Energy-based coupling of smooth particle hydrodynamics and molecular dynamics with thermal fluctuations

We propose a thermodynamically consistent and energy conserving coupling scheme between the atomistic and the continuum domain. The coupling scheme links the two domains using the DPDE (Dissipative Particle Dynamics at constant Energy) thermostat and is designed to handle strong temperature gradients across the atomistic/continuum domain interface. The fundamentally different definitions of temperature in the continuum and atomistic domain – internal energy and heat capacity versus particle velocity – are accounted for in a straightforward and conceptually intuitive way by the DPDE thermostat. We verify the here proposed scheme using a fluid, which is simultaneously represented as a continuum using Smooth Particle Hydrodynamics, and as an atomistically resolved liquid using Molecular Dynamics. In the case of equilibrium contact between both domains, we show that the correct microscopic equilibrium properties of the atomistic fluid are obtained. As an example of a strong non-equilibrium situation, we consider the propagation of a steady shock-wave from the continuum domain into the atomistic domain, and show that the coupling scheme conserves both energy and shock-wave dynamics.     

Structure and magnetic properties of Zn<Subscript>0.9</Subscript>Co<Subscript>0.1</Subscript>O nanorods synthesized by a simple sol–gel method using metal acetylacetonate and poly(vinyl alcohol)

Room-temperature ferromagnetism was observed in Zn_0.9Co_0.1O nanorods with diameters and lengths of ∼100–200 nm and ∼200–1000 nm, respectively. Nanorods were synthesized by a simple sol–gel method using metal acetylacetonate powders of Zn and Co and poly(vinyl alcohol) gel. The XRD, FT-IR and SAED analyses indicated that the nanorods calcined at 873–1073 K have the pure ZnO wurtzite structure without any significant change in the structure affected by Co substitution. Optical absorption measurements showed absorption bands indicating the presence of Co²⁺ in substitution of Zn²⁺. The specific magnetization of the nanorods appeared to increase with a decrease in the lattice constant c of the wurtzite unit cell with the highest value being at 873 K calcination temperature. This magnetic behavior is similar to that of Zn_0.9Co_0.1O nanoparticles prepared by polymerizable precursor method. We suggest that this behavior might be related to hexagonal c-axis being favorable direction of magnetization in Co-doped ZnO and the 873 K (energy of 75 meV) being close to the exciton/donor binding energy of ZnO.     

A multiscale coupling method for the modeling of dynamics of solids with application to brittle cracks

We present a multiscale model for numerical simulations of dynamics of crystalline solids. The method combines the continuum nonlinear elasto-dynamics model, which models the stress waves and physical loading conditions, and molecular dynamics model, which provides the nonlinear constitutive relation and resolves the atomic structures near local defects. The coupling of the two models is achieved based on a general framework for multiscale modeling – the heterogeneous multiscale method (HMM). We derive an explicit coupling condition at the atomistic/continuum interface. Application to the dynamics of brittle cracks under various loading conditions is presented as test examples.     

Supersymmetric quantum-well shape optimization for intersubband bound–continuum second harmonic generation

A method is described for the optimized design of quantum-well structures, with respect to maximizing the second-order susceptibilities relevant for second harmonic generation. The possibility is explored of obtaining resonantly enhanced nonlinear optical susceptibilities in quantum wells with two bound states and a continuum resonance state as the dominant third state. The method relies on applying the isospectral (energy structure preserving) transformations to an initial Hamiltonian in order to generate a parameter-controlled family of Hamiltonians. By changing the values of control parameters one changes the potential shape and thus the values of matrix elements relevant to susceptibility to be maximized. The method was used for the design of Al_xGa_1 − xAs -based QWs. The results indicate the possibility of employing continuum states in resonant second harmonic generation at higher photon energies,ℏω =  200–300 meV.     

Atomistic–continuum interphase model for effective properties of composite materials containing nano-inhomogeneities

Classical micromechanics were revised to study the elastic properties of heterogeneous materials containing nano-inhomogeneities. Contrary to previous studies, this work introduces the concept of an interphase, in contrast to a sharp interface, to account for the interface excess stress effect at the nano-scale. The interphase's constitutive properties are derived from atomistic simulations within the continuum framework. These properties are then incorporated in a micromechanics-based interphase model to compute the effective properties of nano-composites. This scale transition approach bridges the gap between discrete systems (atomic level interactions) and continuum mechanics. An advantage of this approach is that it combines atomistic with continuum models that consider inhomogeneity and interphase morphology. It thereby enables us to account simultaneously for both the shape and the anisotropy of a nano-inhomogeneity and interphase at the continuum level when we compute a material's overall properties. In so doing, it frees us from making any assumptions about the interface characteristics between matrix and the nano-inhomogeneity.     

Terahertz dual-wavelength quantum cascade laser based on GaN active region

In this paper a novel terahertz (THz) quantum cascade laser (QCL) based on GaN/AlGaN quantum wells has been proposed, which emits at two widely separated wavelengths 33 and 52 μm simultaneously in a single active region. The large LO-phonon energy (～90 meV), the ultrafast resonant phonon depopulation of the lower radiative levels, suppression of the electrons that escape to the continuum states and selective carrier injection and extraction all together lead to a considerable enhancement in the operating temperature of the structure. All calculations have been done at a temperature of 265 K. Moreover, similar behavior of the output optical powers is another remarkable feature, which makes both wavelengths useful for special applications.     

Effects of S incorporation on Ag substitutional acceptors in ZnO:(Ag, S) thin films

Ag–S codoped ZnO thin films have been fabricated on Si substrates by radio frequency (RF) magnetron sputtering using a thermal oxidation method. XRD and SEM measurements showed that the sample has hexagonal wurtzite structure with a preferential (002) orientation and the surface is composed of compact and uniform grains. Ag_Zn–nS_O defect complexes were observed in the Ag–S codoped ZnO films by XPS analysis. Low temperature PL spectra showed neutral acceptor bound exciton emission related to Ag_Zn–nS_O. The corresponding acceptor ionization energy of 150 meV is much lower than that of monodoped Ag (246 meV), which is favorable for p-type doping of ZnO.     

Transition temperature reduction for CdS nanoparticles under high pressure

The structure transition of nanoparticles has a significant effect on their practical applications. In this study, the transition temperature of CdS nanoparticles with the size of 3–5 nm from sphalerite to wurtzite structure is significantly reduced to 150 °C under a high pressure of 1 GPa, much lower than that 300–400 °C for CdS nanoparticles and 600 °C for bulk CdS under room pressure. The lower transition temperature leads to an ultrafine grain size d = 5 nm for the formed wurtzite phase as compared with that d = 33 nm yielded under room pressure with a similar transition volume fraction of ~80%. The underlying physical mechanism is discussed.     

Coarse-graining the computations of surface reactions: Nonlinear dynamics from atomistic simulators

We review and discuss the use of equation-free computation in extracting coarse-grained, nonlinear dynamics information from atomistic (lattice-gas) models of surface reactions. The approach is based on circumventing the explicit derivation of macroscopic equations for the system statistics (e.g., average coverage). Short bursts of appropriately initialized computational experimentation with the lattice-gas simulator are designed “on demand” and processed in the spirit of the coarse timestepper introduced in Theodoropoulos et al. (2000) (K. Theodoropoulos, Y.-H. Qian, I.G. Kevrekidis, Proc. Natl. Acad. Sci. USA 97 (2000) 9840). The information derived from these computational experiments, processed through traditional, continuum numerical methods is used to solve the macroscopic equations without ever deriving them in closed form. The approach is illustrated through two computational examples: the CO oxidation reaction, and the NO + CO/Pt(1 0 0) reaction.     

纤锌矿GaN/AlxGa1-xN量子阱中极化子能量

采用LLP变分方法研究了纤锌矿GaN/Al_xGa_1-xN量子阱材料中极化子的能级,给出极化子基态能量、第一激发态能量和第一激发态到基态的跃迁能量与量子阱宽度和量子阱深度变化的函数关系。研究结果表明,极化子基态能量、第一激发态能量和跃迁能量随着阱宽L的增大而开始急剧减小,然后缓慢下降,最后接近于体材料GaN中的相应值。基态能量和第一激发态到基态的跃迁能量随着量子阱深度的增加而逐渐增加,窄阱时这一趋势更明显。纤锌矿氮化物量子阱中电子-声子相互作用对能量的贡献比较大,这一值(约40meV)远远大于闪锌矿(GaAs/Al_xGa_1-xAs)量子阱中相应的值(约3meV)。因此讨论GaN/Al_xGa_1-xN量子阱中电子态问题时应考虑电子-声子相互作用。     

Effect of pressure and mechanical stress on the electronic properties of AlN and GaN

The fundamental properties of the AlN and GaN compounds with a wurtzite structure under external hydrostatic pressure, uniaxial mechanical stress σ_⊥ along the hexagonal axis, and biaxial mechanical stress σ_⊥ in the basal plane of the unit cell have been considered in terms of first-principles calculations in the frame-work of the density functional theory. The pressures of the phase transitions from the structures of wurtzite and zinc blende to the structure of rock salt have been obtained. The behavior of the structural parameters, interband transitions, and positions of the charge neutrality level has been investigated. The calculated pressure coefficients of the band gap are as follows: ∂E _g /∂p = 40.9 meV/GPa, −∂E _g /∂σ _| = −4.2 meV/GPa, and −∂E _g /∂σ _⊥ = 45.2 meV/GPa for AlN and ∂E _g /∂p = 33.0 meV/GPa, −∂E _g /∂σ _| = 23.6 meV/GPa, and −∂E _g /∂σ _⊥ = 9.6 meV/GPa for GaN. The pressure coefficients of the charge neutrality level in almost all cases are substantially smaller than the corresponding values obtained for the band gap E _g .     

Modelling transient heat conduction in solids at multiple length and time scales: A coupled non-equilibrium molecular dynamics/continuum approach

A method for controlling the thermal boundary conditions of non-equilibrium molecular dynamics simulations is presented. The method is simple to implement into a conventional molecular dynamics code and independent of the atomistic model employed. It works by regulating the temperature in a thermostatted boundary region by feedback control to achieve the desired temperature at the edge of an inner region where the true atomistic dynamics are retained. This is necessary to avoid intrinsic boundary effects in non-equilibrium molecular dynamics simulations. Three thermostats are investigated: the global deterministic Nosé–Hoover thermostat and two local stochastic thermostats, Langevin and stadium damping. The latter thermostat is introduced to avoid the adverse reflection of phonons that occurs at an abrupt interface. The method is then extended to allow atomistic/continuum models to be thermally coupled concurrently for the analysis of large steady state and transient heat conduction problems. The effectiveness of the algorithm is demonstrated for the example of heat flow down a three-dimensional atomistic rod of uniform cross-section subjected to a variety of boundary conditions.     

Structural and physical properties of ZnO:Al films grown on glass by direct current magnetron sputtering with the oblique target

ZnO:Al films were deposited on glass substrates at 300 K and 673 K by direct current magnetron sputtering with the oblique target. The Ar pressure was adjusted to 0.4 Pa and 1.2 Pa, respectively. All the films have a wurtzite structure and grow with a c-axis orientation in the film growth direction. The films grow mainly with columnar grains perpendicular to the substrate and some granular grains also exist in the films. The film deposited at 673 K and 0.4 Pa has the largest grains whereas that prepared at 300 K and 0.4 Pa consists of the smallest grains and is porous. The films exhibit an n-type semiconducting behavior at room temperature. The ZnO:Al film deposited at 673 K and 0.4 Pa has the lowest resistivity (3.40 × 10⁻³ Ω cm), the highest free electron concentration (4.63 × 10²⁰ cm⁻³) and a moderate Hall mobility (4.0 cm² V⁻¹ s⁻¹). The film deposited at 300 K and 0.4 Pa has the highest resistivity and the lowest free electron concentration and Hall mobility. A temperature dependence of the resistivity reveals that the carrier transport mechanism is Mott’s variable range hopping in the temperature region below 100 K and thermally activated band conduction above 215 K. The activation energy for the film deposited at 300 K and 0.4 Pa is 41 meV and that for the other films is about 35 meV. All the films have an average optical transmittance of over 85% in the visible wavelength range. The absorption edge of the film deposited at 300 K and 0.4 Pa shifts to the longer wavelength (redshift) relative to the films prepared under the other conditions.     

Van der Waals energy surface of a carbon nanotube sheet

The van der Walls interaction between a carbon nanotube sheet (CNTS) and a rare gas atom, is studied using both atomistic and continuum approaches. We present analytical expressions for the van der Waals energy of continuous nanotubes interacting with a rare gas atom. It is found that the continuum approach does not properly treat the effect of atomistic configurations on the energy surfaces. The energy barriers are small as compared to the thermal energy, which implies the free motion above the CNTS in heights about one nanometer. In contrast to the energy surface of a graphene sheet, the honeycomb lattice structure in the energy surface of a CNTS is imperceivable. Defects alter the energy surface which therefore influence the gas adsorption mechanism.     

Investigation of Mn incorporation in fifteen-period InGaAs/GaAs quantum well system

A ferromagnetic ordering with a Curie temperature of 50 K of fifteen layer of InGaMnAs/GaAs multi quantum wells (MQWs) structure grown on high resistivity (100) p-type GaAs substrates by molecular beam epitaxy (MBE) was found. It is likely that the ferromagnetic exchange coupling of sample with Curie temperature of 50 K is hole-mediated resulting in Mn substituting In or Ga sites. Temperature and excitation power dependent PL emission spectra of InGaMnAs MQWs sample grown at temperature of 170 °C show that an activation energy of Mn ion on the first quantum confinement level in InGaAs quantum well is 36 meV and impurity Mn is partly ionized. It is found that the activation energy of 36 meV of Mn ion in the QW is lower than the activation energy of 110 meV for a substitutional Mn impurity in GaAs. These measurements provide strong evidence that an impurity band existing in the bandgap due to substitutional Mn ions and it is the location of the Fermi level within the impurity band that determines Curie temperature.     

Electron-phonon interaction effects on the surface states in wurtzite nitride semiconductors

A variational approach is used to study the surface states of an electron in a semi-infinite wurtzite nitride semiconductor. The surface-state energy of the electron is calculated, by taking the effects of the electron-surface optical phonon interaction and structure anisotropy into account. The numerical computation has been performed for the energies of the electronic surface states as a function of the surface potential V₀ for wurtzite GaN, AlN, and InN, respectively. The results show that the electron-phonon interaction lowers the surface state energy. It is also found that the energies of the electronic surface-state in wurtzite structures are lower than that in the zinc-blende structures by hundreds of meV for the materials calculated. The influence of e-p-interactions on the surface state of electron cannot be neglected.     

Preparation of pure CdSe nanocrystals through mechanical alloying

Pure CdSe nanocrystals have been successfully synthesized by mechanical alloying Cd and Se elemental powders. XRD results show that pure CdSe compound in wurtzite structure has been fabricated after mechanical alloying the elemental powders for 130 min. All the diffraction peaks from elemental Cd and Se disappeared completely in those XRD patterns of as-milled CdSe nanocrystals for more than 3 h. When the mechanical alloying process was carried out for 40 h, typical zinc blende structure diffraction mode was exhibited in the XRD pattern. Structural evolution of CdSe nanocrystal with ball milling time has been discussed in detail. A phase transformation from wurtzite to zinc blende structure took place when the mechanical alloying process prolonged to 40 h. HRTEM images of the individual as-milled CdSe nanocrystals confirmed such phase transformation. The grain size of the as-milled CdSe nanocrystals ranges from 2 to 30 nm, with majority being distributed within the range from 2 to 8 nm.     

Application of abrupt cut-off models in the analysis of the capacitance spectra of conjugated polymer devices

In this paper, a detailed study of the capacitance spectra obtained from Au/doped-polyaniline/Al structures in the frequency domain (0.05 Hz–10 MHz), and at different temperatures (150–340 K) is carried out. The capacitance spectra behavior in semiconductors can be appropriately described by using abrupt cut-off models, since they assume that the electronic gap states that can follow the ac modulation have response times varying rapidly with a certain abscissa, which is dependent on both temperature and frequency. Two models based on the abrupt cut-off concept, formerly developed to describe inorganic semiconductor devices, have been used to analyze the capacitance spectra of devices based on doped polyaniline (PANI), which is a well-known polymeric semiconductor with innumerous potential technological applications. The application of these models allowed the determination of significant parameters, such as Debye length (≈20 nm), position of bulk Fermi level (≈320 meV) and associated density of states (≈2×10¹⁸ eV⁻¹ cm⁻³), width of the space charge region (≈70 nm), built-in potential (≈780 meV), and the gap states’ distribution.     

Temperature effects on exciton–phonon coupling and Auger recombination in CdTe/ZnTe quantum dots

We report the results of experimental studies on temperature-dependent thermal escape and Auger recombination coefficients in CdTe/ZnTe quantum dots. We show that at low temperatures, there is a thermally activated transition between two different states separated by a localization energy of about 15.8 meV, while the primary non-radiative process at high temperatures is thermal escape assisted multi-longitudinal optical (LO) phonons absorption with three phonons. The most striking result is a rapid increase in the Auger coefficient and a reduction in the decay time with increasing temperature above 35 K. These results show that the Auger process is assisted by the participation of phonons with an energy threshold of 34.4 meV and an LO phonon energy of around 19 meV.     

Elektronenenergieverlustspektren von Graphiteinkristallen und Kohlenstoffaufdampfschichten im Bereich 0,02–0,4 eV

High-resolved electron energy loss spectra of graphite and of evaporated carbon films have been measured in the energy loss range between 20 and 400 meV. The primary energy was 25 keV, the energy resolution between 4 and 7 meV. The energy loss spectrum of graphite is characterized by a strong continuum due to the free charge carriers. Two weak and broad bands at 45 and 128 meV superimposed on this continuum are probably due to electronic excitations. In the energy loss spectrum of evaporated carbon films phonon creations predominate below 160 meV, where several well-separated peaks are observed. An energy loss at 370 meV is caused by a longitudinal band transition.