimate the cohesive energy per bond between macroions on the shells to be approximately -6kT. This number is extracted from analysis based on a charge regulation model in combination with a model for defects on a sphere. The value of the cohesive bond energy is in agreement with the model-independent critical aggregate concentration. This observation points to a new class of thermodynamically stable shell-like objects. We point out the possible relevance our findings have for certain surfactant systems.     

On the transmutation of Am in a fast lead-cooled system

Characteristics of the equilibrium fuel cycle for the core or a blanket of ADS having the structure of the core of a fast lead-cooled reactor of type BREST (Russian abbreviation for ‘Bystryy Reaktor so Svintsovym Teplonositelem’) in a mode of americium transmutation are calculated. Americium loading was taken 5% of heavy atoms. Keeping the average multiplication factor the same as in a standard equilibrium cycle, reactivity swing over 1 year's microcycle is about 1%, that demands partial fuel reloading with a periodicity of about one month. For one year of operation, 61 kg of americium is destroyed, and due to increased ²³⁸Pu content, americium is mainly converted to fission products. Thus in a system of 1 GWt (thermal), 87 kg of americium can be transmuted yearly. The estimate of the reactivity void effect has shown that it increases to 0.6% almost linearly with the void fraction increasing up to 25% and reaches its maximum of 0.7% at a void fraction of about 50%. Application of similar strategy for ADS with a sub-criticality level ≈0.96−0.98 can essentially relax safety problems related to positive void effects.      

Universal behavior in heavy-electron materials

We present our finding that an especially simple scaling expression describes the formation of a new state of quantum matter, the Kondo Fermi liquid (KL) in heavy-electron materials. Emerging at T* as a result of the collective coherent hybridization of localized f electrons and conduction electrons, the KL possesses a non-Landau density of states varying as (1-T/T*)3/2[1+ln(T*/T)]. We show that four independent experimental probes verify this scaling behavior and that for CeIrIn5 the KL state density is in excellent agreement with the recent microscopic calculations.     

Resonant behavior and selective switching of stop bands in three-dimensional photonic crystals with inhomogeneous components

We demonstrate that, in contrast with the well-studied photonic crystals consisting of two homogeneous components, photonic crystals comprised of inhomogeneous or multiple (three or more) components may bring new opportunities to photonics due to the discovered quasiperiodic resonant behavior of their (hkl) stop bands as a function of the reciprocal lattice vector. A resonant stop band cannot be switched off for any permittivity of structural components. Tuning the permittivity or structural parameters allows the selective on-off switching of nonresonant (hkl) stop bands. This independent manipulation of light at different Bragg wavelengths provides a new degree of freedom to design selective optical switches and waveguides. Transmission experiments performed on synthetic opals confirmed the theoretical predictions.     

Retention of the tetragonal to orthorhombic structural transition in F-substituted SmFeAsO: a new phase diagram for SmFeAs(O(1-x)F(x))

In this Letter we propose a new phase diagram for the SmFeAs(O(1-x)F(x)) system, based on careful analysis of synchrotron powder diffraction data, SQUID, and muon spin rotation measurements. The tetragonal to orthorhombic structural transition is slightly affected by F content and is retained for the superconducting samples, even at optimal doping. These findings relate the AFM transition on a different ground with respect to the structural one and suggests that orbital ordering could be the driving force for symmetry breaking.     

Melting of Bi sublattice in nanosized BiFeO3 Perovskite by resonant X-ray diffraction

Free-standing BiFeO3 perovskite particles with a size ranging from polycrystalline bulk down to 5?nm have been studied by high-energy resonant (Bi K edge) x-ray diffraction coupled to differential atomic pair distribution function analysis. Nanosized BiFeO3 particles are found to exhibit extra, i.e., beyond the usual thermal, structural disorder that increases progressively with diminishing their size. In particles of size smaller than approximately 18?nm the disorder destroys the structural coherence of the Bi?sublattice and disturbs that of the Fe-based sublattice in the perovskite structure, substantially affecting the magnetoelectric properties it carries. The new structural information helps better understand the unusual behavior of perovskites structured at the nanoscale.     

Photorefractive two-step recording in a piezoelectric La3Ga5SiO14 crystal doped with praseodymium

The first experimental verification to the authors' knowledge of efficient two-step recording in a photorefractive and piezoelectric crystal of La(3)Ga(5)SiO(14):Pr(3+) with cw laser light (I<20W/cm(2)) is reported. We found nonlinear behavior of the photorefractive sensitivity and photovoltaic current, indicating that the excitation process is connected to excitation of 4f(2) electrons of the Pr(3+) dopant through an intermediate level to the conduction band. This two-step nature of the photorefractive effect makes the crystal an exciting new candidate for applications in holographic storage.     

Thermodynamic study of fluid in terms of equation of state containing physical parameters

We introduce a simple condition for one mole fluid by considering the thermodynamics of molecules pointing towards the effective potential for the cluster.Efforts are made to estimate new physical parameter f in liquid state using the equation of state containing only two physical parameters such as the hard sphere diameter and binding energy.The temperature dependence of the structural properties and the thermodynamic behavior of the clusters are studied.Computations based on f predict the variation of numbers of particles at the contact point of the molecular cavity(radial distribution function).From the thermodynamic profile of the fluid,the model results are discussed in terms of the cavity due to the closed surface along with suitable energy.The present calculation is based upon the sample thermodynamic data for n-hexanol,such as the ultrasonic wave,density,volume expansion coefficient,and ratio of specific heat in the liquid state,and it is consistent with the thermodynamic relations containing physical parameters such as size and energy.Since the data is restricted to n-hexanol,we avoid giving the physical meaning of f,which is the key parameter studied in the present work.     

A relationship between Hurst exponents of slip and waiting time data of earthquakes

We propose a new relationship between the slip and waiting time of real earthquake series. We calculated the Hurst exponents for both time series of slip and waiting time of earthquake sequence in Taiwan CWB (Central Weather Bureau) catalogue. Our findings suggest a good correlation with a correlation coefficient of about 0.8 between the two exponents. Such a good correlation is highly similar to the ones expected from time- or slip-predictable earthquake recurrence models and suggests that the recurrence of real seismicity could be reduced to the time- or slip-predictability in certain sense. This paper, thus, initiates a new direction re-considering earthquake recurrence.     

Structure and formation mechanism of Ge E (') center from divalent defects in Ge-doped SiO2 glass

We have performed ab initio quantum-chemical calculations on clusters of atoms modeling a divalent Ge defect in Ge-doped SiO (2) glasses. It has been found that the divalent Ge defect interacts with a nearby GeO (4) tetrahedron, forming complex structural units that are responsible for the observed photoabsorption band at approximately 5 eV. We have shown that these structural units can be transformed into two equivalent Ge E' centers by way of the positively charged defect center.     

Amplitude and phase of distortion product otoacoustic emissions in the guinea pig in an (f1 ,f2) area study

Lower sideband distortion product otoacoustic emissions (DPOAEs), measured in the ear canal upon stimulation with two continuous pure tones, are the result of interfering contributions from two different mechanisms, the nonlinear distortion component and the linear reflection component. The two contributors have been shown to have a different amplitude and, in particular, a different phase behavior as a function of the stimulus frequencies. The dominance of either component was investigated in an extensive (f1 ,f2) area study of DPOAE amplitude and phase in the guinea pig, which allows for both qualitative and quantitative analysis of isophase contours. Making a minimum of additional assumptions, simple relations between the direction of constant phase in the (f ,f2) plane and the group delays in f1-sweep, f2-sweep, and fixed f2/f1 paradigms can be derived, both for distortion (wave-fixed) and reflection (place-fixed) components. The experimental data indicate the presence of both components in the lower sideband DPOAEs, with the reflection component as the dominant contributor for low f2/f1 ratios and the distortion component for intermediate ratios. At high ratios the behavior cannot be explained by dominance of either component.     

生长温度对磁控溅射ZnO薄膜的结晶特性和光学性能的影响

采用反应射频磁控溅射方法，在Si (100) 基片上制备了具有高c轴择优取向的ZnO薄膜.利用 原子力显微镜、透射电子显微镜、X射线衍射分析、拉曼光谱等表征技术，研究了沉积温度 对ZnO薄膜的表面形貌、晶粒尺度、应力状态等结晶性能的影响；通过沉积温度对透射光谱 和光致荧光光谱的影响，探讨了ZnO薄膜的结晶特性与光学性能之间的关系.研究结果显示， 在室温至500℃的范围内，ZnO薄膜的晶粒尺寸随沉积温度的增加而增加，在沉积温度为500 ℃时达到最大；当沉积温度为750℃时，ZnO薄膜的晶粒尺度有所减小；在室温至750℃的范 围内，薄膜中ZnO晶粒与Si基体之间均存在着相对固定的外延关系；在沉积温度低于500℃时 ，制备的ZnO薄膜处于压应变状态，而750℃时沉积的薄膜表现为张应变状态.沉积温度的不 同导致ZnO薄膜的折射率、消光系数、光学禁带宽度以及光致荧光特性的变化，沉积温度对 紫外光致荧光特性起着决定性的作用.此外，探讨了影响薄膜近紫外光致荧光发射的可能因 素. 关键词： ZnO薄膜 表面形貌 微观结构 光学常数