Thermal decay of Lennard-Jones clusters
International Nuclear Information System (INIS)
Garzon, I.L.; Avalos-Borja, M.
1989-01-01
The decay mechanisms of argon clusters have been studied using molecular dynamics simulations and Lennard-Jones potentials. Heating up processes were applied to Ar 13 up to temperatures in the melting region. In this range of temperatures large fluctuations in the mean kinetic energy of the system are present and a sequential evaporation is observed. The thermal decay of these aggregates occurs in a time scale of nanoseconds. (orig.)
Evaporation of Lennard-Jones clusters
International Nuclear Information System (INIS)
Roman, C.E.; Garzon, I.L.
1991-01-01
Extensive molecular dynamics simulations have been done to study the evaporation of a 13-atom Lennard-Jones cluster. The survival probability and the evaporative lifetime are calculated as a function of the cluster total energy from a classical trajectory analysis. The results are interpreted in terms of the RRK theory of unimolecular dissociation. The calculation of the binding energy of the evaporated species from the evaporation rate and the average kinetic energy release is discussed. (orig.)
Freezing of Lennard-Jones-type fluids
International Nuclear Information System (INIS)
Khrapak, Sergey A.; Chaudhuri, Manis; Morfill, Gregor E.
2011-01-01
We put forward an approximate method to locate the fluid-solid (freezing) phase transition in systems of classical particles interacting via a wide range of Lennard-Jones-type potentials. This method is based on the constancy of the properly normalized second derivative of the interaction potential (freezing indicator) along the freezing curve. As demonstrated recently it yields remarkably good agreement with previous numerical simulation studies of the conventional 12-6 Lennard-Jones (LJ) fluid [S.A.Khrapak, M.Chaudhuri, G.E.Morfill, Phys. Rev. B 134, 052101 (2010)]. In this paper, we test this approach using a wide range of the LJ-type potentials, including LJ n-6 and exp-6 models, and find that it remains sufficiently accurate and reliable in reproducing the corresponding freezing curves, down to the triple-point temperatures. One of the possible application of the method--estimation of the freezing conditions in complex (dusty) plasmas with ''tunable'' interactions--is briefly discussed.
Phase diagram of a modified Lennard-Jones system
International Nuclear Information System (INIS)
Sakagami, Takahiro; Fuchizaki, Kazuhiro
2010-01-01
The well-known Lennard-Jones potential is modified in such a way that it smoothly vanishes at a certain distance. A system whose interparticle interaction is given by such a potential is referred to as a modified Lennard-Jones system, and is served as a standard system describing simple solids and fluids. A phase diagram is determined based on the free energies obtained through thermodynamic integration.
Evaporation of Lennard-Jones fluids.
Cheng, Shengfeng; Lechman, Jeremy B; Plimpton, Steven J; Grest, Gary S
2011-06-14
Evaporation and condensation at a liquid/vapor interface are ubiquitous interphase mass and energy transfer phenomena that are still not well understood. We have carried out large scale molecular dynamics simulations of Lennard-Jones (LJ) fluids composed of monomers, dimers, or trimers to investigate these processes with molecular detail. For LJ monomers in contact with a vacuum, the evaporation rate is found to be very high with significant evaporative cooling and an accompanying density gradient in the liquid domain near the liquid/vapor interface. Increasing the chain length to just dimers significantly reduces the evaporation rate. We confirm that mechanical equilibrium plays a key role in determining the evaporation rate and the density and temperature profiles across the liquid/vapor interface. The velocity distributions of evaporated molecules and the evaporation and condensation coefficients are measured and compared to the predictions of an existing model based on kinetic theory of gases. Our results indicate that for both monatomic and polyatomic molecules, the evaporation and condensation coefficients are equal when systems are not far from equilibrium and smaller than one, and decrease with increasing temperature. For the same reduced temperature T/T(c), where T(c) is the critical temperature, these two coefficients are higher for LJ dimers and trimers than for monomers, in contrast to the traditional viewpoint that they are close to unity for monatomic molecules and decrease for polyatomic molecules. Furthermore, data for the two coefficients collapse onto a master curve when plotted against a translational length ratio between the liquid and vapor phase.
Scaling of the dynamics of flexible Lennard-Jones chains
DEFF Research Database (Denmark)
Veldhorst, Arno; Dyre, Jeppe C.; Schrøder, Thomas
2015-01-01
The previous paper [A. A. Veldhorst et al., J. Chem. Phys. 141, 054904 (2014)] demonstrated that the isomorph theory explains the scaling properties of a liquid of flexible chains consisting of ten Lennard-Jones particles connected by rigid bonds. We here investigate the same model with harmonic......, dynamics, and the excess entropy are invariant. The Lennard-Jones chain liquid with harmonic bondsdoes have curves in the phase diagram along which the structure and dynamics are invariant. The excess entropy is not invariant on these curves, which we refer to as “pseudoisomorphs.” In particular......, this means that Rosenfeld’s excess-entropy scaling (the dynamics being a function of excess entropy only) does not apply for the Lennard-Jones chain with harmonic bonds...
Cluster fusion algorithm: application to Lennard-Jones clusters
DEFF Research Database (Denmark)
Solov'yov, Ilia; Solov'yov, Andrey V.; Greiner, Walter
2006-01-01
paths up to the cluster size of 150 atoms. We demonstrate that in this way all known global minima structures of the Lennard-Jones clusters can be found. Our method provides an efficient tool for the calculation and analysis of atomic cluster structure. With its use we justify the magic number sequence......We present a new general theoretical framework for modelling the cluster structure and apply it to description of the Lennard-Jones clusters. Starting from the initial tetrahedral cluster configuration, adding new atoms to the system and absorbing its energy at each step, we find cluster growing...... for the clusters of noble gas atoms and compare it with experimental observations. We report the striking correspondence of the peaks in the dependence of the second derivative of the binding energy per atom on cluster size calculated for the chain of the Lennard-Jones clusters based on the icosahedral symmetry...
Cluster fusion algorithm: application to Lennard-Jones clusters
DEFF Research Database (Denmark)
Solov'yov, Ilia; Solov'yov, Andrey V.; Greiner, Walter
2008-01-01
paths up to the cluster size of 150 atoms. We demonstrate that in this way all known global minima structures of the Lennard-Jones clusters can be found. Our method provides an efficient tool for the calculation and analysis of atomic cluster structure. With its use we justify the magic number sequence......We present a new general theoretical framework for modelling the cluster structure and apply it to description of the Lennard-Jones clusters. Starting from the initial tetrahedral cluster configuration, adding new atoms to the system and absorbing its energy at each step, we find cluster growing...... for the clusters of noble gas atoms and compare it with experimental observations. We report the striking correspondence of the peaks in the dependence of the second derivative of the binding energy per atom on cluster size calculated for the chain of the Lennard-Jones clusters based on the icosahedral symmetry...
Free energy of the Lennard-Jones solid
Hoef, van der M.A.
2000-01-01
We have determined a simple expression for the absolute Helmholtz free energy of the fcc Lennard-Jones solid from molecular dynamics simulations. The pressure and energy data from these simulations have been fitted to a simple functional form (18 parameters) for densities ranging from around
Scaling of the dynamics of flexible Lennard-Jones chains
DEFF Research Database (Denmark)
Veldhorst, Arno; Dyre, J. C.; Schrøder, Thomas
2014-01-01
functions of excess entropy) which has been observed in simulations of both molecular and polymeric systems. Doing molecular dynamics simulations of flexible Lennard-Jones chains (LJC) with rigid bonds, we here provide the first detailed test of the isomorph theory applied to flexible chain molecules. We...
Thermal conductivity of the Lennard-Jones chain fluid model.
Galliero, Guillaume; Boned, Christian
2009-12-01
Nonequilibrium molecular dynamics simulations have been performed to estimate, analyze, and correlate the thermal conductivity of a fluid composed of short Lennard-Jones chains (up to 16 segments) over a large range of thermodynamic conditions. It is shown that the dilute gas contribution to the thermal conductivity decreases when the chain length increases for a given temperature. In dense states, simulation results indicate that the residual thermal conductivity of the monomer increases strongly with density, but is weakly dependent on the temperature. Compared to the monomer value, it has been noted that the residual thermal conductivity of the chain was slightly decreasing with its length. Using these results, an empirical relation, including a contribution due to the critical enhancement, is proposed to provide an accurate estimation of the thermal conductivity of the Lennard-Jones chain fluid model (up to 16 segments) over the domain 0.8values of the Lennard-Jones chain fluid model merge on the same "universal" curve when plotted as a function of the excess entropy. Furthermore, it is shown that the reduced configurational thermal conductivity of the Lennard-Jones chain fluid model is approximately proportional to the reduced excess entropy for all fluid states and all chain lengths.
Equilibrium spherically curved two-dimensional Lennard-Jones systems
Voogd, J.M.; Sloot, P.M.A.; van Dantzig, R.
2005-01-01
To learn about basic aspects of nano-scale spherical molecular shells during their formation, spherically curved two-dimensional N-particle Lennard-Jones systems are simulated, studying curvature evolution paths at zero-temperature. For many N-values (N < 800) equilibrium configu- rations are traced
Phase diagram of a Lennard-Jones solid
International Nuclear Information System (INIS)
Choi, Y.; Ree, T.; Ree, F.H.
1993-01-01
A phase diagram of a Lennard-Jones solid at kT/ε≥0.8 is constructed by our recent perturbation theory. It shows the stability of the face-centered-cubic phase except within a small pressure and temperature domain, where the hexagonal-close packed phase may occur. The theory predicts anharmonic contributions to the Helmholtz free energy (important to the crystal stability) in good agreement with Monte Carlo data
Melting of 2D monatomic solids: Lennard-Jones system
International Nuclear Information System (INIS)
Yi, Y.M.; Guo, Z.C.
1987-09-01
The Lennard-Jones interaction has been introduced into the Collins mix lattice of 2D liquids. By means of rigorous calculation of the total potential and the free area, the Gibbs functions for 2D liquid and solid have been derived. The melting line obtained from the phase transition equation agrees quite well with the result of recent computer simulation experiments. The obtained reduced temperature of the triple point T* t =0.438 agrees with the data measured in experiments of some inert gas monolayers adsorbed on graphite as well as in computer simulation experiments. (author). 11 refs, 7 figs, 3 tabs
Radiation damage in an amorphous Lennard-Jones solid
International Nuclear Information System (INIS)
Chaki, T.K.; Li, J.C.M.
1985-01-01
A molecular-dynamics simulation of radiation damage in an amorphous Lennard-Jones solid has been undertaken. A three-dimensional structure of 685 atoms with periodic boundary conditions was used. An atom was injected inward from the middle of one surface, and as it lost its energy its velocity and position were recorded. The temperature profile around the injection direction was also calculated. The amorphous structure was examined before and after irradiation by calculating the volume distribution of the Voronoi polyhedra and its time evolution. The production of vacancies and interstitials was observed. The interstitials were found to disappear rapidly, and the vacancies slowly. (author)
A Lennard-Jones-like perspective on first order transitions in biological helices
DEFF Research Database (Denmark)
Oskolkov, Nikolay N.; Bohr, Jakob
2013-01-01
Helical structures with Lennard-Jones self-interactions are studied for optimal conformations. For this purpose, their self-energy is analyzed for extrema with respect to the geometric parameters of the helices. It is found that Lennard-Jones helices exhibit a first order phase transition from...
Glass of monatomic Lennard-Jones system at nanoscale
International Nuclear Information System (INIS)
Vo Van Hoang
2010-01-01
Structure and stability of glass of monatomic Lennard-Jones (LJ) system at nanoscale compared with those of the bulk counterparts have been studied using the classical molecular dynamics (MD) method. Models have been obtained by cooling from the melts. Structure of the systems was analyzed via radial distribution function (RDF), interatomic distances, the Honeycutt-Andersen analysis and coordination number distributions. Surface and core structures of LJ nanoparticles have been analyzed in details. Density dependence and cooling rate effects on structure of the systems have been found and discussed. In addition, size dependence of structure and properties of nanoparticles has been analyzed in detail. Indeed, we found glass formation in monatomic LJ systems; however, their stability is not high. Evolution of structure and thermodynamics of the systems upon cooling from the melts was found. We also discussed annealing-induced crystallization of LJ glass.
Phase behavior of the 38-atom Lennard-Jones cluster
International Nuclear Information System (INIS)
Sehgal, Ray M.; Maroudas, Dimitrios; Ford, David M.
2014-01-01
We have developed a coarse-grained description of the phase behavior of the isolated 38-atom Lennard-Jones cluster (LJ 38 ). The model captures both the solid-solid polymorphic transitions at low temperatures and the complex cluster breakup and melting transitions at higher temperatures. For this coarse model development, we employ the manifold learning technique of diffusion mapping. The outcome of the diffusion mapping analysis over a broad temperature range indicates that two order parameters are sufficient to describe the cluster's phase behavior; we have chosen two such appropriate order parameters that are metrics of condensation and overall crystallinity. In this well-justified coarse-variable space, we calculate the cluster's free energy landscape (FEL) as a function of temperature, employing Monte Carlo umbrella sampling. These FELs are used to quantify the phase behavior and onsets of phase transitions of the LJ 38 cluster
Water in the presence of inert Lennard-Jones obstacles
Kurtjak, Mario; Urbic, Tomaz
2014-04-01
Water confined by the presence of a 'sea' of inert obstacles was examined. In the article, freely mobile two-dimensional Mercedes-Benz (MB) water put to a disordered, but fixed, matrix of Lennard-Jones disks was studied by the Monte Carlo computer simulations. For the MB water molecules in the matrix of Lennard-Jones disks, we explored the structures, hydrogen-bond-network formation and thermodynamics as a function of temperature and size and density of matrix particles. We found that the structure of model water is perturbed by the presence of the obstacles. Density of confined water, which was in equilibrium with the bulk water, was smaller than the density of the bulk water and the temperature dependence of the density of absorbed water did not show the density anomaly in the studied temperature range. The behaviour observed as a consequence of confinement is similar to that of increasing temperature, which can for a matrix lead to a process similar to capillary evaporation. At the same occupancy of space, smaller matrix molecules cause higher destruction effect on the absorbed water molecules than the bigger ones. We have also tested the hypothesis that at low matrix densities the obstacles induce an increased ordering and 'hydrogen bonding' of the MB model molecules, relative to pure fluid, while at high densities the obstacles reduce MB water structuring, as they prevent the fluid to form good 'hydrogen-bonding' networks. However, for the size of matrix molecules similar to that of water, we did not observe this effect.
Contact angle of sessile drops in Lennard-Jones systems.
Becker, Stefan; Urbassek, Herbert M; Horsch, Martin; Hasse, Hans
2014-11-18
Molecular dynamics simulations are used for studying the contact angle of nanoscale sessile drops on a planar solid wall in a system interacting via the truncated and shifted Lennard-Jones potential. The entire range between total wetting and dewetting is investigated by varying the solid-fluid dispersive interaction energy. The temperature is varied between the triple point and the critical temperature. A correlation is obtained for the contact angle in dependence of the temperature and the dispersive interaction energy. Size effects are studied by varying the number of fluid particles at otherwise constant conditions, using up to 150,000 particles. For particle numbers below 10,000, a decrease of the contact angle is found. This is attributed to a dependence of the solid-liquid surface tension on the droplet size. A convergence to a constant contact angle is observed for larger system sizes. The influence of the wall model is studied by varying the density of the wall. The effective solid-fluid dispersive interaction energy at a contact angle of θ = 90° is found to be independent of temperature and to decrease linearly with the solid density. A correlation is developed that describes the contact angle as a function of the dispersive interaction, the temperature, and the solid density. The density profile of the sessile drop and the surrounding vapor phase is described by a correlation combining a sigmoidal function and an oscillation term.
Longitudinal and bulk viscosities of Lennard-Jones fluids
Tankeshwar, K.; Pathak, K. N.; Ranganathan, S.
1996-12-01
Expressions for the longitudinal and bulk viscosities have been derived using Green Kubo formulae involving the time integral of the longitudinal and bulk stress autocorrelation functions. The time evolution of stress autocorrelation functions are determined using the Mori formalism and a memory function which is obtained from the Mori equation of motion. The memory function is of hyperbolic secant form and involves two parameters which are related to the microscopic sum rules of the respective autocorrelation function. We have derived expressions for the zeroth-, second-and fourth- order sum rules of the longitudinal and bulk stress autocorrelation functions. These involve static correlation functions up to four particles. The final expressions for these have been put in a form suitable for numerical calculations using low- order decoupling approximations. The numerical results have been obtained for the sum rules of longitudinal and bulk stress autocorrelation functions. These have been used to calculate the longitudinal and bulk viscosities and time evolution of the longitudinal stress autocorrelation function of the Lennard-Jones fluids over wide ranges of densities and temperatures. We have compared our results with the available computer simulation data and found reasonable agreement.
Vacancy behavior in a compressed fcc Lennard-Jones crystal
International Nuclear Information System (INIS)
Beeler, J.R. Jr.
1981-12-01
This computer experiment study concerns the determination of the stable vacancy configuration in a compressed fcc Lennard-Jones crystal and the migration of this defect in a compressed crystal. Isotropic and uniaxial compression stress conditions were studied. The isotropic and uniaxial compression magnitudes employed were 0.94 less than or equal to eta less than or equal to 1.5, and 1.0 less than or equal to eta less than or equal to 1.5, respectively. The site-centered vacancy (SCV) was the stable vacancy configuration whenever cubic symmetry was present. This includes all of the isotropic compression cases and the particular uniaxial compression case (eta = √2) that give a bcc structure. In addition, the SCV was the stable configuration for uniaxial compression eta 1.20, the SV-OP is an extended defect and, therefore, a saddle point for SV-OP migration could not be determined. The mechanism for the transformation from the SCV to the SV-OP as the stable form at eta = 1.29 appears to be an alternating sign [101] and/or [011] shear process
Phase diagram of power law and Lennard-Jones systems: Crystal phases
International Nuclear Information System (INIS)
Travesset, Alex
2014-01-01
An extensive characterization of the low temperature phase diagram of particles interacting with power law or Lennard-Jones potentials is provided from Lattice Dynamical Theory. For power law systems, only two lattice structures are stable for certain values of the exponent (or softness) (A15, body centered cube (bcc)) and two more (face centered cubic (fcc), hexagonal close packed (hcp)) are always stable. Among them, only the fcc and bcc are equilibrium states. For Lennard-Jones systems, the equilibrium states are either hcp or fcc, with a coexistence curve in pressure and temperature that shows reentrant behavior. The hcp solid never coexists with the liquid. In all cases analyzed, for both power law and Lennard-Jones potentials, the fcc crystal has higher entropy than the hcp. The role of anharmonic terms is thoroughly analyzed and a general thermodynamic integration to account for them is proposed
Simulation of depositions of a Lennard-Jones cluster on a crystalline surface
International Nuclear Information System (INIS)
Saitoh, Kuniyasu; Hayakawa, Hisao
2009-01-01
Depositions of amorphous Lennard-Jones clusters on a crystalline surface are numerically investigated. From the results of the molecular dynamics simulation, we found that the deposited clusters exhibit a transition from multilayered adsorption to monolayered adsorption at a critical incident speed. Employing the energy conservation law, we can explain the behavior of the ratio of the number of atoms adsorbed on the substrate to the cluster size. The boundary shape of the deposited cluster depends strongly on the incident speed, and some unstable modes grow during the spread of the deposited cluster on the substrate. We also discuss the wettability between different Lennard-Jones atoms. (author)
RISM theory distribution functions for Lennard--Jones interaction site fluids
International Nuclear Information System (INIS)
Johnson, E.; Hazoume, R.P.
1978-01-01
Reference interaction site model (RISM) theory distribution functions for Lennard-Jones interaction site fluids are discussed. The comparison with computer simulation results suggests that these distribution functions are as accurate as RISM distribution functions for fused hard sphere molecular fluids
Formation of global energy minimim structures in the growth process of Lennard-Jones clusters
DEFF Research Database (Denmark)
Solov'yov, Ilia; Koshelev, Andrey; Shutovich, Andrey
2003-01-01
that in this way all known global minimum structures of the Lennard-Jones (LJ) clusters can be found. Our method provides an efficient tool for the calculation and analysis of atomic cluster structure. With its use we justify the magic numbers sequence for the clusters of noble gases atoms and compare...
Application of the RISM theory to Lennard-Jones interaction site molecular fluids
International Nuclear Information System (INIS)
Johnson, E.; Hazoume, R.P.
1979-01-01
It seems that reference interaction site model (RISM) theory atom--atom distribution functions have been obtained directly from the RISM equations only for fused hard sphere molecular fluids. RISM distribution functions for Lennard-Jones interaction site fluids are presented. Results presented suggest that these distribution functions are as accurate as RISM distribution functions for fused hard sphere molecular fluids
Atomic size effect on the formation of ionized cluster beam epitaxy in Lennard-Jones systems
International Nuclear Information System (INIS)
Hsieh Horngming; Averback, R.S.
1991-01-01
Ionized cluster beam deposition is studied by molecular dynamics simulations in which the atomic size of incident cluster atoms is different from the size of substrate atoms. Lennard-Jones interatomic potentials are used for the two-component system. The results provide the morphologies of the overlayers for various atomic sizes and are compared to simulation results of molecular beam epitaxy. (orig.)
DEFF Research Database (Denmark)
D'ovidio, Francesco; Bohr, Henrik; Lindgård, Per-Anker
2005-01-01
We study the propagation of solitons along the hydrogen bonds of an alpha helix. Modeling the hydrogen and peptide bonds with Lennard-Jones potentials, we show that the solitons can appear spontaneously and have long lifetimes. Remarkably, even if no explicit solution is known for the Lennard-Jones...... potential, the solitons can be characterized analytically with a good quantitative agreement using formulas for a Toda potential with parameters fitted to the Lennard-Jones potential. We also discuss and show the robustness of the family of periodic solutions called cnoidal waves, corresponding to phonons...
Molecular dynamics study of the hydration of Lennard-Jones solutes
International Nuclear Information System (INIS)
Geiger, A.; Rahman, A.; Stillinger, F.H.
1979-01-01
In order to clarify the nature of hydrophobic interactions in water, we have used the molecular dynamics simulation method to study a system comprising two Lennard-Jones solute particles and 214 water molecules. Although the solutes were placed initially in contact, forces in the system drive them slightly apart to permit formation of vertex-sharing solvent ''cages.'' Definite orientational preferences have been observed for water molecules in the first solvation layer around the Lennard-Jones solutes; these preferences are loosely reminiscent of structure in clathrates. Nevertheless, substantial local disorder is obviously present. The dynamical data show that translational and rotational motions of solvation--sheath water molecules are perceptibly slower (by at least 20%) than those in pure bulk water
Collision kernels in the eikonal approximation for Lennard-Jones interaction potential
International Nuclear Information System (INIS)
Zielinska, S.
1985-03-01
The velocity changing collisions are conveniently described by collisional kernels. These kernels depend on an interaction potential and there is a necessity for evaluating them for realistic interatomic potentials. Using the collision kernels, we are able to investigate the redistribution of atomic population's caused by the laser light and velocity changing collisions. In this paper we present the method of evaluating the collision kernels in the eikonal approximation. We discuss the influence of the potential parameters Rsub(o)sup(i), epsilonsub(o)sup(i) on kernel width for a given atomic state. It turns out that unlike the collision kernel for the hard sphere model of scattering the Lennard-Jones kernel is not so sensitive to changes of Rsub(o)sup(i) as the previous one. Contrary to the general tendency of approximating collisional kernels by the Gaussian curve, kernels for the Lennard-Jones potential do not exhibit such a behaviour. (author)
Fluctuations and thermodynamic response functions in a Lennard-Jones solid
International Nuclear Information System (INIS)
Li, M.; Johnson, W.L.
1992-01-01
Thermodynamic response functions of a nearest-neighbor Lennard-Jones solid--heat capacity, thermal-expansion coefficient, compressibility, and elastic constants--are calculated directly from fluctuations using molecular-dynamics simulations. The algorithm used is the earlier Parrinello-Rahman molecular dynamics modified to take into account symmetry and rotation invariance of the system under investigation. The convergence is very fast and results are in good agreement with existing Monte Carlo and molecular-dynamics results
Melting in Two-Dimensional Lennard-Jones Systems: Observation of a Metastable Hexatic Phase
International Nuclear Information System (INIS)
Chen, K.; Kaplan, T.; Mostoller, M.
1995-01-01
Large scale molecular dynamics simulations of two-dimensional melting have been carried out using a recently revised Parrinello-Rahman scheme on massively parallel supercomputers. A metastable state is observed between the solid and liquid phases in Lennard-Jones systems of 36 864 and 102 400 atoms. This intermediate state shows the characteristics of the hexatic phase predicted by the theory of Kosterlitz, Thouless, Halperin, Nelson, and Young
Dynamics of an assembly of finite-size Lennard-Jones spheres
International Nuclear Information System (INIS)
Singh, P.
1996-01-01
The time-averaged Fourier spectra of the number density, velocity, and force fields are obtained numerically for an assembly of spherical particles interacting via the Lennard-Jones potential. The magnitude spectra determine the dominant wave numbers, and the phase difference between the Lennard-Jones force and number density spectra determines the nature of the particle dynamics. The latter is used to show that for every wave number k there is a critical frequency ω c (k), such that when ω c (k) the phase difference is π/2 and when ω approx-gt ω c (k) the phase difference is -π/2. The ratio of the frequency and the wave number at which the phase difference changes sign is used to define an effective sound speed for the particle system. The effective sound speed is shown to be a function of the dimensionless wave number, and is locally minimum at the same dimensionless wave numbers for which the static structure factor is minimum. It is also shown that the dynamical response of the particle system for waves with speeds greater than the effective sound speed is similar to the response of the hyperbolic systems of equations, and for waves with speeds smaller than the effective sound speed the response is similar to the response of the elliptic systems. The convection effects are shown to be of the same order of magnitude as the Lennard-Jones forces, and the change of type of the equations from hyperbolic to elliptic occurs when the magnitude of the convection term is comparable to the magnitude of the Lennard-Jones force term. It is also shown that the change of type cannot occur in a theory where the convection term is neglected. copyright 1996 The American Physical Society
Stability of relaxed Lennard-Jones models made of 500 to 6000 atoms
International Nuclear Information System (INIS)
Raoult, B.; Farges, J.; Feraudy, M.F. de; Torchet, G.
1989-01-01
We present a study of the stability of clusters models made of a number N of atoms in the range 500 to 6000 atoms, freely interacting through the Lennard-Jones potential. The potential energy per atom, calculated for relaxed models, shows that stable models belong to an icosahedral sequence when N<1600 and to a decahedral sequence beyond. A coexistence size range of both structures is discussed in connection with experimental results on argon clusters in free jet expansions. (orig.)
Effect of Energy Polydispersity on the Nature of Lennard-Jones Liquids
Ingebrigtsen, Trond S.; Tanaka, Hajime
2016-01-01
In the companion paper [T. S. Ingebrigtsen and H. Tanaka, J. Phys. Chem. B 119, 11052 (2015)] the effect of size polydispersity on the nature of Lennard-Jones (LJ) liquids, which represent most molecular liquids without hydrogen bonds, was studied. More specifically, it was shown that even highly size polydisperse LJ liquids are Roskilde-simple (RS) liquids. RS liquids are liquids with strong correlation between constant volume equilibrium fluctuations of virial and potential energy and are s...
Metastability, spectrum, and eigencurrents of the Lennard-Jones-38 network
International Nuclear Information System (INIS)
Cameron, Maria K.
2014-01-01
We develop computational tools for spectral analysis of stochastic networks representing energy landscapes of atomic and molecular clusters. Physical meaning and some properties of eigenvalues, left and right eigenvectors, and eigencurrents are discussed. We propose an approach to compute a collection of eigenpairs and corresponding eigencurrents describing the most important relaxation processes taking place in the system on its way to the equilibrium. It is suitable for large and complex stochastic networks where pairwise transition rates, given by the Arrhenius law, vary by orders of magnitude. The proposed methodology is applied to the network representing the Lennard-Jones-38 cluster created by Wales's group. Its energy landscape has a double funnel structure with a deep and narrow face-centered cubic funnel and a shallower and wider icosahedral funnel. However, the complete spectrum of the generator matrix of the Lennard-Jones-38 network has no appreciable spectral gap separating the eigenvalue corresponding to the escape from the icosahedral funnel. We provide a detailed description of the escape process from the icosahedral funnel using the eigencurrent and demonstrate a superexponential growth of the corresponding eigenvalue. The proposed spectral approach is compared to the methodology of the Transition Path Theory. Finally, we discuss whether the Lennard-Jones-38 cluster is metastable from the points of view of a mathematician and a chemical physicist, and make a connection with experimental works
Analytic Debye-Grüneisen equation of state for a generalized Lennard-Jones solids
Institute of Scientific and Technical Information of China (English)
孙久勋; 吴强; 蔡灵仓; 经福谦
2003-01-01
The approximate method to treat the practical quantum anharmonic solids proposed by Hardy,Lacks and Shukla is reformulated with explicit physical meanings.It is shown that the quantum effect is important at low temperature,it can be treated in the harmonic framework; and the anharmonic effect is important at high temperature and tends to zero at low temperature,it can be treated by using a classical approximation.The alternative formulation is easier for various applications,and is applied to a Debye-Gruneisen solid with the generalized Lennard-Jones intermolecular interaction.The expressions for the Debye temperature and Gruneisen parameter as a function of volume are analytically derived.The analytic equation of state is applied to predict the thermodynamic properties of solid xenon at normal-pressure with the nearest-neighbour Lennard-Jones interaction,and is further applied to research the properties of solid xenon and krypton at high pressure by using an all-neighbour Lennard-Jones interaction.The theoretical results are in agreement with the experiments.
Reinisch, S; Schweiger, K; Pablik, E; Collet-Fenetrier, B; Peyrin-Biroulet, L; Alfaro, I; Panés, J; Moayyedi, P; Reinisch, W
2016-09-01
The Lennard-Jones criteria are considered the gold standard for diagnosing Crohn's disease (CD) and include the items granuloma, macroscopic discontinuity, transmural inflammation, fibrosis, lymphoid aggregates and discontinuous inflammation on histology. The criteria have never been subjected to a formal validation process. To develop a validated and improved diagnostic index based on the items of Lennard-Jones criteria. Included were 328 adult patients with long-standing CD (median disease duration 10 years) from three centres and classified as 'established', 'probable' or 'non-CD' by Lennard-Jones criteria at time of diagnosis. Controls were patients with ulcerative colitis (n = 170). The performance of each of the six diagnostic items of Lennard-Jones criteria was modelled by logistic regression and a new index based on stepwise backward selection and cut-offs was developed. The diagnostic value of the new index was analysed by comparing sensitivity, specificity and accuracy vs. Lennard-Jones criteria. By Lennard-Jones criteria 49% (n = 162) of CD patients would have been diagnosed as 'non-CD' at time of diagnosis (sensitivity/specificity/accuracy, 'established' CD: 0.34/0.99/0.67; 'probable' CD: 0.51/0.95/0.73). A new index was derived from granuloma, fibrosis, transmural inflammation and macroscopic discontinuity, but excluded lymphoid aggregates and discontinuous inflammation on histology. Our index provided improved diagnostic accuracy for 'established' and 'probable' CD (sensitivity/specificity/accuracy, 'established' CD: 0.45/1/0.72; 'probable' CD: 0.8/0.85/0.82), including the subgroup isolated colonic CD ('probable' CD, new index: 0.73/0.85/0.79; Lennard-Jones criteria: 0.43/0.95/0.69). We developed an index based on items of Lennard-Jones criteria providing improved diagnostic accuracy for the differential diagnosis between CD and UC. © 2016 John Wiley & Sons Ltd.
Numerical simulation of pool boiling of a Lennard-Jones liquid
Inaoka, Hajime
2013-09-01
We performed a numerical simulation of pool boiling by a molecular dynamics model. In the simulation, a liquid composed of Lennard-Jones particles in a uniform gravitational field is heated by a heat source at the bottom of the system. The model successfully reproduces the change in regimes of boiling from nucleate boiling to film boiling with the increase of the heat source temperature. We present the pool boiling curve by the model, whose general behavior is consistent with those observed in experiments of pool boiling. © 2013 Elsevier B.V. All rights reserved.
Numerical simulation of pool boiling of a Lennard-Jones liquid
Inaoka, Hajime; Ito, Nobuyasu
2013-01-01
We performed a numerical simulation of pool boiling by a molecular dynamics model. In the simulation, a liquid composed of Lennard-Jones particles in a uniform gravitational field is heated by a heat source at the bottom of the system. The model successfully reproduces the change in regimes of boiling from nucleate boiling to film boiling with the increase of the heat source temperature. We present the pool boiling curve by the model, whose general behavior is consistent with those observed in experiments of pool boiling. © 2013 Elsevier B.V. All rights reserved.
Cell-model prediction of the melting of a Lennard-Jones solid
International Nuclear Information System (INIS)
Holian, B.L.
1980-01-01
The classical free energy of the Lennard-Jones 6-12 solid is computed from a single-particle anharmonic cell model with a correction to the entropy given by the classical correlational entropy of quasiharmonic lattice dynamics. The free energy of the fluid is obtained from the Hansen-Ree analytic fit to Monte Carlo equation-of-state calculations. The resulting predictions of the solid-fluid coexistence curves by this corrected cell model of the solid are in excellent agreement with the computer experiments
Third-order WKBJ eigenvalues for Lennard-Jones and Varshni V potentials
International Nuclear Information System (INIS)
Kesarwani, R.N.; Varshni, Y.P.
1978-01-01
The WKBJ method is applied to the third order for obtaining the eigenvalues for the fifth potential of Varshni, and the relevant integrals are analytically evaluated. Numerical results are obtained for the Lennard-Jones Potential, which is a special case of the Varshni V potential, and are compared to the results of Harrison and Bernstein obtained by a numerical integration of the wave equation. Error estimates are made. It is shown that for diatomic potentials, the Langer correction is not needed if the WKBJ approximation is carried to second and higher orders. (author)
Self-diffusion coefficients of the metastable Lennard-Jones vapor
International Nuclear Information System (INIS)
Nie Chu; Zhou Youhua; Marlow, W H; Hassan, Y A
2008-01-01
Self-diffusion coefficients of a metastable Lennard-Jones vapor were obtained using the memory function formalism and the frequency moments of the velocity autocorrelation function at reduced temperatures from 0.75 to 1.0. The radial density distribution functions used to evaluate the second, fourth and sixth frequency moments of the velocity autocorrelation function were obtained from the restricted canonical ensemble Monte Carlo simulation (Corti and Debenedetti 1994 Chem. Eng. Sci. 49 2717). The self-diffusion coefficients at reduced temperature 0.75 do not vary monotonically as the density increases, and for the other three temperatures the self-diffusion coefficients vary normally
Self-diffusion coefficients of the metastable Lennard-Jones vapor
Energy Technology Data Exchange (ETDEWEB)
Nie Chu; Zhou Youhua [School of Physics and Information Engineering, Jianghan University, Wuhan 430056 (China); Marlow, W H; Hassan, Y A [Department of Nuclear Engineering, Texas A and M University, College Station, TX 77843 (United States)], E-mail: yhzhou@jhun.edu.cn
2008-10-15
Self-diffusion coefficients of a metastable Lennard-Jones vapor were obtained using the memory function formalism and the frequency moments of the velocity autocorrelation function at reduced temperatures from 0.75 to 1.0. The radial density distribution functions used to evaluate the second, fourth and sixth frequency moments of the velocity autocorrelation function were obtained from the restricted canonical ensemble Monte Carlo simulation (Corti and Debenedetti 1994 Chem. Eng. Sci. 49 2717). The self-diffusion coefficients at reduced temperature 0.75 do not vary monotonically as the density increases, and for the other three temperatures the self-diffusion coefficients vary normally.
Evidence of hexatic phase formation in two-dimensional Lennard-Jones binary arrays
International Nuclear Information System (INIS)
Li, M.; Johnson, W.L.; Goddard, W.A. III
1996-01-01
We report evidence of the hexatic phase formation in Lennard-Jones binary substitutional random arrays from isothermal-isobaric molecular-dynamics simulations. The hexatic phase is analogous to those predicted in Kosterlitz-Thouless theory of melting that is characterized by short-range translational order and quasi-long-range orientational order. At the crystal to hexatic phase transition, dislocation pairs are observed to unbind into isolated dislocations. Further disordering of the hexatic phase, however, does not lead to dissociation of dislocations into disclinations. Instead, the dislocations become clustered and form dislocation networks which results in formation of amorphous phases. copyright 1996 The American Physical Society
Crystallisation of a Lennard-Jones fluid by large scale molecular dynamics simulation
International Nuclear Information System (INIS)
Snook, I.
1998-01-01
Full text: The evolution of the structure of a large system of atoms interacting via a Lennard-Jones pair potential was simulated by the use of the Molecular Dynamics computer simulation technique. The system was initially equilibrated in the one phase region of the phase diagram at a temperature above critical then a temperature quench was performed which placed the system in a region were the single fluid phase was unstable. Quenches to below the triple point temperature gave rise to crystallisation The mechanism and final morphology is shown to depend strongly on the starting conditions e.g. the starting density
The potential energy landscape in the Lennard-Jones binary mixture model
International Nuclear Information System (INIS)
Sampoli, M; Benassi, P; Eramo, R; Angelani, L; Ruocco, G
2003-01-01
The potential energy landscape in the Kob-Andersen Lennard-Jones binary mixture model has been studied carefully from the liquid down to the supercooled regime, from T = 2 down to 0.46. One thousand independent configurations along the time evolution locus have been examined at each temperature investigated. From the starting configuration, we searched for the nearest saddle (or quasi-saddle) and minimum of the potential energy. The vibrational densities of states for the starting and the two derived configurations have been evaluated. Besides the number of negative eigenvalues of the saddles other quantities show some signature of the approach of the dynamical arrest temperature
Molecular dynamics studies of the dynamics of supercooled Lennard-Jones liquids
International Nuclear Information System (INIS)
De Leeuw, S.W.; Brakkee, M.J.D.
1990-01-01
Results are presented of molecular dynamics experiments, in which the Lennard-Jones liquid is cooled isobarically into the metastable temperature region below the freezing temperature. The variation of the density-density and transverse current correlation functions with temperature is studied. We observed a power-law behaviour for the temperature dependence of dynamical properties (viscosity and coefficienty of self-diffusion) with an exponent in good agreement with prediction of mode coupling theories and recent experimental results. (author). 23 refs, 5 figs
Nonlinear transport processes and fluid dynamics: Cylindrical Couette flow of Lennard-Jones fluids
International Nuclear Information System (INIS)
Khayat, R.E.; Eu, B.C.
1988-01-01
In this paper we report on calculations of flow profiles for cylindrical Couette flow of a Lennard-Jones fluid. The flow is subjected to a temperature gradient and thermoviscous effects are taken into consideration. We apply the generalized fluid dynamic equations which are provided by the modified moment method for the Boltzmann equation reported previously. The results of calculations are in good agreement with the Monte Carlo direct simulation method by K. Nanbu [Phys. Fluids 27, 2632 (1984)] for most of Knudsen numbers for which the simulation data are available
International Nuclear Information System (INIS)
Kim, Soon-Chul; Lee, Song Hi
2004-01-01
A density functional perturbation approximation (DFPT), which is based both on the fundamental-measure theory (FMT) to the hard-sphere repulsion and on the weighted-density approximations (WDAs) to the attractive contribution, has been proposed for studying the structural properties of model fluids with an attractive part of the potential. The advantage of the present theory is the simplicity of the calculation of the weight function due to the attractive contribution. It has been applied to predict the equilibrium particle density distributions and adsorption isotherms of Lennard-Jones fluids at interfaces. The theoretical results show that the present theory describes quite well the adsorption isotherms of a Lennard-Jones ethane in a graphite slit pore as well as the equilibrium particle density distributions of a Lennard-Jones fluid near a planar slit pore
Phase Diagram of Kob-Andersen-Type Binary Lennard-Jones Mixtures
Pedersen, Ulf R.; Schrøder, Thomas B.; Dyre, Jeppe C.
2018-04-01
The binary Kob-Andersen (KA) Lennard-Jones mixture is the standard model for computational studies of viscous liquids and the glass transition. For very long simulations, the viscous KA system crystallizes, however, by phase separating into a pure A particle phase forming a fcc crystal. We present the thermodynamic phase diagram for KA-type mixtures consisting of up to 50% small (B ) particles showing, in particular, that the melting temperature of the standard KA system at liquid density 1.2 is 1.028(3) in A particle Lennard-Jones units. At large B particle concentrations, the system crystallizes into the CsCl crystal structure. The eutectic corresponding to the fcc and CsCl structures is cutoff in a narrow interval of B particle concentrations around 26% at which the bipyramidal orthorhombic PuBr3 structure is the thermodynamically stable phase. The melting temperature's variation with B particle concentration at two constant pressures, as well as at the constant density 1.2, is estimated from simulations at pressure 10.19 using isomorph theory. Our data demonstrate approximate identity between the melting temperature and the onset temperature below which viscous dynamics appears. Finally, the nature of the solid-liquid interface is briefly discussed.
International Nuclear Information System (INIS)
Vorob'ev, V.S.
2003-01-01
We suggest a concept of multiple disordering scaling of the crystalline state. Such a scaling procedure applied to a crystal leads to the liquid and (in low density limit) gas states. This approach provides an explanation to a high value of configuration (common) entropy of liquefied noble gases, which can be deduced from experimental data. We use the generalized nearest-neighbor approach to calculate free energy and pressure of the Lennard-Jones systems after performing this scaling procedure. These thermodynamic functions depend on one parameter characterizing the disordering only. Condensed states of the system (liquid and solid) correspond to small values of this parameter. When this parameter tends to unity, we get an asymptotically exact equation of state for a gas involving the second virial coefficient. A reasonable choice of the values for the disordering parameter (ranging between zero and unity) allows us to find the lines of coexistence between different phase states in the Lennard-Jones systems, which are in a good agreement with the available experimental data
Glass transitions in one-, two-, three-, and four-dimensional binary Lennard-Jones systems
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Bruening, Ralf; St-Onge, Denis A; Patterson, Steve [Physics Department, Mount Allison University, Sackville, NB, E4L 1E6 (Canada); Kob, Walter [Laboratoire des Colloides, Verres et Nanomateriaux, UMR5587, Universite Montpellier II and CNRS, 34095 Montpellier Cedex (France)], E-mail: rbruening@mta.ca
2009-01-21
We investigate the calorimetric liquid-glass transition by performing simulations of a binary Lennard-Jones mixture in one through four dimensions. Starting at a high temperature, the systems are cooled to T = 0 and heated back to the ergodic liquid state at constant rates. Glass transitions are observed in two, three and four dimensions as a hysteresis between the cooling and heating curves. This hysteresis appears in the energy and pressure diagrams, and the scanning rate dependence of the area and height of the hysteresis can be described using power laws. The one-dimensional system does not experience a glass transition but its specific heat curve resembles the shape of the D{>=}2 results in the supercooled liquid regime above the glass transition. As D increases, the radial distribution functions reflect reduced geometric constraints. Nearest neighbor distances become smaller with increasing D due to interactions between nearest and next-nearest neighbors. Simulation data for the glasses are compared with crystal and melting data obtained with a Lennard-Jones system with only one type of particle and we find that with increasing D crystallization becomes increasingly more difficult.
Energy Technology Data Exchange (ETDEWEB)
Barbante, Paolo [Dipartimento di Matematica, Politecnico di Milano - Piazza Leonardo da Vinci 32 - 20133 Milano (Italy); Frezzotti, Aldo; Gibelli, Livio [Dipartimento di Scienze e Tecnologie Aerospaziali, Politecnico di Milano - Via La Masa 34 - 20156 Milano (Italy)
2014-12-09
The unsteady evaporation of a thin planar liquid film is studied by molecular dynamics simulations of Lennard-Jones fluid. The obtained results are compared with the predictions of a diffuse interface model in which capillary Korteweg contributions are added to hydrodynamic equations, in order to obtain a unified description of the liquid bulk, liquid-vapor interface and vapor region. Particular care has been taken in constructing a diffuse interface model matching the thermodynamic and transport properties of the Lennard-Jones fluid. The comparison of diffuse interface model and molecular dynamics results shows that, although good agreement is obtained in equilibrium conditions, remarkable deviations of diffuse interface model predictions from the reference molecular dynamics results are observed in the simulation of liquid film evaporation. It is also observed that molecular dynamics results are in good agreement with preliminary results obtained from a composite model which describes the liquid film by a standard hydrodynamic model and the vapor by the Boltzmann equation. The two mathematical model models are connected by kinetic boundary conditions assuming unit evaporation coefficient.
Icosahedral binary clusters of glass-forming Lennard-Jones binary alloy
International Nuclear Information System (INIS)
Iwamatsu, Masao
2007-01-01
It is widely believed that the local icosahedral structure is related to the formation of bulk metallic glasses (BMGs). Specifically the existence of 13-atom icosahedral cluster in undercooled liquid is imagined to play a key role to initiate the glass formation as the seed of amorphous structure or to block the nucleation of regular crystal as the impurity. The existence of 13-atom icosahedral clusters in one-component liquids was predicted more than half a century ago by Frank from his total energy calculation for isolated clusters. In BMG alloys, however, the situation is less clear. In this report, we present the lowest-energy structures of 13-atom Lennard-Jones binary cluster calculated from the modified space-fixed genetic algorithm. We study, in particular, the artificial Lennard-Jones potential designed by Kob and Andersen [W. Kob, H.C. Andersen, Phys. Rev. E 51 (1995) 4626] that is known to form BMG. Curiously, the lowest-energy structures of 13-atom cluster are non-icosahedral for almost all compositions. Our result suggests that the existence of the icosahedral cluster is not a necessary condition but only a sufficient condition for glass formation
Binding energy of large icosahedral and cuboctahedral Lennard-Jones clusters
International Nuclear Information System (INIS)
Northby, J.A.; Xie, J.
1989-01-01
It is widely believed that the lowest energy configurations for small rare gas clusters have icosahedral symmetry. This contrasts with the bulk crystal structures which have cuboctahedral fcc symmetry. It is of interest to understand the transition between this finite and bulk behavior. To model this transition in rare gas clusters we have undertaken optimization studies within the Lennard-Jones pair potential model. Using a combination of Monte Carlo and Partan Search optimization methods, the lowest energy relaxed structures of Lennard-Jones clusters having icosahedral and cuboctahedral symmetry were found. Studies were performed for complete shell clusters ranging in size from one shell having 13 atoms to 14 shells having 10,179 atoms. It was found that the icosahedral structures are lower in energy than the cuboctahedral structures for cluster sizes having 13 shells or fewer. Additional studies were performed using the more accurate Aziz-Chen [HFD-C] pair potential parameterized for argon. The conclusions appear to be relatively insensitive to the form of the potential. (orig.)
An accurate expression for radial distribution function of the Lennard-Jones fluid
International Nuclear Information System (INIS)
Morsali, Ali; Goharshadi, Elaheh K.; Ali Mansoori, G.; Abbaspour, Mohsen
2005-01-01
A simple and accurate expression for radial distribution function (RDF) of the Lennard-Jones fluid is presented. The expression explicitly states the RDF as a continuous function of reduced interparticle distance, temperature, and density. It satisfies the limiting conditions of zero density and infinite distance imposed by statistical thermodynamics. The distance dependence of this expression is expressed by an equation which contains 11 adjustable parameters. These parameters are fitted to 353 RDF data, obtained by molecular dynamics calculations, and then expressed as functions of reduced distance, temperature and density. This expression, having a total of 65 constants, reproduces the RDF data with an average root-mean-squared deviation of 0.0152 for the range of state variables of 0.5= * = * = * =ρσ 3 are reduced temperature and density, respectively). The expression predicts the pressure and the internal energy of the Lennard-Jones fluid with an uncertainty that is comparable to that obtained directly from the molecular dynamics simulations
DEFF Research Database (Denmark)
Cotterill, Rodney M J; Madsen, J.
1986-01-01
Sections of configuration space for Lennard-Jones matter were obtained by probing all the normal-mode energy profiles, following diagonalization of the dynamical matrix for a 240-particle system. For the crystal and sufficiently cold glass, these are single welled, whereas increasing numbers...... of double wells occur as the glass is warmed toward the fluid. This indicates that there might be a fundamental difference between the topologies of the constant-potential-energy hypersurfaces of crystalline and noncrystalline Lennard-Jones matter....
DEFF Research Database (Denmark)
Friisberg, Ida Marie; Costigliola, Lorenzo; Dyre, Jeppe C.
2017-01-01
This paper investigates the relation between the density-scaling exponent γ and the virial potentialenergy coefficient R at several thermodynamic state points in three dimensions for the generalized (2n, n) Lennard-Jones (LJ) system for n = 4, 9, 12, 18, as well as for the standard n = 6 LJ syste...
Viscous Growth in Spinodal Decomposition of the Two-component Lennard-Jones Model in Two Dimensions
DEFF Research Database (Denmark)
Laradji, M.; Toxvaerd, S.; Mouritsen, Ole G.
1997-01-01
The dynamics of phase separation of a two-component Lennard-Jones model in three dimensions is investigated by means of large scale molecular dynamics simulation. A systematic study over a wide range of quench temperatures within the coexistence region shows that the binary system reaches...
The Monte Carlo dynamics of a binary Lennard-Jones glass-forming mixture
International Nuclear Information System (INIS)
Berthier, L; Kob, W
2007-01-01
We use a standard Monte Carlo algorithm to study the slow dynamics of a binary Lennard-Jones glass-forming mixture at low temperature. We find that the Monte Carlo approach is by far the most efficient way to simulate a stochastic dynamics since the relaxation is about 10 times faster than in Brownian dynamics and about 30 times faster than in stochastic dynamics. Moreover, the average dynamical behaviour of the system is in quantitative agreement with that obtained using Newtonian dynamics, apart from at very short times where thermal vibrations are suppressed. We show, however, that dynamic fluctuations quantified by four-point dynamic susceptibilities do retain a dependence on the microscopic dynamics, as recently predicted theoretically
The effect of atom mismatch on the fragility of supercooled Lennard-Jones binary mixtures
International Nuclear Information System (INIS)
Sun Minhua; Sun Yongli; Wang Aiping; Ma Congxiao; Li Jiayun; Cheng Weidong; Liu Fang
2006-01-01
The shear viscosity of the well-known binary Lennard-Jones mixture is simulated under constant temperature and constant volume conditions (NVT) by a molecular-dynamics (MD) method. The effect of atomic size mismatch on the fragility parameter and glass-forming ability is studied. The fragility parameters calculated from shear viscosity data decrease with the increment of the atomic size mismatch. The value of the fragility changes from 168.963 to 22.976 when the mismatch changes from 0.023 to 0.25. It is shown that the fragility parameter is sensitive to the atomic size mismatch. The calculated pair distribution functions and mean square displacements indicate that the glass-forming ability increases with the atomic size mismatch
Dynamics of vacancies in two-dimensional Lennard-Jones crystals
Yao, Zhenwei; Olvera de La Cruz, Monica
2015-03-01
Vacancies represent an important class of crystallographic defects, and their behaviors can be strongly coupled with relevant material properties. We report the rich dynamics of vacancies in two-dimensional Lennard-Jones crystals in several thermodynamic states. Specifically, we numerically observe significantly faster diffusion of the 2-point vacancy with two missing particles in comparison with other types of vacancies; it opens the possibility of doping 2-point vacancies into atomic materials to enhance atomic migration. In addition, the resulting dislocations in the healing of a long vacancy suggest the intimate connection between vacancies and topological defects that may provide an extra dimension in the engineering of defects in extensive crystalline materials for desired properties. We thank the financial support from the U.S. Department of Commerce, National Institute of Standards and Technology, the Office of the Director of Defense Research and Engineering (DDR&E) and the Air Force Office of Scientific Research.
Theoretical prediction of crystallization kinetics of a supercooled Lennard-Jones fluid
Gunawardana, K. G. S. H.; Song, Xueyu
2018-05-01
The first order curvature correction to the crystal-liquid interfacial free energy is calculated using a theoretical model based on the interfacial excess thermodynamic properties. The correction parameter (δ), which is analogous to the Tolman length at a liquid-vapor interface, is found to be 0.48 ± 0.05 for a Lennard-Jones (LJ) fluid. We show that this curvature correction is crucial in predicting the nucleation barrier when the size of the crystal nucleus is small. The thermodynamic driving force (Δμ) corresponding to available simulated nucleation conditions is also calculated by combining the simulated data with a classical density functional theory. In this paper, we show that the classical nucleation theory is capable of predicting the nucleation barrier with excellent agreement to the simulated results when the curvature correction to the interfacial free energy is accounted for.
Thermal conductivity of the Lennard-Jones fluid: An empirical correlation
International Nuclear Information System (INIS)
Bugel, Mathilde; Galliero, Guillaume
2008-01-01
In this work, is presented an empirical correlation on the thermal conductivity of the Lennard-Jones fluid based on extensive non-equilibrium molecular dynamics simulations results (103 points). Finite size and cutoff radius effects are investigated and taken into account to develop the correlation. This last, composed of low-density, residual and critical enhancement contributions, is built for a wide range of thermodynamics states, even at the vicinity of the critical point, and yields an average absolute deviation of 1.29% compared to our simulations. In addition, a careful analysis of the different contributions to the microscopic flux is carried out which sheds light on the underlying mechanism of the results. Finally, are discussed the limitations of the proposed model when applied to real simple fluids and mixtures using a standard corresponding states scheme and the van der Waals one-fluid approximation
Crystal phases of a glass-forming Lennard-Jones mixture
International Nuclear Information System (INIS)
Fernandez, Julian R.; Harrowell, Peter
2003-01-01
We compare the potential energy at zero temperature of a range of crystal structures for a glass-forming binary mixture of Lennard-Jones particles. The lowest-energy ordered state consists of coexisting phases of a single component face centered cubic structure and an equimolar cesium chloride structure. An infinite number of layered crystal structures are identified with energies close to this ground state. We demonstrate that the finite size increase of the energy of the coexisting crystal with incoherent interfaces is sufficient to destabilize this ordered phase in simulations of typical size. Two specific local coordination structures are identified as of possible structural significance in the amorphous state. We observe rapid crystal growth in the equimolar mixture
Simulasi Sifat Fisis Model Molekuler Dinamik Gas Argon dengan Potensial Lennard-Jones
Directory of Open Access Journals (Sweden)
Wira Bahari Nurdin
2014-01-01
Full Text Available DOWNLOAD PDFTelah dilakukan pembuatan dan pengujian suatu simulasi tentang sifat fisis gasargon dengan menggunakan dinamika molekuler menggunakan potensial Lennard-Jonesdalam sistem terisolasi (ensemble mikrokanonik. Jumlah molekul, energi total sistem danluas kotak simulasi telah divariasikan. Untuk menghitung perubahan posisi digunakanalgoritma Verlet. Sifat fisis yang ditentukan dalam simulasi adalah temperatur dan energitotal sistem untuk menentukan adanya fase transisi. Dari hasil simulasi, terdapatkesesuaian antara simulasi dengan gas argon dan tidak diperoleh adanya fase transisi.Kata kunci: Simulasi dinamika molekul, argon, potensial Lennard-Jones, ensemblemikrokanonik, algoritma Verlet
A molecular dynamics study of Lennard-Jones physisorption on W(100)
International Nuclear Information System (INIS)
Broughton, J.Q.
1980-01-01
The physisorption of Xe on W(100) was modeled by Lennard-Jones pair-wise interaction potentials and the dynamics of coverages ranging from one to four adlayers obtained by molecular dynamics simulation. At 115 K, the first two layers were well-ordered and each adsorbed with c(2 x 2) symmetry. Further adsorption produced a surface similar to that of a distorted Xe(100) face. In accord with the work of Broughton and Woodcock, the top layers of the three- and four-adlayer coverages were rough and had liquid-like diffusion coefficients. The potential energies of all layers other than the first were similar, thus corroborating one of the postulates of BET theory. Generally, the effect of adsorbing a layer was to reduce the entropy of all those beneath. (orig.)
Phase diagram and universality of the Lennard-Jones gas-liquid system
Watanabe, Hiroshi
2012-01-01
The gas-liquid phase transition of the three-dimensional Lennard-Jones particles system is studied by molecular dynamics simulations. The gas and liquid densities in the coexisting state are determined with high accuracy. The critical point is determined by the block density analysis of the Binder parameter with the aid of the law of rectilinear diameter. From the critical behavior of the gas-liquid coexisting density, the critical exponent of the order parameter is estimated to be β = 0.3285(7). Surface tension is estimated from interface broadening behavior due to capillary waves. From the critical behavior of the surface tension, the critical exponent of the correlation length is estimated to be ν = 0.63(4). The obtained values of β and ν are consistent with those of the Ising universality class. © 2012 American Institute of Physics.
Freezing and melting line invariants of the Lennard-Jones system
DEFF Research Database (Denmark)
Costigliola, Lorenzo; Schrøder, Thomas; Dyre, Jeppe C.
2016-01-01
The invariance of several structural and dynamical properties of the Lennard-Jones (LJ) system along the freezing and melting lines is interpreted in terms of isomorph theory. First the freezing/melting lines of the LJ system are shown to be approximated by isomorphs. Then we show...... that the invariants observed along the freezing and melting isomorphs are also observed on other isomorphs in the liquid and crystalline phases. The structure is probed by the radial distribution function and the structure factor and dynamics are probed by the mean-square displacement, the intermediate scattering...... function, and the shear viscosity. Studying these properties with reference to isomorph theory explains why the known single-phase melting criteria hold, e.g., the Hansen–Verlet and the Lindemann criteria, and why the Andrade equation for the viscosity at freezing applies, e.g., for most liquid metals. Our...
Shear viscosity of the Lennard-Jones fluid near the triple point: Green-Kubo results
International Nuclear Information System (INIS)
Erpenbeck, J.J.
1988-01-01
The long-standing disagreement over the shear viscosity coefficient of the Lennard-Jones fluid near the triple point is reexamined through a series of very extensive Monte Carlo molecular-dynamics calculations of this transport coefficient based on the Green-Kubo theory. The stress autocorrelation function is shown to exhibit a slow decay, principally in the kinetic-potential and the potential-potential terms, which is large compared with the kinetic-kinetic long-time tail predicted by simple mode-coupling theory. Nonetheless, the viscosity coefficient, exclusive of any correction for this tail for times greater than are accessible numerically, is found to agree with that of Schoen and Hoheisel (who discounted the existence of such a tail) as well as nonequilibrium molecular-dynamics calculations. The large value of the viscosity coefficient found by Levesque and co-workers for 864 particles is brought into statistical agreement with the present results by a modest, but not unrealistic, increase in its statistical uncertainty. The pressure is found to exhibit an anomalous dependence on the size of the system, but the viscosity as well as the self-diffusion constant appear to be linear in the inverse of the number of particles, within the precision of our calculations. The viscosity coefficient, including a long-time-tail contribution based on the extended mode-coupling theory is (3.796 +- 0.068)σepsilon-c/m)/sup 1/2/ for the Lennard-Jones potential, fitted to a cubic spline, and (3.345 +- 0.068)σepsilon-c/m)/sup 1/2/ for the potential truncated at 2.5σ
International Nuclear Information System (INIS)
Mulero, A.; Cuadros, F; Faundez, C.A.
1999-01-01
Vapour-liquid equilibrium properties for both three- and two-dimensional Lennard-Jones fluids were obtained using simple cubic-in-density equations of state proposed by the authors. Results were compared with those obtained by other workers from computer simulations and also with results given by other more complex semi-theoretical or semi-empirical equations of state. In the three-dimensional case good agreement is found for all properties and all temperatures. In the two-dimensional case only the coexistence densities were compared, producing good agreement for low temperatures only. The present work is the first to give numerical data for the vapour-liquid equilibrium properties of Lennard-Jones fluids calculated from equations of state. Copyright (1999) CSIRO Australia
International Nuclear Information System (INIS)
Adebayo, G.A.; Anusionwu, B.C.; Njah, A.N.; Adeniran, O.J.; Mathew, B.; Sunmonu, R.S.
2009-01-01
Arising from the inability of theoretical calculations to give accurate descriptions of (shear) viscosity in rare gases at high densities, we investigated the likely cause of discrepancy between theory and experiments. Molecular Dynamics simulations were performed to calculate transport coefficients and collision frequency of rare gases at high densities and different temperatures using a Lennard-Jones modelled pair potential. The results, when compared with experiments show an underestimation of the viscosity calculated through the Green-Kubo formalism, but in agreement with some other calculations performed by other groups. In the present work the origin of the underestimation is considered. Analyses of the transport coefficients show a very high collision frequency which suggests an atom may spend much less time in the neighbourhood of the fields of force of another atom and that the distribution in the systems studied adjusts itself to a nearly Maxwellian type which resulted in a locally and temporarily slowly varying temperature. We show that the time spent in the fields of force is so small compared with relaxation time thereby leading to a possible reduction in local velocity auto-correlation between atoms. (author)
Single-site Lennard-Jones models via polynomial chaos surrogates of Monte Carlo molecular simulation
Energy Technology Data Exchange (ETDEWEB)
Kadoura, Ahmad, E-mail: ahmad.kadoura@kaust.edu.sa, E-mail: adil.siripatana@kaust.edu.sa, E-mail: shuyu.sun@kaust.edu.sa, E-mail: omar.knio@kaust.edu.sa; Sun, Shuyu, E-mail: ahmad.kadoura@kaust.edu.sa, E-mail: adil.siripatana@kaust.edu.sa, E-mail: shuyu.sun@kaust.edu.sa, E-mail: omar.knio@kaust.edu.sa [Computational Transport Phenomena Laboratory, The Earth Sciences and Engineering Department, The Physical Sciences and Engineering Division, King Abdullah University of Science and Technology, Thuwal 23955-6900 (Saudi Arabia); Siripatana, Adil, E-mail: ahmad.kadoura@kaust.edu.sa, E-mail: adil.siripatana@kaust.edu.sa, E-mail: shuyu.sun@kaust.edu.sa, E-mail: omar.knio@kaust.edu.sa; Hoteit, Ibrahim, E-mail: ibrahim.hoteit@kaust.edu.sa [Earth Fluid Modeling and Predicting Group, The Earth Sciences and Engineering Department, The Physical Sciences and Engineering Division, King Abdullah University of Science and Technology, Thuwal 23955-6900 (Saudi Arabia); Knio, Omar, E-mail: ahmad.kadoura@kaust.edu.sa, E-mail: adil.siripatana@kaust.edu.sa, E-mail: shuyu.sun@kaust.edu.sa, E-mail: omar.knio@kaust.edu.sa [Uncertainty Quantification Center, The Applied Mathematics and Computational Science Department, The Computer, Electrical and Mathematical Sciences and Engineering Division, King Abdullah University of Science and Technology, Thuwal 23955-6900 (Saudi Arabia)
2016-06-07
In this work, two Polynomial Chaos (PC) surrogates were generated to reproduce Monte Carlo (MC) molecular simulation results of the canonical (single-phase) and the NVT-Gibbs (two-phase) ensembles for a system of normalized structureless Lennard-Jones (LJ) particles. The main advantage of such surrogates, once generated, is the capability of accurately computing the needed thermodynamic quantities in a few seconds, thus efficiently replacing the computationally expensive MC molecular simulations. Benefiting from the tremendous computational time reduction, the PC surrogates were used to conduct large-scale optimization in order to propose single-site LJ models for several simple molecules. Experimental data, a set of supercritical isotherms, and part of the two-phase envelope, of several pure components were used for tuning the LJ parameters (ε, σ). Based on the conducted optimization, excellent fit was obtained for different noble gases (Ar, Kr, and Xe) and other small molecules (CH{sub 4}, N{sub 2}, and CO). On the other hand, due to the simplicity of the LJ model used, dramatic deviations between simulation and experimental data were observed, especially in the two-phase region, for more complex molecules such as CO{sub 2} and C{sub 2} H{sub 6}.
A test of the mean density approximation for Lennard-Jones mixtures with large size ratios
International Nuclear Information System (INIS)
Ely, J.F.
1986-01-01
The mean density approximation for mixture radial distribution functions plays a central role in modern corresponding-states theories. This approximation is reasonably accurate for systems that do not differ widely in size and energy ratios and which are nearly equimolar. As the size ratio increases, however, or if one approaches an infinite dilution of one of the components, the approximation becomes progressively worse, especially for the small molecule pair. In an attempt to better understand and improve this approximation, isothermal molecular dynamics simulations have been performed on a series of Lennard-Jones mixtures. Thermodynamic properties, including the mixture radial distribution functions, have been obtained at seven compositions ranging from 5 to 95 mol%. In all cases the size ratio was fixed at two and three energy ratios were investigated, 22 / 11 =0.5, 1.0, and 1.5. The results of the simulations are compared with the mean density approximation and a modification to integrals evaluated with the mean density approximation is proposed
A perturbed Lennard-Jones chain equation of state for liquid metals
Energy Technology Data Exchange (ETDEWEB)
Mousazadeh, M H; Marageh, M Ghanadi [AEOI, JIH Research Laboratory, 11365/8486, Tehran (Iran, Islamic Republic of)
2006-05-24
The perturbed Lennard-Jones chain (PLJC) equation of state is formulated based on first-order variational perturbation theory. The model uses two parameters for a monatomic system, segment size, {sigma}, and segment energy, {epsilon}/k. In this work, we employed the PLJC equation to calculate the liquid density of 26 metals, including alkali and alkali earth metals, iron, cobalt, nickel, copper, silver, gold, zinc, cadmium, mercury, aluminium, gallium, indium, thallium, tin, lead, antimony, and bismuth, for which accurate experimental data exist in the literature. The calculations cover a broad range of temperatures ranging from the melting point to close to the critical point and pressures ranging from the vapour-pressure curve up to pressures as high as 2000 bar. The average absolute deviation in the liquid density predicted by the PLJC equation of state in the saturation line compared with experimental data is 1.26%. Also, using the normal melting temperature and liquid density at melting point (T{sub m}, {rho}{sub m}) as input data for the estimation of the equation of state parameters provides a good correlation of liquid density at saturated and compressed pressures.
Thermodynamic equivalence between the Lennard-Jones and hard-core attractive Yukawa systems
International Nuclear Information System (INIS)
Kadiri, Y.; Albaki, R.; Bretonnet, J.L.
2008-01-01
The investigation of the thermodynamic properties of the Lennard-Jones (LJ) fluid is made by means of a system of particles interacting with a potential of hard-core plus attractive Yukawa tail (HCY). Due to the similarity between the LJ potential and the HCY potential in its overall form, it is worthwhile seeking to approximate the LJ potential in much the same way that the hard-sphere reference potential has been so used. The study consists in describing the thermodynamics of the LJ fluid in terms of the equivalent HCY system, whose the properties are known accurately, by means of mapping the thermodynamic quantities for the HCY potential parameters. The method is feasible owing to a convenient analytical expression of the Helmholtz free energy from the mean-spherical approximation expanded in power of the inverse temperature. Two different procedures are used to determine the parameters of the HCY potential as a function of the thermodynamic states: one is based on the simultaneous fits of pressure and internal energy of the LJ system and the other uses the concept of collision frequency. The reasonable homogeneity of the results in both procedures of mapping makes that the HCY potential is a very good reference system, whose the proposed theoretical expressions can be used confidently to predict the thermodynamic properties of more realistic potentials
Modeling Aggregation Processes of Lennard-Jones particles Via Stochastic Networks
Forman, Yakir; Cameron, Maria
2017-07-01
We model an isothermal aggregation process of particles/atoms interacting according to the Lennard-Jones pair potential by mapping the energy landscapes of each cluster size N onto stochastic networks, computing transition probabilities from the network for an N-particle cluster to the one for N+1, and connecting these networks into a single joint network. The attachment rate is a control parameter. The resulting network representing the aggregation of up to 14 particles contains 6427 vertices. It is not only time-irreversible but also reducible. To analyze its transient dynamics, we introduce the sequence of the expected initial and pre-attachment distributions and compute them for a wide range of attachment rates and three values of temperature. As a result, we find the configurations most likely to be observed in the process of aggregation for each cluster size. We examine the attachment process and conduct a structural analysis of the sets of local energy minima for every cluster size. We show that both processes taking place in the network, attachment and relaxation, lead to the dominance of icosahedral packing in small (up to 14 atom) clusters.
Spray flow-network flow transition of binary Lennard-Jones particle system
Inaoka, Hajime
2010-07-01
We simulate gas-liquid flows caused by rapid depressurization using a molecular dynamics model. The model consists of two types of Lennard-Jones particles, which we call liquid particles and gas particles. These two types of particles are distinguished by their mass and strength of interaction: a liquid particle has heavier mass and stronger interaction than a gas particle. By simulations with various initial number densities of these particles, we found that there is a transition from a spray flow to a network flow with an increase of the number density of the liquid particles. At the transition point, the size of the liquid droplets follows a power-law distribution, while it follows an exponential distribution when the number density of the liquid particles is lower than the critical value. The comparison between the transition of the model and that of models of percolation is discussed. The change of the average droplet size with the initial number density of the gas particles is also presented. © 2010 Elsevier B.V. All rights reserved.
Efficient Implementations of Molecular Dynamics Simulations for Lennard-Jones Systems
Watanabe, H.
2011-08-01
Efficient implementations of the classical molecular dynamics (MD) method for Lennard-Jones particle systems are considered. Not only general algorithms but also techniques that are efficient for some specific CPU architectures are also explained. A simple spatialdecomposition-based strategy is adopted for parallelization. By utilizing the developed code, benchmark simulations are performed on a HITACHI SR16000/J2 system consisting of IBM POWER6 processors which are 4.7 GHz at the National Institute for Fusion Science (NIFS) and an SGI Altix ICE 8400EX system consisting of Intel Xeon processors which are 2.93 GHz at the Institute for Solid State Physics (ISSP), the University of Tokyo. The parallelization efficiency of the largest run, consisting of 4.1 billion particles with 8192 MPI processes, is about 73% relative to that of the smallest run with 128 MPI processes at NIFS, and it is about 66% relative to that of the smallest run with 4 MPI processes at ISSP. The factors causing the parallel overhead are investigated. It is found that fluctuations of the execution time of each process degrade the parallel efficiency. These fluctuations may be due to the interference of the operating system, which is known as OS Jitter.
Pieprzyk, S.; Brańka, A. C.; Maćkowiak, Sz.; Heyes, D. M.
2018-03-01
The equation of state (EoS) of the Lennard-Jones fluid is calculated using a new set of molecular dynamics data which extends to higher temperature than in previous studies. The modified Benedict-Webb-Rubin (MBWR) equation, which goes up to ca. T ˜ 6, is reparametrized with new simulation data. A new analytic form for the EoS, which breaks the fluid range into two regions with different analytic forms and goes up to ca. T ≃ 35, is also proposed. The accuracy of the new formulas is at least as good as the MBWR fit and goes to much higher temperature allowing it to now encompass the Amagat line. The fitted formula extends into the high temperature range where the system can be well represented by inverse power potential scaling, which means that our specification of the equation of state covers the entire (ρ, T) plane. Accurate analytic fit formulas for the Boyle, Amagat, and inversion curves are presented. Parametrizations of the extrema loci of the isochoric, CV, and isobaric, CP, heat capacities are given. As found by others, a line maxima of CP terminates in the critical point region, and a line of minima of CP terminates on the freezing line. The line of maxima of CV terminates close to or at the critical point, and a line of minima of CV terminates to the right of the critical point. No evidence for a divergence in CV in the critical region is found.
Enhancement of the droplet nucleation in a dense supersaturated Lennard-Jones vapor
Energy Technology Data Exchange (ETDEWEB)
Zhukhovitskii, D. I., E-mail: dmr@ihed.ras.ru [Joint Institute of High Temperatures, Russian Academy of Sciences, Izhorskaya 13, Bd. 2, 125412 Moscow (Russian Federation)
2016-05-14
The vapor–liquid nucleation in a dense Lennard-Jones system is studied analytically and numerically. A solution of the nucleation kinetic equations, which includes the elementary processes of condensation/evaporation involving the lightest clusters, is obtained, and the nucleation rate is calculated. Based on the equation of state for the cluster vapor, the pre-exponential factor is obtained. The latter diverges as a spinodal is reached, which results in the nucleation enhancement. The work of critical cluster formation is calculated using the previously developed two-parameter model (TPM) of small clusters. A simple expression for the nucleation rate is deduced and it is shown that the work of cluster formation is reduced for a dense vapor. This results in the nucleation enhancement as well. To verify the TPM, a simulation is performed that mimics a steady-state nucleation experiments in the thermal diffusion cloud chamber. The nucleating vapor with and without a carrier gas is simulated using two different thermostats for the monomers and clusters. The TPM proves to match the simulation results of this work and of other studies.
A model-adaptivity method for the solution of Lennard-Jones based adhesive contact problems
Ben Dhia, Hachmi; Du, Shuimiao
2018-05-01
The surface micro-interaction model of Lennard-Jones (LJ) is used for adhesive contact problems (ACP). To address theoretical and numerical pitfalls of this model, a sequence of partitions of contact models is adaptively constructed to both extend and approximate the LJ model. It is formed by a combination of the LJ model with a sequence of shifted-Signorini (or, alternatively, -Linearized-LJ) models, indexed by a shift parameter field. For each model of this sequence, a weak formulation of the associated local ACP is developed. To track critical localized adhesive areas, a two-step strategy is developed: firstly, a macroscopic frictionless (as first approach) linear-elastic contact problem is solved once to detect contact separation zones. Secondly, at each shift-adaptive iteration, a micro-macro ACP is re-formulated and solved within the multiscale Arlequin framework, with significant reduction of computational costs. Comparison of our results with available analytical and numerical solutions shows the effectiveness of our global strategy.
Liquid-vapour phase behaviour of a polydisperse Lennard-Jones fluid
International Nuclear Information System (INIS)
Wilding, Nigel B; Sollich, Peter
2005-01-01
We describe a simulation study of the liquid-vapour phase behaviour of a model polydisperse fluid. Particle interactions are given by a Lennard-Jones potential in which polydispersity features both in the particle sizes and the amplitude of their interactions. We address the computational problem of accurately locating the cloud curve for such a system using Monte Carlo simulations within the grand canonical ensemble. The strongly nonlinear variation of the fractional volumes of the phases across the coexistence region precludes naive extrapolation to determine the cloud point density. Instead we propose an improved estimator for the cloud point location and use scaling arguments to predicts its finite-size behaviour. Excellent agreement is found with the simulation results. Application of the method reveals that the measured cloud curve is highly sensitive to the presence of large particles, even when they are extremely rare. This finding is expected to have implications for the reproducibility of experimentally measured phase diagrams in colloids and polymers
Dodecagonal order in a two-dimensional Lennard-Jones system
International Nuclear Information System (INIS)
Leung, P.W.; Henley, C.L.; Chester, G.V.
1989-01-01
We investigate a two-dimensional Lennard-Jones mixture with the interaction parameters chosen so as to favor configurations where the large atoms form squares and equilateral triangles. Many such configurations are possible which by our choice of interactions are nearly degenerate in energy. It is hypothesized that a thermal equilibrium state with 12-fold orientational order exists. Several Monte Carlo simulations were performed to cool the system to a temperature approaching zero. The ordering process was studied by following the evolution of the configurations with temperature. The onset of ordering seemed to be very diffuse in space rather than nucleated at a point. The resulting configurations consist of squares and triangles, except for a few dislocations, and thus have perfect orientational order. We also characterized the deviation from ideal quasiperiodicity in terms of the ''phason strain''; this was analyzed both by fitting a linear relation between the physical space coordinates of the atoms and the corresponding ''perpendicular space'' coordinates, and also by calculating the diffraction peaks. The latter are shifted and broadened, relative to an ideal 12-fold diffraction pattern, as in real quasicrystals
Single-site Lennard-Jones models via polynomial chaos surrogates of Monte Carlo molecular simulation
Kadoura, Ahmad Salim
2016-06-01
In this work, two Polynomial Chaos (PC) surrogates were generated to reproduce Monte Carlo (MC) molecular simulation results of the canonical (single-phase) and the NVT-Gibbs (two-phase) ensembles for a system of normalized structureless Lennard-Jones (LJ) particles. The main advantage of such surrogates, once generated, is the capability of accurately computing the needed thermodynamic quantities in a few seconds, thus efficiently replacing the computationally expensive MC molecular simulations. Benefiting from the tremendous computational time reduction, the PC surrogates were used to conduct large-scale optimization in order to propose single-site LJ models for several simple molecules. Experimental data, a set of supercritical isotherms, and part of the two-phase envelope, of several pure components were used for tuning the LJ parameters (ε, σ). Based on the conducted optimization, excellent fit was obtained for different noble gases (Ar, Kr, and Xe) and other small molecules (CH4, N2, and CO). On the other hand, due to the simplicity of the LJ model used, dramatic deviations between simulation and experimental data were observed, especially in the two-phase region, for more complex molecules such as CO2 and C2 H6.
Spray flow-network flow transition of binary Lennard-Jones particle system
Inaoka, Hajime; Yukawa, Satoshi; Ito, Nobuyasu
2010-01-01
We simulate gas-liquid flows caused by rapid depressurization using a molecular dynamics model. The model consists of two types of Lennard-Jones particles, which we call liquid particles and gas particles. These two types of particles are distinguished by their mass and strength of interaction: a liquid particle has heavier mass and stronger interaction than a gas particle. By simulations with various initial number densities of these particles, we found that there is a transition from a spray flow to a network flow with an increase of the number density of the liquid particles. At the transition point, the size of the liquid droplets follows a power-law distribution, while it follows an exponential distribution when the number density of the liquid particles is lower than the critical value. The comparison between the transition of the model and that of models of percolation is discussed. The change of the average droplet size with the initial number density of the gas particles is also presented. © 2010 Elsevier B.V. All rights reserved.
Fowler's approximation for the surface tension and surface energy of Lennard-Jones fluids revisited
International Nuclear Information System (INIS)
Mulero, A; Galan, C; Cuadros, F
2003-01-01
We present a detailed study of the validity of Fowler's approximation for calculating the surface tension and the surface energy of Lennard-Jones fluids. To do so, we consider three different explicit analytical expressions for the radial distribution function (RDF), including one proposed by our research group, together with very accurate expressions for the liquid and vapour densities, also proposed by our group. The calculation of the surface tension from the direct correlation function using both the Percus-Yevick and the hypernetted-chain approximations is also considered. Finally, our results are compared with those obtained by other authors by computer simulations or through relevant theoretical approximations. In particular, we consider the analytical expression proposed by Kalikmanov and Hofmans (1994 J. Phys.: Condens. Matter 6 2207-14) for the surface tension. Our results indicate that the values for the surface energy in Fowler's approximation obtained by other authors are adequate, and can be calculated from the RDF models. For the surface tension, however, the values considered as valid in previous works seem to be incorrect. The correct values can be obtained from our model for the RDF or from the Kalikmanov and Hofmans expression with suitable inputs
International Nuclear Information System (INIS)
Garcia, N.
1978-01-01
The GR method for solving the scattering equations of atoms from a hard corrugated surface is applied on accelerated particles above a hard corrugated surface and a hard corrugated surface with an attractive well. The solutions are given for the Rayleigh hypothesis that under the range of corrugation presented in this paper leads to the exact ones. Threshold resonances are studied observing that the appearance and disappearance of beams must be for a general theory with vertical tangent. The structure of the Lennard-Jones resonances given for the model mentioned above. For the first time it is stressed that Lennard-Jones resonances are not observed in metal surfaces in general, and, accordingly, they are unobserved in compact metallic surfaces. This is correlated with the fact that diffraction has not been observed. Both facts are due to the very weak corrugation of the gas-metal interaction potential. According to our results, the Lennard-Jones resonances in metals present greater difficulties to be observed experimentally. It is also noted that the absence of diffraction in compact metal surfaces is because they are almost plane and not because of the Debye-Waller effect. Finally, the lifetimes of the atoms at the crystal surfaces are calculated. These are larger, the smaller the incident energy and the larger the corrugation. But the lifetimes are particularly large at resonance conditions (10 -11 s). (Auth.)
Ab initio study of the atomic motion in liquid metal surfaces: comparison with Lennard-Jones systems
International Nuclear Information System (INIS)
Gonzalez, Luis E; Gonzalez, David J
2006-01-01
It is established that liquid metals exhibit surface layering at the liquid-vapour interface, while dielectric simple systems, like those interacting through Lennard-Jones potentials, show a monotonic decay from the liquid density to that of the vapour. First principles molecular dynamics simulations of the free liquid surface of several liquid metals (Li, Na, K, Rb, Cs, Mg, Ba, Al, Tl and Si), and the Na 3 K 7 alloy near their triple points have been performed in order to study the atomic motion at the interface, mainly at the outer layer. Comparison with the results of classical molecular dynamics simulations of a Lennard-Jones system shows interesting differences and similarities. The probability distribution function of the time of residence in a layer shows a peak at very short times and a long-lasting tail. The mean residence time in a layer increases when approaching the interfacial region, slightly in the Lennard-Jones system but strongly in the metallic systems. The motion within the layers, parallel to the interface, can be described as diffusion enhanced (strongly in the case of the outermost layer) with respect to the bulk, for both types of systems, despite its reduced dimensionality in metals
International Nuclear Information System (INIS)
Lee, Song Hi
2010-01-01
We presented a molecular dynamics (MD) simulation study of friction behavior between two very massive Brownian particles (BPs) oriented along the z axis with BP centers at -R 12 /2 and R 12 /2 in a Lennard-Jones solvent as a function of the inter-particle separation, R 12 . In order to fix the BPs in space an MD simulation method with the mass of the BP as 10 90 g/mol was employed in which the total momentum of the system was conserved. The cross friction coefficients of x- and y-components are nearly insensitive to R 12 but that of z-component varies with R 12 in good accord with the simple hydrodynamic approximation. On the other hand, the self-friction coefficients are estimated as a very small difference from the single particle friction coefficients, ξ 0 , at all inter-particle separations which agrees with the simple hydrodynamic approximation. Consequently ξ (-) xx is nearly independent of R 12 and equal to its asymptotic value of twice the single particle friction coefficient, and the other relative friction, ξ (-) zz , is in good agreement with the simple hydrodynamic approximation. Molecular theory of Brownian motion of a single heavy particle in a fluid had received a considerable attention in earlier years. After molecular dynamics (MD) simulation technique was utilized, this subject has been widely studied by a variety of MD simulation methods. The common issues here were about the long time behavior of the force and velocity autocorrelation functions, the system size dependent friction coefficient of a massive Brownian particle, and test of the Stokes-Einstein law
Properties of Organic Liquids when Simulated with Long-Range Lennard-Jones Interactions.
Fischer, Nina M; van Maaren, Paul J; Ditz, Jonas C; Yildirim, Ahmet; van der Spoel, David
2015-07-14
In order to increase the accuracy of classical computer simulations, existing methodologies may need to be adapted. Hitherto, most force fields employ a truncated potential function to model van der Waals interactions, sometimes augmented with an analytical correction. Although such corrections are accurate for homogeneous systems with a long cutoff, they should not be used in inherently inhomogeneous systems such as biomolecular and interface systems. For such cases, a variant of the particle mesh Ewald algorithm (Lennard-Jones PME) was already proposed 20 years ago (Essmann et al. J. Chem. Phys. 1995, 103, 8577-8593), but it was implemented only recently (Wennberg et al. J. Chem. Theory Comput. 2013, 9, 3527-3537) in a major simulation code (GROMACS). The availability of this method allows surface tensions of liquids as well as bulk properties to be established, such as density and enthalpy of vaporization, without approximations due to truncation. Here, we report on simulations of ≈150 liquids (taken from a force field benchmark: Caleman et al. J. Chem. Theory Comput. 2012, 8, 61-74) using three different force fields and compare simulations with and without explicit long-range van der Waals interactions. We find that the density and enthalpy of vaporization increase for most liquids using the generalized Amber force field (GAFF, Wang et al. J. Comput. Chem. 2004, 25, 1157-1174) and the Charmm generalized force field (CGenFF, Vanommeslaeghe et al. J. Comput. Chem. 2010, 31, 671-690) but less so for OPLS/AA (Jorgensen and Tirado-Rives, Proc. Natl. Acad. Sci. U.S.A. 2005, 102, 6665-6670), which was parametrized with an analytical correction to the van der Waals potential. The surface tension increases by ≈10(-2) N/m for all force fields. These results suggest that van der Waals attractions in force fields are too strong, in particular for the GAFF and CGenFF. In addition to the simulation results, we introduce a new version of a web server, http
Liquid-liquid interfacial properties of a symmetrical Lennard-Jones binary mixture
Energy Technology Data Exchange (ETDEWEB)
Martínez-Ruiz, F. J.; Blas, F. J., E-mail: felipe@uhu.es [Laboratorio de Simulación Molecular y Química Computacional, CIQSO-Centro de Investigación en Química Sostenible and Departamento de Física Aplicada, Universidad de Huelva, 21007 Huelva (Spain); Moreno-Ventas Bravo, A. I. [Laboratorio de Simulación Molecular y Química Computacional, CIQSO-Centro de Investigación en Química Sostenible and Departamento de Geología, Universidad de Huelva, 21007 Huelva (Spain)
2015-09-14
We determine the interfacial properties of a symmetrical binary mixture of equal-sized spherical Lennard-Jones molecules, σ{sub 11} = σ{sub 22}, with the same dispersive energy between like species, ϵ{sub 11} = ϵ{sub 22}, but different dispersive energies between unlike species low enough to induce phase separation. We use the extensions of the improved version of the inhomogeneous long-range corrections of Janecek [J. Phys. Chem. B 110, 6264 (2006)], presented recently by MacDowell and Blas [J. Chem. Phys. 131, 074705 (2009)] and Martínez-Ruiz et al. [J. Chem. Phys. 141, 184701 (2014)], to deal with the interaction energy and microscopic components of the pressure tensor. We perform Monte Carlo simulations in the canonical ensemble to obtain the interfacial properties of the symmetrical mixture with different cut-off distances r{sub c} and in combination with the inhomogeneous long-range corrections. The pressure tensor is obtained using the mechanical (virial) and thermodynamic route. The liquid-liquid interfacial tension is also evaluated using three different procedures, the Irving-Kirkwood method, the difference between the macroscopic components of the pressure tensor, and the test-area methodology. This allows to check the validity of the recent extensions presented to deal with the contributions due to long-range corrections for intermolecular energy and pressure tensor in the case of binary mixtures that exhibit liquid-liquid immiscibility. In addition to the pressure tensor and the surface tension, we also obtain density profiles and coexistence densities and compositions as functions of pressure, at a given temperature. According to our results, the main effect of increasing the cut-off distance r{sub c} is to sharpen the liquid-liquid interface and to increase the width of the biphasic coexistence region. Particularly interesting is the presence of a relative minimum in the total density profiles of the symmetrical mixture. This minimum is related
Liquid-liquid interfacial properties of a symmetrical Lennard-Jones binary mixture
International Nuclear Information System (INIS)
Martínez-Ruiz, F. J.; Blas, F. J.; Moreno-Ventas Bravo, A. I.
2015-01-01
We determine the interfacial properties of a symmetrical binary mixture of equal-sized spherical Lennard-Jones molecules, σ 11 = σ 22 , with the same dispersive energy between like species, ϵ 11 = ϵ 22 , but different dispersive energies between unlike species low enough to induce phase separation. We use the extensions of the improved version of the inhomogeneous long-range corrections of Janecek [J. Phys. Chem. B 110, 6264 (2006)], presented recently by MacDowell and Blas [J. Chem. Phys. 131, 074705 (2009)] and Martínez-Ruiz et al. [J. Chem. Phys. 141, 184701 (2014)], to deal with the interaction energy and microscopic components of the pressure tensor. We perform Monte Carlo simulations in the canonical ensemble to obtain the interfacial properties of the symmetrical mixture with different cut-off distances r c and in combination with the inhomogeneous long-range corrections. The pressure tensor is obtained using the mechanical (virial) and thermodynamic route. The liquid-liquid interfacial tension is also evaluated using three different procedures, the Irving-Kirkwood method, the difference between the macroscopic components of the pressure tensor, and the test-area methodology. This allows to check the validity of the recent extensions presented to deal with the contributions due to long-range corrections for intermolecular energy and pressure tensor in the case of binary mixtures that exhibit liquid-liquid immiscibility. In addition to the pressure tensor and the surface tension, we also obtain density profiles and coexistence densities and compositions as functions of pressure, at a given temperature. According to our results, the main effect of increasing the cut-off distance r c is to sharpen the liquid-liquid interface and to increase the width of the biphasic coexistence region. Particularly interesting is the presence of a relative minimum in the total density profiles of the symmetrical mixture. This minimum is related with a desorption of the
Hoheisel, C.
1988-09-01
Equilibrium molecular dynamics calculations with constraints have been performed for model liquids SF6 and CF4. The computations were carried out with four- and six-center Lennard-Jones potentials and up to 2×105 integration steps. Shear, bulk viscosity and the thermal conductivity have been calculated with use of Green-Kubo relations in the formulation of ``molecule variables.'' Various thermodynamic states were investigated. For SF6, a detailed comparison with experimental data was possible. For CF4, the MD results could only be compared with experiment for one liquid state. For the latter liquid, a complementary comparison was performed using MD results obtained with a one-center Lennard-Jones potential. A limited test of the particle number dependence of the results is presented. Partial and total correlations functions are shown and discussed with respect to findings obtained for the one-center Lennard-Jones liquid.
Flory-Huggins parameter χ, from binary mixtures of Lennard-Jones particles to block copolymer melts
International Nuclear Information System (INIS)
Chremos, Alexandros; Nikoubashman, Arash; Panagiotopoulos, Athanassios Z.
2014-01-01
In this contribution, we develop a coarse-graining methodology for mapping specific block copolymer systems to bead-spring particle-based models. We map the constituent Kuhn segments to Lennard-Jones particles, and establish a semi-empirical correlation between the experimentally determined Flory-Huggins parameter χ and the interaction of the model potential. For these purposes, we have performed an extensive set of isobaric–isothermal Monte Carlo simulations of binary mixtures of Lennard-Jones particles with the same size but with asymmetric energetic parameters. The phase behavior of these monomeric mixtures is then extended to chains with finite sizes through theoretical considerations. Such a top-down coarse-graining approach is important from a computational point of view, since many characteristic features of block copolymer systems are on time and length scales which are still inaccessible through fully atomistic simulations. We demonstrate the applicability of our method for generating parameters by reproducing the morphology diagram of a specific diblock copolymer, namely, poly(styrene-b-methyl methacrylate), which has been extensively studied in experiments
Flory-Huggins parameter χ, from binary mixtures of Lennard-Jones particles to block copolymer melts
Energy Technology Data Exchange (ETDEWEB)
Chremos, Alexandros, E-mail: achremos@imperial.ac.uk [Department of Chemical Engineering, Centre for Process Systems Engineering, Imperial College London, South Kensington Campus, London SW7 2AZ (United Kingdom); Nikoubashman, Arash, E-mail: arashn@princeton.edu; Panagiotopoulos, Athanassios Z. [Department of Chemical and Biological Engineering, Princeton University, Princeton, New Jersey 08544 (United States)
2014-02-07
In this contribution, we develop a coarse-graining methodology for mapping specific block copolymer systems to bead-spring particle-based models. We map the constituent Kuhn segments to Lennard-Jones particles, and establish a semi-empirical correlation between the experimentally determined Flory-Huggins parameter χ and the interaction of the model potential. For these purposes, we have performed an extensive set of isobaric–isothermal Monte Carlo simulations of binary mixtures of Lennard-Jones particles with the same size but with asymmetric energetic parameters. The phase behavior of these monomeric mixtures is then extended to chains with finite sizes through theoretical considerations. Such a top-down coarse-graining approach is important from a computational point of view, since many characteristic features of block copolymer systems are on time and length scales which are still inaccessible through fully atomistic simulations. We demonstrate the applicability of our method for generating parameters by reproducing the morphology diagram of a specific diblock copolymer, namely, poly(styrene-b-methyl methacrylate), which has been extensively studied in experiments.
International Nuclear Information System (INIS)
Johnson, W.R.; Dzuba, V.A.; Safronova, U.I.; Safronova, M.S.
2004-01-01
A finite-field scaling method is applied to evaluate the Lennard-Jones interaction constant C 3 for alkali-metal atoms. The calculations are based on the relativistic single-double approximation in which single and double excitations of Dirac-Hartree-Fock wave functions are included to all orders in perturbation theory
Bazhenov, Alexiev M.; Heyes, David M.
1990-01-01
The thermodynamics, structure, and transport coefficients, as defined by the Green-Kubo integrals, of the one-dimensional Lennard-Jones fluid are evaluated for a wide range of state points by molecular dynamics computer simulation. These calculations are performed for the first time for thermal conductivity and the viscosity. We observe a transition from hard-rod behavior at low number density to harmonic-spring fluid behavior in the close-packed limit. The self-diffusion coefficient decays with increasing density to a finite limiting value. The thermal conductivity increases with density, tending to ∞ in the close-packed limit. The viscosity in contrast maximizes at intermediate density, tending to zero in the zero density and close-packed limits.
Hoheisel, C.
1989-01-01
For several liquid states of CF4 and SF4, the shear and the bulk viscosity as well as the thermal conductivity were determined by equilibrium molecular dynamics (MD) calculations. Lennard-Jones four- and six-center pair potentials were applied, and the method of constraints was chosen for the MD. The computed Green-Kubo integrands show a steep time decay, and no particular longtime behavior occurs. The molecule number dependence of the results is found to be small, and 3×105 integration steps allow an accuracy of about 10% for the shear viscosity and the thermal conductivity coefficient. Comparison with experimental data shows a fair agreement for CF4, while for SF6 the transport coefficients fall below the experimental ones by about 30%.
International Nuclear Information System (INIS)
Hoheisel, C.
1989-01-01
For several liquid states of CF 4 and SF 6 , the shear and the bulk viscosity as well as the thermal conductivity were determined by equilibrium molecular dynamics (MD) calculations. Lennard-Jones four- and six-center pair potentials were applied, and the method of constraints were chosen for the MD. The computed Green-Kubo integrands show a steep time decay, and no particular longtime behavior occurs. The molecule number dependence of the results is found to be small, and 3 x 10 5 integration steps allow an accuracy of about 10% for the shear viscosity and the thermal conductivity coefficient. Comparison with experimental data shows a fair agreement for CF 4 , while for SF 6 the transport coefficients fall below the experimental ones by about 30%
International Nuclear Information System (INIS)
Merabia, Samy; Termentzidis, Konstantinos
2012-01-01
We characterize the thermal Kapitza conductance between Lennard-Jones solids using non-equilibrium molecular dynamics simulations. We consider a series of perfect interfaces between mass-mismatched solids. We show that both the acoustic mismatch model (AMM) and the diffuse mismatch model (DMM) fail to predict the interfacial conductance even for large acoustic mismatched solids. This poor agreement may be explained by the use of equilibrium distributions of phonons in the expression of the conductance. On the other hand, we show that an extension of AMM taking into account the out-of-equilibrium phonon distribution on both sides of the interface leads to a good agreement with the simulation results, even for interfaces between almost similar materials. This opens the way to understand interfacial heat transport across real semi-conductors and dielectrics.
International Nuclear Information System (INIS)
Lin, T.; Bian, X.F.; Jiang, J.
2006-01-01
Two metallic bulk glasses, Cu 60 Zr 30 Ti 10 and Cu 47 Ti 33 Zr 11 Ni 8 Si 1 , with a diameter of 3 mm were prepared by copper mold casting method. Dilatometric measurement was carried out on the two glassy alloys to obtain information about the average nearest-neighbour distance r 0 and the effective depth of pair potential V 0 . By assuming a Lennard-Jones potential, r 0 and V 0 were calculated to be 0.28 nm and 0.16 eV for Cu 60 Zr 30 Ti 10 and 0.27 nm and 0.13 eV for Cu 47 Ti 33 Zr 11 Ni 8 Si 1 , respectively. It was found that the glassy alloy Cu 60 Zr 30 Ti 10 was more stable than Cu 47 Ti 33 Zr 11 Ni 8 Si 1 against heating from both experiment and calculation
International Nuclear Information System (INIS)
Olivi-Tran, N.; Faivre, A.
2009-01-01
We computed a Lennard-Jones frozen liquid with a free surface using classical molecular dynamics. The structure factor curves on the free surface of this sample were calculated for different depths knowing that we have periodic boundary conditions on the other parts of the sample. The resulting structure factor curves show an horizontal shift of their first peak depending on how deep in the sample the curves are computed. We analyze our resulting curves in the light of spatial correlation functions during melting. The conclusion is that the differences between bulk and surface are quite small during melting and that at the end of melting, only the very surface happens to be less dense than the bulk. This result is intrinsic to the shape of the Lennard-Jones potential and does not depend on any other parameter.
International Nuclear Information System (INIS)
Staśkiewicz, B.; Okrasiński, W.
2012-01-01
We propose a simple analytical form of the vapor–liquid equilibrium curve near the critical point for Lennard-Jones fluids. Coexistence densities curves and vapor pressure have been determined using the Van der Waals and Dieterici equation of state. In described method the Bernoulli differential equations, critical exponent theory and some type of Maxwell's criterion have been used. Presented approach has not yet been used to determine analytical form of phase curves as done in this Letter. Lennard-Jones fluids have been considered for analysis. Comparison with experimental data is done. The accuracy of the method is described. -- Highlights: ► We propose a new analytical way to determine the VLE curve. ► Simple, mathematically straightforward form of phase curves is presented. ► Comparison with experimental data is discussed. ► The accuracy of the method has been confirmed.
International Nuclear Information System (INIS)
Garcia, N.
1976-01-01
This paper considers the effect of the attractive part of the interaction potential on the scattering of He atoms from a LiF(001) surface. We calculate, in particular, the Lennard-Jones resonances on the intensities and the phases of the scattered amplitudes, using a square well in the front of a hard corrugated surface model. We show that the amplitudes for incident energies smaller than the depth of the well are dominated by the resonances
Mirzaeinia, Ali; Feyzi, Farzaneh; Hashemianzadeh, Seyed Majid
2017-12-07
Simple and accurate expressions are presented for the equation of state (EOS) and absolute Helmholtz free energy of a system composed of simple atomic particles interacting through the repulsive Lennard-Jones potential model in the fluid and solid phases. The introduced EOS has 17 and 22 coefficients for fluid and solid phases, respectively, which are regressed to the Monte Carlo (MC) simulation data over the reduced temperature range of 0.6≤T * ≤6.0 and the packing fraction range of 0.1 ≤ η ≤ 0.72. The average absolute relative percent deviation in fitting the EOS parameters to the MC data is 0.06 and 0.14 for the fluid and solid phases, respectively. The thermodynamic integration method is used to calculate the free energy using the MC simulation results. The Helmholtz free energy of the ideal gas is employed as the reference state for the fluid phase. For the solid phase, the values of the free energy at the reduced density equivalent to the close-packed of a hard sphere are used as the reference state. To check the validity of the predicted values of the Helmholtz free energy, the Widom particle insertion method and the Einstein crystal technique of Frenkel and Ladd are employed. The results obtained from the MC simulation approaches are well agreed to the EOS results, which show that the proposed model can reliably be utilized in the framework of thermodynamic theories.
International Nuclear Information System (INIS)
Dowell, F.
1983-01-01
Two average-environment simple cubic lattice models: a refined model and a simple model, both having site-site (segmental) pair Lennard-Jones (LJ) interactions: for molecules composed of rigid cores having semiflexible tails are presented. The calculated values of the following properties at the nematic-isotropic transition for rigid rods of varying length are compared with relevant experimental data for PAA (p-azoxyanisole, or 4,4'-dimethoxyazoxybenzene): temperature, core orientational order parameter, nematic density and volume, relative density change, and relative entropy change. The temperature change as a function of volume change at constant order parameter is also discussed. In general, both LJ models give considerably better quantitative agreement with experiment, especially for the temperature and the relative density change, than do the earlier lattice models with hard repulsions, with or without constant segmental pair interaction energies. In most aspects, these LJ models give good quantitative agreement with experiment. These LJ models elucidate the importance of realistic intermolecular potentials, especially the role of soft repulsions, in describing an order-disorder transition between two condensed phases
International Nuclear Information System (INIS)
Van Zon, Ramses; Ashwin, S S; Cohen, E G D
2008-01-01
To describe short time (picosecond) and small scale (nanometre) transport in fluids, a Green's function approach was recently developed. This approach relies on an expansion of the distribution of single particle displacements around a Gaussian function, yielding an infinite series of correction terms. Applying a recent theorem (van Zon and Cohen 2006 J. Stat. Phys. 123 1–37) shows that for sufficiently small times the terms in this series become successively smaller, so that truncating the series near or at the Gaussian level might provide a good approximation. In this paper, we derive a theoretical estimate for the time scale at which truncating the series at or near the Gaussian level could be supposed to be accurate for equilibrium nanoscale systems. In order to numerically estimate this time scale, the coefficients for the first few terms in the series are determined in computer simulations for a Lennard-Jones (LJ) fluid, an isotopic LJ mixture and a suspension of a LJ-based model of nanoparticles in a LJ fluid. The results suggest that for LJ fluids an expansion around a Gaussian is accurate at time scales up to a picosecond, while for nanoparticles in suspension (a nanofluid), the characteristic time scale up to which the Gaussian is accurate becomes of the order of 5–10 ps. (invited article)
International Nuclear Information System (INIS)
Saeidi, Mohammadreza; Vaezzadeh, Majid; Badakhshan, Farzaneh
2011-01-01
Influence of DC electric field on carbon nanotube (CNT) growth in chemical vapor deposition is studied. Investigation of electric field effect in van der Waals interaction shows that increase in DC electric field raises the magnitude of attractive term of the Lennard-Jones potential. By using a theoretical model based on phonon vibrations of CNT on catalyst, it is shown that there is an optimum field for growth. Also it is observed that CNT under optimum electric field is longer than CNT in the absence of field. Finally, the relation between optimum DC electric field and type of catalyst is investigated and for some intervals of electric field, the best catalyst is introduced, which is very useful for experimental researches. -- Research highlights: → Influence of DC electric field on CNT growth in CVD. → Effect of electric field on van der Waals interaction between CNT and its catalyst. → Applying DC electric field increases attractive term of Lennard-Jonespotential. → There is an optimum DC field for CNT growth. → For catalyst with stronger van der Waals interaction, optimum field is smaller.
Fowler's approximation for the surface tension and surface energy of Lennard-Jones fluids revisited
Energy Technology Data Exchange (ETDEWEB)
Mulero, A [Departamento de Fisica, Universidad de Extremadura, 06071-Badajoz (Spain); Galan, C [Departamento de Fisica, Universidad de Extremadura, 06071-Badajoz (Spain); Cuadros, F [Departamento de Fisica, Universidad de Extremadura, 06071-Badajoz (Spain)
2003-04-16
We present a detailed study of the validity of Fowler's approximation for calculating the surface tension and the surface energy of Lennard-Jones fluids. To do so, we consider three different explicit analytical expressions for the radial distribution function (RDF), including one proposed by our research group, together with very accurate expressions for the liquid and vapour densities, also proposed by our group. The calculation of the surface tension from the direct correlation function using both the Percus-Yevick and the hypernetted-chain approximations is also considered. Finally, our results are compared with those obtained by other authors by computer simulations or through relevant theoretical approximations. In particular, we consider the analytical expression proposed by Kalikmanov and Hofmans (1994 J. Phys.: Condens. Matter 6 2207-14) for the surface tension. Our results indicate that the values for the surface energy in Fowler's approximation obtained by other authors are adequate, and can be calculated from the RDF models. For the surface tension, however, the values considered as valid in previous works seem to be incorrect. The correct values can be obtained from our model for the RDF or from the Kalikmanov and Hofmans expression with suitable inputs.
Scaling relation and regime map of explosive gas–liquid flow of binary Lennard-Jones particle system
Inaoka, Hajime
2012-02-01
We study explosive gasliquid flows caused by rapid depressurization using a molecular dynamics model of Lennard-Jones particle systems. A unique feature of our model is that it consists of two types of particles: liquid particles, which tend to form liquid droplets, and gas particles, which remain supercritical gaseous states under the depressurization realized by simulations. The system has a pipe-like structure similar to the model of a shock tube. We observed physical quantities and flow regimes in systems with various combinations of initial particle number densities and initial temperatures. It is observed that a physical quantity Q, such as pressure, at position z measured along a pipe-like system at time t follows a scaling relation Q(z,t)=Q(zt) with a scaling function Q(ζ). A similar scaling relation holds for time evolution of flow regimes in a system. These scaling relations lead to a regime map of explosive flows in parameter spaces of local physical quantities. The validity of the scaling relations of physical quantities means that physics of equilibrium systems, such as an equation of state, is applicable to explosive flows in our simulations, though the explosive flows involve highly nonequilibrium processes. In other words, if the breaking of the scaling relations is observed, it means that the explosive flows cannot be fully described by physics of equilibrium systems. We show the possibility of breaking of the scaling relations and discuss its implications in the last section. © 2011 Elsevier B.V. All rights reserved.
International Nuclear Information System (INIS)
Erpenbeck, J.J.
1987-01-01
We apply the so-called ''synthetic'' nonequilibrium molecular-dynamics method to the calculation of the self-diffusion constant of a Lennard-Jones fluid at a number density of 0.85/σ 3 and a temperature of 1.08 epsilon-c/k/sub B/ (where epsilon-c and σ are the energy and length parameters of the potential and k/sub B/ is the Boltzmann constant). By comparing with the Green-Kubo calculation for the same state of the system and for the same number of particles, N, we find the latter calculation to yield more precise values of the self-diffusion constant for a given number of molecular-dynamics time steps. Even at small values of the diffusion current, a nontrivial time is needed for the nonequilibrium calculation to reach the steady state. For larger values of the driving force, the steady-state flow appears to become unstable and evidence of a secondary flow pattern is presented. The presence of these instabilities acts as a limit to the range of the driving force for which the steady-state method can be applied. With increasing N the range of stable values of the diffusion current density decreases. For the Green-Kubo calculations, the N dependence of the self-diffusion constant is found to be anomalous for N = 108, with the 1/N dependence only exhibited for at least 500 particles. The nonequilibrium results, while approximately independent of N for 108 and 500 particles, are found to have a similar anomalous N dependence when we extend the calculations to 1372 particles, thereby bringing the Green-Kubo and nonequilibrium results into agreement in the large-system limit
Karbowniczek, Paweł; Chrzanowska, Agnieszka
2017-11-01
A two-dimensional Lennard-Jones system in a circular and rotating container has been studied by means of molecular dynamics technique. A nonequilibrium transition to the rotating stage has been detected in a delayed time since an instant switching of the frame rotation. This transition is attributed to the increase of the density at the wall because of the centrifugal force. At the same time the phase transition occurs, the inner system changes its configuration of the solid-state type into the liquid type. Impact of angular frequency and molecular roughness on the transport properties of the nonrotating and rotating systems is analyzed.
DEFF Research Database (Denmark)
Nellemann, Camilla
2017-01-01
This is a Danish version. This case focuses on an owner-manager's considerations regarding his exit. Carsten Joost established Joost El in 2005. It currently employs 10 people. He has two sons but no intention to hand over the business to them. Rather, he hopes that his key employee eventually...
International Nuclear Information System (INIS)
Costigliola, Lorenzo; Schrøder, Thomas B.; Dyre, Jeppe C.
2016-01-01
The recent theoretical prediction by Maimbourg and Kurchan [e-print http://arxiv.org/abs/1603.05023 (2016)] that for regular pair-potential systems the virial potential-energy correlation coefficient increases towards unity as the dimension d goes to infinity is investigated for the standard 12-6 Lennard-Jones fluid. This is done by computer simulations for d = 2, 3, 4 going from the critical point along the critical isotherm/isochore to higher density/temperature. In both cases the virial potential-energy correlation coefficient increases significantly. For a given density and temperature relative to the critical point, with increasing number of dimension the Lennard-Jones system conforms better to the hidden-scale-invariance property characterized by high virial potential-energy correlations (a property that leads to the existence of isomorphs in the thermodynamic phase diagram, implying that it becomes effectively one-dimensional in regard to structure and dynamics). The present paper also gives the first numerical demonstration of isomorph invariance of structure and dynamics in four dimensions. Our findings emphasize the need for a universally applicable 1/d expansion in liquid-state theory; we conjecture that the systems known to obey hidden scale invariance in three dimensions are those for which the yet-to-be-developed 1/d expansion converges rapidly.
Vogelsang, R.; Hoheisel, C.
1987-02-01
Molecular-dynamics (MD) calculations are reported for three thermodynamic states of a Lennard-Jones fluid. Systems of 2048 particles and 105 integration steps were used. The transverse current autocorrelation function, Ct(k,t), has been determined for wave vectors of the range 0.5viscosities which showed a systematic behavior as a function of k. Extrapolation to the hydrodynamic region at k=0 gave shear viscosity coefficients in good agreement with direct Green-Kubo results obtained in previous work. The two-exponential model fit for the memory function proposed by other authors does not provide a reasonable description of the MD results, as the fit parameters show no systematic wave-vector dependence, although the Ct(k,t) functions are somewhat better fitted. Similarly, the semiempirical interpolation formula for the decay time based on the viscoelastic concept proposed by Akcasu and Daniels fails to reproduce the correct k dependence for the wavelength range investigated herein.
International Nuclear Information System (INIS)
Vogelsang, R.; Hoheisel, C.
1987-01-01
For a large region of dense fluid states of a Lennard-Jones system, they have calculated the friction coefficient by the force autocorrelation function of a Brownian-type particle by molecular dynamics (MD). The time integral over the force autocorrelation function showed an interesting behavior and the expected plateau value when the mass of the Brownian particle was chosen to be about a factor of 100 larger than the mass of the fluid particle. Sufficient agreement was found for the friction coefficient calculated by this way and that obtained by calculations of the self-diffusion coefficient using the common relation between these coefficients. Furthermore, a modified friction coefficient was determined by integration of the force autocorrelation function up to the first maximum. This coefficient can successfully be used to derive a reasonable soft part of the friction coefficient necessary for the Rice-Allnatt approximation for the shear velocity and simple liquids
Energy Technology Data Exchange (ETDEWEB)
Mamedov, Bahtiyar A. [Department of Physics, Gaziosmanpaşa University, 60250, Tokat (Turkey); Somuncu, Elif; Askerov, Iskender M. [Department of Physics, Giresun University, Giresun (Turkey)
2016-08-10
In this work, a new theoretical approach is proposed for calculating fourth virial coefficient with Lennard-Jones potential. The established algorithm can be used to evaluate the thermodynamics properties and the intermolecular interaction potentials of liquids and gases with an improved accuracy. Note that the evaluation of the high-order virial coefficients is very valuable for accurate calculation of thermodynamic parameters. By using the suggested method, the fourth virial coefficient of CH{sub 4}, Ar, C{sub 2}H{sub 6} and SF{sub 6} molecules are evaluated. The calculation results are useful for accurate interpretation of the experimental data and of the determination of related physical properties.
Directory of Open Access Journals (Sweden)
W. Kurniawan
2016-11-01
Full Text Available Penyelesaian persamaan Schrödinger dengan berbagai model potensial sangat penting dilakukan untuk memberikan gambaran perilaku zarah di bawah pengaruh potensial tersebut. Solusinya berupa fungsi gelombang yang memuat informasi penting tentang perilaku gelombang yang ditunjukkan dengan energi terikatnya. Pada penelitian ini kasus yang ingin diteliti adalah model potensial Lennard-Jones dengan menggunakan metode analisa goal seek yang tersedia pada Microsoft excel. Persamaannya dijabarkan dengan metode Euler terlebih dahulu selanjutnya syarat batas ditentukan agar ketelitian hasil diperoleh. Agar perhitungan goal seek dapat dilakukan maka harus diubah dari besaran fisis menjadi besaran yang tidak berdimensi dimana parameter v menunjukkan keklasikan suatu sistem dan nilai ε menunjukkan kuantisasi energi. Hasil yang diperoleh adalah bahwa dengan memasukkan parameter kontrol nilai v tertentu, telah diperoleh beberapa keadaan energi dengan batas zkiri dan zkanan tertentu. Ketika masukan parameter v yang diberikan semakin besar keadaan energinya pun lebih rapat (ditunjukkan energy state yang diperoleh semakin banyak dibandingkan bila masukan v-nya lebih kecil. Penelitian ini bermanfaat untuk menyederhanakan kasus potensial yang lebih rumit, dimana solusinya dapat diperoleh dengan mudah dan konsep kuantisasi energi akibat model potensial L-J dapat dipahami secara utuh. Solution of the Schrödinger equation in various potential model is very important in order to provide an overview of behaviour’s particle under influence of potential model. The solution is a wave function that contains important information are shown by energy state. In this research, the investigated is Lennard Jones potential by using Goal Seek analysis which are available in Microsoft Excel. The equation is described by the Euler method and then boundary condition is determined to perecision result which are obtained. It must be changed in terms dimensionless where
Georgescu, Ionuţ; Mandelshtam, Vladimir A
2012-10-14
The theory of self-consistent phonons (SCP) was originally developed to address the anharmonic effects in condensed matter systems. The method seeks a harmonic, temperature-dependent Hamiltonian that provides the "best fit" for the physical Hamiltonian, the "best fit" being defined as the one that optimizes the Helmholtz free energy at a fixed temperature. The present developments provide a scalable O(N) unified framework that accounts for anharmonic effects in a many-body system, when it is probed by either thermal (ℏ → 0) or quantum fluctuations (T → 0). In these important limits, the solution of the nonlinear SCP equations can be reached in a manner that requires only the multiplication of 3N × 3N matrices, with no need of diagonalization. For short range potentials, such as Lennard-Jones, the Hessian, and other related matrices are highly sparse, so that the scaling of the matrix multiplications can be reduced from O(N(3)) to ~O(N). We investigate the role of quantum effects by continuously varying the de-Boer quantum delocalization parameter Λ and report the N-Λ (T = 0), and also the classical N-T (Λ = 0) phase diagrams for sizes up to N ~ 10(4). Our results demonstrate that the harmonic approximation becomes inadequate already for such weakly quantum systems as neon clusters, or for classical systems much below the melting temperatures.
Oh, Inrok; Choi, Saehyun; Jung, YounJoon; Kim, Jun Soo
2015-08-28
Phase separation in a biological cell nucleus occurs in a heterogeneous environment filled with a high density of chromatins and thus it is inevitably influenced by interactions with chromatins. As a model system of nuclear body formation in a cell nucleus filled with chromatins, we simulate the phase separation of a low-density Lennard-Jones (LJ) fluid interacting with a long, condensed polymer chain. The influence of the density variation of LJ particles above and below the phase boundary and the role of attractive interactions between LJ particles and polymer segments are investigated at a fixed value of strong self-interaction between LJ particles. For a density of LJ particles above the phase boundary, phase separation occurs and a dense domain of LJ particles forms irrespective of interactions with the condensed polymer chain whereas its localization relative to the polymer chain is determined by the LJ-polymer attraction strength. Especially, in the case of moderately weak attractions, the domain forms separately from the polymer chain and subsequently associates with the polymer chain. When the density is below the phase boundary, however, the formation of a dense domain is possible only when the LJ-polymer attraction is strong enough, for which the domain grows in direct contact with the interacting polymer chain. In this work, different growth behaviors of LJ particles result from the differences in the density of LJ particles and in the LJ-polymer interaction, and this work suggests that the distinct formation of activity-dependent and activity-independent nuclear bodies (NBs) in a cell nucleus may originate from the differences in the concentrations of body-specific NB components and in their interaction with chromatins.
Energy Technology Data Exchange (ETDEWEB)
Martínez-Ruiz, F. J.; Blas, F. J., E-mail: felipe@uhu.es [Departamento de Física Aplicada, Universidad de Huelva, 21071 Huelva (Spain); Centro de Investigación de Física Teórica y Matemática, Universidad de Huelva, 21071 Huelva (Spain); Mendiboure, B. [Laboratoire des Fluides Complexes et leurs Réservoirs, UMR5150, Université de Pau et des Pays de l’Adour, B. P. 1155, Pau Cedex 64014 (France); Moreno-Ventas Bravo, A. I. [Centro de Investigación de Física Teórica y Matemática, Universidad de Huelva, 21071 Huelva (Spain); Departamento de Geología, Facultad de Ciencias Experimentales, Universidad de Huelva, 21071 Huelva (Spain)
2014-11-14
We propose an extension of the improved version of the inhomogeneous long-range corrections of Janeček [J. Phys. Chem. B 110, 6264–6269 (2006)], presented recently by MacDowell and Blas [J. Chem. Phys. 131, 074705 (2009)] to account for the intermolecular potential energy of spherical, rigid, and flexible molecular systems, to deal with the contributions to the microscopic components of the pressure tensor due to the dispersive long-range corrections. We have performed Monte Carlo simulations in the canonical ensemble to obtain the interfacial properties of spherical Lennard-Jones molecules with different cutoff distances, r{sub c} = 2.5, 3, 4, and 5σ. In addition, we have also considered cutoff distances r{sub c} = 2.5 and 3σ in combination with the inhomogeneous long-range corrections proposed in this work. The normal and tangential microscopic components of the pressure tensor are obtained using the mechanical or virial route in combination with the recipe of Irving and Kirkwood, while the macroscopic components are calculated using the Volume Perturbation thermodynamic route proposed by de Miguel and Jackson [J. Chem. Phys. 125, 164109 (2006)]. The vapour-liquid interfacial tension is evaluated using three different procedures, the Irving-Kirkwood method, the difference between the macroscopic components of the pressure tensor, and the Test-Area methodology. In addition to the pressure tensor and the surface tension, we also obtain density profiles, coexistence densities, vapour pressure, critical temperature and density, and interfacial thickness as functions of temperature, paying particular attention to the effect of the cutoff distance and the long-range corrections on these properties. According to our results, the main effect of increasing the cutoff distance (at fixed temperature) is to sharpen the vapour-liquid interface, to decrease the vapour pressure, and to increase the width of the biphasic coexistence region. As a result, the interfacial
International Nuclear Information System (INIS)
Martínez-Ruiz, F. J.; Blas, F. J.; Mendiboure, B.; Moreno-Ventas Bravo, A. I.
2014-01-01
We propose an extension of the improved version of the inhomogeneous long-range corrections of Janeček [J. Phys. Chem. B 110, 6264–6269 (2006)], presented recently by MacDowell and Blas [J. Chem. Phys. 131, 074705 (2009)] to account for the intermolecular potential energy of spherical, rigid, and flexible molecular systems, to deal with the contributions to the microscopic components of the pressure tensor due to the dispersive long-range corrections. We have performed Monte Carlo simulations in the canonical ensemble to obtain the interfacial properties of spherical Lennard-Jones molecules with different cutoff distances, r c = 2.5, 3, 4, and 5σ. In addition, we have also considered cutoff distances r c = 2.5 and 3σ in combination with the inhomogeneous long-range corrections proposed in this work. The normal and tangential microscopic components of the pressure tensor are obtained using the mechanical or virial route in combination with the recipe of Irving and Kirkwood, while the macroscopic components are calculated using the Volume Perturbation thermodynamic route proposed by de Miguel and Jackson [J. Chem. Phys. 125, 164109 (2006)]. The vapour-liquid interfacial tension is evaluated using three different procedures, the Irving-Kirkwood method, the difference between the macroscopic components of the pressure tensor, and the Test-Area methodology. In addition to the pressure tensor and the surface tension, we also obtain density profiles, coexistence densities, vapour pressure, critical temperature and density, and interfacial thickness as functions of temperature, paying particular attention to the effect of the cutoff distance and the long-range corrections on these properties. According to our results, the main effect of increasing the cutoff distance (at fixed temperature) is to sharpen the vapour-liquid interface, to decrease the vapour pressure, and to increase the width of the biphasic coexistence region. As a result, the interfacial thickness
Characterization of signaling and traffic in Joost
Alhaisoni, M.; Liotta, A.
2009-01-01
Peer-to-Peer (P2P) IPTV applications have increasingly been considered as a potential approach to online broadcasting. Recently, many applications such as PPlive, PPStream, and Sopcast have been deployed to deliver live streaming via P2P. One of the latest systems is Joost, which can deliver both
Dong, Dengpan; Vatamanu, Jenel P.; Wei, Xiaoyu; Bedrov, Dmitry
2018-05-01
Atomistic molecular dynamics simulations were conducted to study the wetting states of 1-ethyl-3-methylimidazolium bis(trifluoro-methylsulfonyl)-imide ionic liquid (IL) nanodroplets on surfaces with different strengths of van der Waals (VDW) interactions and in the presence of an electric field. By adjusting the depth of Lennard-Jones potential, the van der Waals interaction between the solid surface and ionic liquid was systematically varied. The shape of the droplets was analyzed to extract the corresponding contact angle utilized to characterize wetting states of the nanodroplets. The explored range of surface-IL interactions allowed contact angles ranging from complete IL spreading on the surface to poor wettability. The effect of the external electrical field was explored by adding point charges to the surface atoms. Systems with two charge densities (±0.002 e/atom and ±0.004 e/atom) that correspond to 1.36 V/nm and 2.72 V/nm electric fields were investigated. Asymmetrical wetting states were observed for both cases. At 1.36 V/nm electric field, contributions of IL-surface VDW interactions and Coulombic interactions to the wetting state were competitive. At 2.72 V/nm field, electrostatic interactions dominate the interaction between the nanodroplet and surface, leading to enhanced wettability on all surfaces.
Uhiuus orkester Tallinn Sinfonietta / Ivo Lille ja Risto Joost ; intervjueerinud Kristina Kõrver
Lille, Ivo, 1977-
2009-01-01
Kontserdiagentuurist HIMusic Agency ja Tallinn Sinfoniettast räägivad dirigent R. Joost ja I. Lille. Avakontserdist Vene Kultuurikeskuses, kus oli kavas Mozarti sümfooniad 1, 10 ja 40 ning kontsertaariad bulgaaria soprani Sonya Youncheva esituses
Boekbespreking Ronald Meester en Joost Hulshof: Wiskunde in je vingers : Hogere wiskunde omlaaghalen
Caspers, Wim; Timmer, Mark
“Een oppepcursus voor liefhebbers en andere freaks”, zo omschrijven Ronald Meester en Joost Hulshof hun boek W={kunde} in je vingers. Wim Caspers en Mark Timmer, allebei docent aan een middelbare school en lerarenopleider, bekeken het boek ieder vanuit beide rollen en gingen op bezoek bij de
Spinning superfluid 4He nanodroplets
Ancilotto, Francesco; Barranco, Manuel; Pi, Martí
2018-05-01
We have studied spinning superfluid 4He nanodroplets at zero temperature using density functional theory. Due to the irrotational character of the superfluid flow, the shapes of the spinning nanodroplets are very different from those of a viscous normal fluid drop in steady rotation. We show that when vortices are nucleated inside the superfluid droplets, their morphology, which evolves from axisymmetric oblate to triaxial prolate to two-lobed shapes, is in good agreement with experiments. The presence of vortex arrays confers to the superfluid droplets the rigid-body behavior of a normal fluid in steady rotation, and this is the ultimate reason for the surprising good agreement between recent experiments and the classical models used for their description.
An EQT-based cDFT approach for a confined Lennard-Jones fluid mixture
Energy Technology Data Exchange (ETDEWEB)
Motevaselian, M. H.; Mashayak, S. Y.; Aluru, N. R., E-mail: aluru@illinois.edu [Department of Mechanical Science and Engineering, Beckman Institute for Advanced Science and Technology, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801 (United States)
2015-09-28
Empirical potential-based quasi-continuum theory (EQT) provides a route to incorporate atomistic detail into continuum framework such as the Nernst-Planck equation. EQT can also be used to construct a grand potential functional for classical density functional theory (cDFT). The combination of EQT and cDFT provides a simple and fast approach to predict the inhomogeneous density, potential profiles, and thermodynamic properties of confined fluids. We extend the EQT-cDFT approach to confined fluid mixtures and demonstrate it by simulating a mixture of methane and hydrogen inside slit-like channels of graphene. We show that the EQT-cDFT predictions for the structure of the confined fluid mixture compare well with the molecular dynamics simulation results. In addition, our results show that graphene slit nanopores exhibit a selective adsorption of methane over hydrogen.
Fusion process of Lennard-Jones clusters: global minima and magic numbers formation
DEFF Research Database (Denmark)
Solov'yov, Ilia; Solov'yov, Andrey V.; Greiner, Walter
2004-01-01
We present a new theoretical framework for modeling the fusion process of Lennard–Jones (LJ) clusters. Starting from the initial tetrahedral cluster configuration, adding new atoms to the system and absorbing its energy at each step, we find cluster growing paths up to the cluster size of 150 atoms...
Efficient Implementations of Molecular Dynamics Simulations for Lennard-Jones Systems
Watanabe, H.; Suzuki, M.; Ito, N.
2011-01-01
simple spatialdecomposition-based strategy is adopted for parallelization. By utilizing the developed code, benchmark simulations are performed on a HITACHI SR16000/J2 system consisting of IBM POWER6 processors which are 4.7 GHz at the National Institute
Interaction forces between nanoparticles in Lennard-Jones (L-J) solvents
International Nuclear Information System (INIS)
Sinha, Indrajit; Mukherjee, Ashim K
2014-01-01
Molecular simulations, such as Monte Carlo (MC) and molecular dynamics (MD) have been recently used for understanding the forces between colloidal nanoparticles that determine the dispersion and stability of nanoparticle suspensions. Herein we review the current status of research in the area of nanoparticles immersed in L-J solvents. The first study by Shinto et al. used large smooth spheres to depict nanoparticles in L-J and soft sphere solvents. The nanoparticles were held fixed at a particular interparticle distance and only the solvents were allowed to equilibrate. Both Van-der-waals and solvation forces were computed at different but fixed interparticle separation. Later Qin and Fitchthorn improved on this model by considering the nanoparticles as collection of molecules, thus taking into the account the effect of surface roughness of nanoparticles. Although the inter particle distance was fixed, the rotation of such nanoparticles with respect to each other was also investigated. Recently, in keeping with the experimental situation, we modified this model by allowing the nanoparticles to move and rotate freely. Solvophilic, neutral and solvophobic interactions between the solvent atoms and those that make up the nanoparticles were modelled. While neutral and solvophobic nanoparticles coalesce even at intermediate distances, solvophilic nanoparticles are more stable in solution due to the formation of a solvent shield
Molecular dynamics calculation of half-lives for thermal decay of Lennard-Jones clusters
International Nuclear Information System (INIS)
Smith, R.W.
1991-01-01
Molecular dynamics has been used with a Lenard-Jones (6-12) potential in order to study the decay behavior of neutral Argon clusters containing between 12 and 14 atoms. The clusters were heated to temperatures well above their melting points and then tracked in time via molecular dynamics until evaporation of one or more atoms was observed. In each simulation, the mode of evaporation, energy released during evaporation, and cluster lifetime were recorded. Results from roughly 2000 simulation histories were combined in order to compute statistically significant values of cluster half-lives and decay energies. It was found that cluster half-life decreases with increasing energy and that for a given value of excess energy (defined as E=(E tot -E gnd )/n), the 13 atom cluster is more stable against decay than clusters containing either 12 or 14 atoms. The dominant decay mechanism for all clusters was determined to be single atom emission. (orig.)
Single-site Lennard-Jones models via polynomial chaos surrogates of Monte Carlo molecular simulation
Kadoura, Ahmad Salim; Siripatana, Adil; Sun, Shuyu; Knio, Omar; Hoteit, Ibrahim
2016-01-01
In this work, two Polynomial Chaos (PC) surrogates were generated to reproduce Monte Carlo (MC) molecular simulation results of the canonical (single-phase) and the NVT-Gibbs (two-phase) ensembles for a system of normalized structureless Lennard
A Nanodroplet Processor for Advanced Microencapsulated Drug Formulations, Phase I
National Aeronautics and Space Administration — The objective of this proposal is to provide a demonstration of a nanodroplet synthesis of multifunctional liposomes for drug delivery based on immiscible...
Thermophoretic Motion of Water Nanodroplets confined inside Carbon Nanotubes
DEFF Research Database (Denmark)
Zambrano, Harvey A; Walther, Jens Honore; Koumoutsakos, Petros
2009-01-01
We study the thermophoretic motion of water nanodroplets confined inside carbon nanotubes using molecular dynamics simulations. We find that the nanodroplets move in the direction opposite the imposed thermal gradient with a terminal velocity that is linearly proportional to the gradient....... The translational motion is associated with a solid body rotation of the water nanodroplet coinciding with the helical symmetry of the carbon nanotube. The thermal diffusion displays a weak dependence on the wetting of the water-carbon nanotube interface. We introduce the use of the Moment Scaling Spectrum (MSS......) in order to determine the characteristics of the motion of the nanoparticles inside the carbon nanotube. The MSS indicates that affinity of the nanodroplet with the walls of the carbon nanotubes is important for the isothermal diffusion, and hence for the Soret coefficient of the system....
A Nanodroplet Processor for Advanced Microencapsulated Drug Formulations, Phase II
National Aeronautics and Space Administration — During this Phase II program we propose to build on the key aspects of the nanodroplet encapsulation technology to demonstrate optimized formulation and...
Chakraborty, Monojit; Chowdhury, Anamika; Bhusan, Richa; DasGupta, Sunando
2015-10-20
Droplet motion on a surface with chemical energy induced wettability gradient has been simulated using molecular dynamics (MD) simulation to highlight the underlying physics of molecular movement near the solid-liquid interface including the contact line friction. The simulations mimic experiments in a comprehensive manner wherein microsized droplets are propelled by the surface wettability gradient against forces opposed to motion. The liquid-wall Lennard-Jones interaction parameter and the substrate temperature are varied to explore their effects on the three-phase contact line friction coefficient. The contact line friction is observed to be a strong function of temperature at atomistic scales, confirming their experimentally observed inverse functionality. Additionally, the MD simulation results are successfully compared with those from an analytical model for self-propelled droplet motion on gradient surfaces.
Docetaxel-loaded multilayer nanoparticles with nanodroplets for cancer therapy.
Oh, Keun Sang; Kim, Kyungim; Yoon, Byeong Deok; Lee, Hye Jin; Park, Dal Yong; Kim, Eun-Yeong; Lee, Kiho; Seo, Jae Hong; Yuk, Soon Hong
2016-01-01
A mixture of docetaxel (DTX) and Solutol(®) HS 15 (Solutol) transiently formed nanodroplets when it was suspended in an aqueous medium. However, nanodroplets that comprised DTX and Solutol showed a rapid precipitation of DTX because of their unstable characteristics in the aqueous medium. The incorporation of nanodroplets that comprised DTX and Solutol through vesicle fusion and subsequent stabilization was designed to prepare multilayer nanoparticles (NPs) with a DTX-loaded Solutol nanodroplet (as template NPs) core for an efficient delivery of DTX as a chemotherapeutic drug. As a result, the DTX-loaded Solutol nanodroplets (~11.7 nm) were observed to have an increased average diameter (from 11.7 nm to 156.1 nm) and a good stability of the hydrated NPs without precipitation of DTX by vesicle fusion and multilayered structure, respectively. Also, a long circulation of the multilayer NPs was observed, and this was due to the presence of Pluronic F-68 on the surface of the multilayer NPs. This led to an improved antitumor efficacy based on the enhanced permeation and retention effect. Therefore, this study indicated that the multilayer NPs have a considerable potential as a drug delivery system with an enhanced therapeutic efficacy by blood circulation and with low side effects.
Theoretical Studies Of Nucleation Kinetics And Nanodroplet Microstructure
International Nuclear Information System (INIS)
Wilemski, Gerald
2009-01-01
The goals of this project were to (1) explore ways of bridging the gap between fundamental molecular nucleation theories and phenomenological approaches based on thermodynamic reasoning, (2) test and improve binary nucleation theory, and (3) provide the theoretical underpinning for a powerful new experimental technique, small angle neutron scattering (SANS) from nanodroplet aerosols, that can probe the compositional structure of nanodroplets. This report summarizes the accomplishments of this project in realizing these goals. Publications supported by this project fall into three general categories: (1) theoretical work on nucleation theory (2) experiments and modeling of nucleation and condensation in supersonic nozzles, and (3) experimental and theoretical work on nanodroplet structure and neutron scattering. These publications are listed and briefly summarized in this report.
Dynamics of metal nanodroplets; Dynamik metallischer Nanotroepfchen
Energy Technology Data Exchange (ETDEWEB)
Habenicht, Anja
2007-11-12
In this work flat metal nanostructures on inert substrates like glass, silicon or graphite have been illuminated by single intensive laser pulses with fluences above the melting threshold. The liquid structures produced in this way are far from their equilibrium shape and a dewetting process starts. On a timescale of a few nanoseconds, the liquid but still flat nanostructure transforms toward a sphere. During this deformation the center of mass moves upward, which can lead to detachment of droplets from the surface due to inertia. The velocity of the detaching nanodroplets is measured with a light barrier technique. The experiment shows that the velocity of the detached droplet is constant over a large range of laser energy densities. This supports the model of a dewetting driven process: The droplet gains surface energy by transforming toward a sphere which is then converted into kinetic energy. Loss mechanisms like excitation of droplet oscillations and dissipation due to viscous friction are discussed. With this model the escape velocity was predicted for nanostructures of different materials and forms, hence other material parameters like surface tension or density and has been confirmed experimentally. The droplets are landed on another surface. Two scenarios are found: There are spheres with a similar shape as the droplet or heavily deformed structures. These structures of splashing and rebounding are identical to the structures which can be observed in the macroscopic impact of liquids. The two scenarios can be explained by different temperatures of the droplets when reaching the substrate. (orig.)
God as burden: A theological reflection on art, death and God in the work of Joost Zwagerman
Directory of Open Access Journals (Sweden)
Rein Brouwer
2017-06-01
Full Text Available In one of his essays on art, Dutch author and essayist Joost Zwagerman (1963–2015 reflects onthe work of (Dutch South African artist Marlene Dumas (1953. Zwagerman addresses inparticular Dumas’ My Mother Before She Became My Mother (2010, painted 3 years after hermother died. In his reflections, Zwagerman proposes an interpretation of Dumas’ work. Hesuggests that Dumas, in her art, does not accept the omnipotence of death. Maybe againstbetter judgement, but Dumas keeps creating images that not only illustrate the desire formeaning but also embody this desire. The image and the desire for meaning merge in Dumas’paintings. The painting itself becomes an autonomous ‘desire machine’, according toZwagerman. In this article, a (practical theological reading of Zwagerman’s own posthumouslypublished volume of poetry, ‘Wakend over God’ (2016, is presented, with a specific interest inart, death and God. The sacramental hermeneutics of Richard Kearney and the theopoetics ofJohn Caputo are brought into the conversation to elicit the dimensions of faith and religion inZwagerman’s own ‘desire machine’.
Femtosecond water dynamics in reverse-micellar nanodroplets
Cringus, D; Lindner, J; Milder, MTW; Pshenichnikov, MS; Vohringer, P; Wiersma, DA; Milder, Maaike T.W.; Pshenichnikov, Maxim S.; Vöhringer, Peter
2005-01-01
Vibrational energy relaxation and ultrafast thermalization following impulsive excitation of the OH-stretching band of water nanodroplets confined to reverse micelles is studied by infrared pump-probe spectroscopy with sub-100 fs time resolution. The self-consistent analysis of experimental data for
Impulsive Laser Induced Alignment of Molecules Dissolved in Helium Nanodroplets
DEFF Research Database (Denmark)
Pentlehner, Dominik; H. Nielsen, Jens; Slenczka, Alkwin
2013-01-01
We show that a 450 fs nonresonant, moderately intense, linearly polarized laser pulse can induce field-free molecular axis alignment of methyliodide (CH3I) molecules dissolved in a helium nanodroplet. Time-resolved measurements reveal rotational dynamics much slower than that of isolated molecules...
Docetaxel-loaded multilayer nanoparticles with nanodroplets for cancer therapy
Directory of Open Access Journals (Sweden)
Oh KS
2016-03-01
Full Text Available Keun Sang Oh,1,* Kyungim Kim,1,* Byeong Deok Yoon,1 Hye Jin Lee,1 Dal Yong Park,1 Eun-yeong Kim,1 Kiho Lee,1 Jae Hong Seo,2 Soon Hong Yuk1,2 1College of Pharmacy, Korea University, Sejong, 2Biomedical Research Center, Korea University Guro Hospital, Guro-gu, Seoul, Republic of Korea *These authors contributed equally to this work Abstract: A mixture of docetaxel (DTX and Solutol® HS 15 (Solutol transiently formed nanodroplets when it was suspended in an aqueous medium. However, nanodroplets that comprised DTX and Solutol showed a rapid precipitation of DTX because of their unstable characteristics in the aqueous medium. The incorporation of nanodroplets that comprised DTX and Solutol through vesicle fusion and subsequent stabilization was designed to prepare multilayer nanoparticles (NPs with a DTX-loaded Solutol nanodroplet (as template NPs core for an efficient delivery of DTX as a chemotherapeutic drug. As a result, the DTX-loaded Solutol nanodroplets (~11.7 nm were observed to have an increased average diameter (from 11.7 nm to 156.1 nm and a good stability of the hydrated NPs without precipitation of DTX by vesicle fusion and multilayered structure, respectively. Also, a long circulation of the multilayer NPs was observed, and this was due to the presence of Pluronic F-68 on the surface of the multilayer NPs. This led to an improved antitumor efficacy based on the enhanced permeation and retention effect. Therefore, this study indicated that the multilayer NPs have a considerable potential as a drug delivery system with an enhanced therapeutic efficacy by blood circulation and with low side effects. Keywords: multilayer nanoparticles, Solutol, Pluronic F-68, docetaxel, cancer therapy
Positron probe to study the freezing of nanodroplets
International Nuclear Information System (INIS)
Pujari, P.K.
2010-01-01
Positron is an excellent in situ probe to study the phase behavior of fluid confined in nanodomains. The study of phase behavior (freezing/melting) of nano confined fluid or nanodroplet has great relevance in fundamental research as well as applications in nano-tribology, nanofabrication, membrane separation, interfacial adhesion and lubrication. It is seen that the properties of freezing/melting of nanodroplets are different from their bulk behavior due to the combined effects of finite size, surface force, surface anisotropy, pore disorder and reduced dimensionality. We have used positron annihilation spectroscopy (PAS) to study the freezing/melting behavior of different organic liquids like benzene, ethylene glycol and isopropanol confined in nanopores of ZSM5 zeolite and silica gel
Drug Release from Phase-Changeable Nanodroplets Triggered by Low-Intensity Focused Ultrasound
Cao, Yang; Chen, Yuli; Yu, Tao; Guo, Yuan; Liu, Fengqiu; Yao, Yuanzhi; Li, Pan; Wang, Dong; Wang, Zhigang; Chen, Yu; Ran, Haitao
2018-01-01
Background: As one of the most effective triggers with high tissue-penetrating capability and non-invasive feature, ultrasound shows great potential for controlling the drug release and enhancing the chemotherapeutic efficacy. In this study, we report, for the first time, construction of a phase-changeable drug-delivery nanosystem with programmable low-intensity focused ultrasound (LIFU) that could trigger drug-release and significantly enhance anticancer drug delivery. Methods: Liquid-gas phase-changeable perfluorocarbon (perfluoropentane) and an anticancer drug (doxorubicin) were simultaneously encapsulated in two kinds of nanodroplets. By triggering LIFU, the nanodroplets could be converted into microbubbles locally in tumor tissues for acoustic imaging and the loaded anticancer drug (doxorubicin) was released after the microbubble collapse. Based on the acoustic property of shell materials, such as shell stiffness, two types of nanodroplets (lipid-based nanodroplets and PLGA-based nanodroplets) were activated by different acoustic pressure levels. Ultrasound irradiation duration and power of LIFU were tested and selected to monitor and control the drug release from nanodroplets. Various ultrasound energies were introduced to induce the phase transition and microbubble collapse of nanodroplets in vitro (3 W/3 min for lipid nanodroplets; 8 W/3 min for PLGA nanodroplets). Results: We detected three steps in the drug-releasing profiles exhibiting the programmable patterns. Importantly, the intratumoral accumulation and distribution of the drug with LIFU exposure were significantly enhanced, and tumor proliferation was substantially inhibited. Co-delivery of two drug-loaded nanodroplets could overcome the physical barriers of tumor tissues during chemotherapy. Conclusion: Our study provides a new strategy for the efficient ultrasound-triggered chemotherapy by nanocarriers with programmable LIFU capable of achieving the on-demand drug release. PMID:29507623
Effect of surface tension on the behavior of adhesive contact based on Lennard-Jones potential law
Zhu, Xinyao; Xu, Wei
2018-02-01
The present study explores the effect of surface tension on adhesive contact behavior where the adhesion is interpreted by long-range intermolecular forces. The adhesive contact is analyzed using the equivalent system of a rigid sphere and an elastic half space covered by a membrane with surface tension. The long-range intermolecular forces are modeled with the Lennard‒Jones (L‒J) potential law. The current adhesive contact issue can be represented by a nonlinear integral equation, which can be solved by Newton‒Raphson method. In contrast to previous studies which consider intermolecular forces as short-range, the present study reveals more details of the features of adhesive contact with surface tension, in terms of jump instabilities, pull-off forces, pressure distribution within the contact area, etc. The transition of the pull-off force is not only consistent with previous studies, but also presents some new interesting characteristics in the current situation.
Molecular Simulation of the Vapor-Liquid Phase Behavior of Lennard-Jones Mixtures in Porous Solids
2006-09-01
sur la Catalyse, Centre National de la Recherche Scientifique, Group de Chimie Theorique, 2 Avenue Albert Einstein, 69626 Villeurbanne Cedex, France...and Group de Chimie Theorique, Ecole Normale Superieure de Lyon, 46 Allee d’Italie, 69364 Lyon, Cedex 07, France 14. ABSTRACT We present vapor...Scientifique, Group de Chimie Theorique, 2 Avenue Albert Einstein, 69626 Villeurbanne Cedex, France and Group de Chimie Theorique, Ecole Normale
Scaling relation and regime map of explosive gas–liquid flow of binary Lennard-Jones particle system
Inaoka, Hajime; Yukawa, Satoshi; Ito, Nobuyasu
2012-01-01
liquid droplets, and gas particles, which remain supercritical gaseous states under the depressurization realized by simulations. The system has a pipe-like structure similar to the model of a shock tube. We observed physical quantities and flow regimes
International Nuclear Information System (INIS)
Hoover, W.G.; Evans, D.J.; Hickman, R.B.; Ladd, A.J.C.; Ashurst, W.T.; Moran, B.
1980-01-01
A new Hamiltonian method for deformation simulations is related to the Green-Kubo fluctuation theory through perturbation theory and linear-response theory. Numerical results for the bulk and shear viscosity coefficients are compared to corresponding Green-Kubo calculations. Both viscosity coefficients depend similarly on frequency, in a way consistent with enhanced ''long-time tails.''
Lennard-Jones fluids in two-dimensional nano-pores. Multi-phase coexistence and fluid structure
Yatsyshin, Petr; Savva, Nikos; Kalliadasis, Serafim
2014-03-01
We present a number of fundamental findings on the wetting behaviour of nano-pores. A popular model for fluid confinement is a one-dimensional (1D) slit pore formed by two parallel planar walls and it exhibits capillary condensation (CC): a first-order phase transition from vapour to capillary-liquid (Kelvin shift). Capping such a pore at one end by a third orthogonal wall forms a prototypical two-dimensional (2D) pore. We show that 2D pores possess a wetting temperature such that below this temperature CC remains of first order, above it becomes a continuous phase transition manifested by a slab of capillary-liquid filling the pore from the capping wall. Continuous CC exhibits hysteresis and can be preceded by a first-order capillary prewetting transition. Additionally, liquid drops can form in the corners of the 2D pore (remnant of 2D wedge prewetting). The three fluid phases, vapour, capillary-liquid slab and corner drops, can coexist at the pore triple point. Our model is based on the statistical mechanics of fluids in the density functional formulation. The fluid-fluid and fluid-substrate interactions are dispersive. We analyze in detail the microscopic fluid structure, isotherms and full phase diagrams. Our findings also suggest novel ways to control wetting of nano-pores. We are grateful to the European Research Council via Advanced Grant No. 247031 for support.
Atomic Scale Imaging of Nucleation and Growth Trajectories of an Interfacial Bismuth Nanodroplet.
Li, Yingxuan; Bunes, Benjamin R; Zang, Ling; Zhao, Jie; Li, Yan; Zhu, Yunqing; Wang, Chuanyi
2016-02-23
Because of the lack of experimental evidence, much confusion still exists on the nucleation and growth dynamics of a nanostructure, particularly of metal. The situation is even worse for nanodroplets because it is more difficult to induce the formation of a nanodroplet while imaging the dynamic process with atomic resolution. Here, taking advantage of an electron beam to induce the growth of Bi nanodroplets on a SrBi2Ta2O9 platelet under a high resolution transmission electron microscope (HRTEM), we directly observed the detailed growth pathways of Bi nanodroplets from the earliest stage of nucleation that were previously inaccessible. Atomic scale imaging reveals that the dynamics of nucleation involves a much more complex trajectory than previously predicted based on classical nucleation theory (CNT). The monatomic Bi layer was first formed in the nucleation process, which induced the formation of the prenucleated clusters. Following that, critical nuclei for the nanodroplets formed both directly from the addition of atoms to the prenucleated clusters by the classical growth process and indirectly through transformation of an intermediate liquid film based on the Stranski-Krastanov growth mode, in which the liquid film was induced by the self-assembly of the prenucleated clusters. Finally, the growth of the Bi nanodroplets advanced through the classical pathway and sudden droplet coalescence. This study allows us to visualize the critical steps in the nucleation process of an interfacial nanodroplet, which suggests a revision of the perspective of CNT.
Directory of Open Access Journals (Sweden)
Sophie Reinders
2012-03-01
Full Text Available This article analyzes Joost van den Vondel's career strategies and shows that the ambition for obtaining patronage as a poet played a crucial role in the dedications of his consecutive Vergil translations. In the period 1646-1660 Vondel published three Dutch translations of Vergil, one in prose, one 'preview' of the poetry translation, and a final translation of the complete works rendered in verse. For each of the individual dedicatees, the Prince of Orange, the son of the Amsterdam burgomaster Cornelis de Graeff, and the mighty burgomaster himself, the publications' paratexts work to achieve a single goal by means of this work of art: obtaining structural patronage for composing an epic.
Docetaxel-loaded multilayer nanoparticles with nanodroplets for cancer therapy
Oh, Keun Sang; Kim, Kyungim; Yoon, Byeong Deok; Lee, Hye Jin; Park, Dal Yong; Kim, Eun-yeong; Lee, Kiho; Seo, Jae Hong; Yuk, Soon Hong
2016-01-01
Keun Sang Oh,1,* Kyungim Kim,1,* Byeong Deok Yoon,1 Hye Jin Lee,1 Dal Yong Park,1 Eun-yeong Kim,1 Kiho Lee,1 Jae Hong Seo,2 Soon Hong Yuk1,2 1College of Pharmacy, Korea University, Sejong, 2Biomedical Research Center, Korea University Guro Hospital, Guro-gu, Seoul, Republic of Korea *These authors contributed equally to this work Abstract: A mixture of docetaxel (DTX) and Solutol® HS 15 (Solutol) transiently formed nanodroplets when it was suspended in an aqueous medium. However, n...
Dipole moments of molecules solvated in helium nanodroplets
International Nuclear Information System (INIS)
Stiles, Paul L.; Nauta, Klaas; Miller, Roger E.
2003-01-01
Stark spectra are reported for hydrogen cyanide and cyanoacetylene solvated in helium nanodroplets. The goal of this study is to understand the influence of the helium solvent on measurements of the permanent electric dipole moment of a molecule. We find that the dipole moments of the helium solvated molecules, calculated assuming the electric field is the same as in vacuum, are slightly smaller than the well-known gas-phase dipole moments of HCN and HCCCN. A simple elliptical cavity model quantitatively accounts for this difference, which arises from the dipole-induced polarization of the helium
Electron driven water formation from oxyhydrogen clusters in superfluid helium nanodroplets
International Nuclear Information System (INIS)
Renzler, Michael; Kranabetter, Lorenz; Barwa, Erik; Scheier, Paul; Illenberger, Eugen
2015-01-01
Helium nanodroplets provide an enviroment that allow studies of chemical reactions at ultracold temperatures. We use these droplets as a matrix to study the formation of water upon electron bombardment of oxyhydrogen clusters (paper)
Analysis of the Efficiency of Surfactant-Mediated Stabilization Reactions of EGaIn Nanodroplets.
Finkenauer, Lauren R; Lu, Qingyun; Hakem, Ilhem F; Majidi, Carmel; Bockstaller, Michael R
2017-09-26
A methodology based on light scattering and spectrophotometry was developed to evaluate the effect of organic surfactants on the size and yield of eutectic gallium/indium (EGaIn) nanodroplets formed in organic solvents by ultrasonication. The process was subsequently applied to systematically evaluate the role of headgroup chemistry as well as polar/apolar interactions of aliphatic surfactant systems on the efficiency of nanodroplet formation. Ethanol was found to be the most effective solvent medium in promoting the formation and stabilization of EGaIn nanodroplets. For the case of thiol-based surfactants in ethanol, the yield of nanodroplet formation increased with the number of carbon atoms in the aliphatic part. In the case of the most effective surfactant system-octadecanethiol-the nanodroplet yield increased by about 370% as compared to pristine ethanol. The rather low overall efficiency of the reaction process along with the incompatibility of surfactant-stabilized EGaIn nanodroplets in nonpolar organic solvents suggests that the stabilization mechanism differs from the established self-assembled monolayer formation process that has been widely observed in nanoparticle formation.
Evaluating the Laplace pressure of water nanodroplets from simulations
Malek, Shahrazad M. A.; Sciortino, Francesco; Poole, Peter H.; Saika-Voivod, Ivan
2018-04-01
We calculate the components of the microscopic pressure tensor as a function of radial distance r from the centre of a spherical water droplet, modelled using the TIP4P/2005 potential. To do so, we modify a coarse-graining method for calculating the microscopic pressure (Ikeshoji et al 2003 Mol. Simul. 29 101) in order to apply it to a rigid molecular model of water. As test cases, we study nanodroplets ranging in size from 776 to 2880 molecules at 220 K. Beneath a surface region comprising approximately two molecular layers, the pressure tensor becomes approximately isotropic and constant with r. We find that the dependence of the pressure on droplet radius is that expected from the Young-Laplace equation, despite the small size of the droplets.
Dynamics of photoexcited Ba+ cations in 4He nanodroplets
International Nuclear Information System (INIS)
2UB, Universitat de Barcelona, Diagonal 645, 08028 Barcelona (Spain))" data-affiliation=" (Departament ECM, Facultat de Física, and IN2UB, Universitat de Barcelona, Diagonal 645, 08028 Barcelona (Spain))" >Leal, Antonio; 2UB, Universitat de Barcelona, Diagonal 645, 08028 Barcelona (Spain))" data-affiliation=" (Departament ECM, Facultat de Física, and IN2UB, Universitat de Barcelona, Diagonal 645, 08028 Barcelona (Spain))" >Pi, Martí; Zhang, Xiaohang; Drabbels, Marcel; 2UB, Universitat de Barcelona, Diagonal 645, 08028 Barcelona (Spain); Laboratoire des Collisions, Agrégats, Réactivité, IRSAMC, UMR 5589, CNRS et Université Paul Sabatier-Toulouse 3, 118 route de Narbonne, F-31062 Toulouse Cedex 09 (France))" data-affiliation=" (Departament ECM, Facultat de Física, and IN2UB, Universitat de Barcelona, Diagonal 645, 08028 Barcelona (Spain); Laboratoire des Collisions, Agrégats, Réactivité, IRSAMC, UMR 5589, CNRS et Université Paul Sabatier-Toulouse 3, 118 route de Narbonne, F-31062 Toulouse Cedex 09 (France))" >Barranco, Manuel; Cargnoni, Fausto; Hernando, Alberto; Mateo, David; Mella, Massimo
2016-01-01
We present a joint experimental and theoretical study on the desolvation of Ba + cations in 4 He nanodroplets excited via the 6p ← 6s transition. The experiments reveal an efficient desolvation process yielding mainly bare Ba + cations and Ba + He n exciplexes with n = 1 and 2. The speed distributions of the ions are well described by Maxwell-Boltzmann distributions with temperatures ranging from 60 to 178 K depending on the excitation frequency and Ba + He n exciplex size. These results have been analyzed by calculations based on a time-dependent density functional description for the helium droplet combined with classical dynamics for the Ba + . In agreement with experiment, the calculations reveal the dynamical formation of exciplexes following excitation of the Ba + cation. In contrast to experimental observation, the calculations do not reveal desolvation of excited Ba + cations or exciplexes, even when relaxation pathways to lower lying states are included.
Chang, Nan; Lu, Shukuan; Qin, Dui; Xu, Tianqi; Han, Meng; Wang, Supin; Wan, Mingxi
2018-07-01
A HIFU sequence with extremely short pulse duration and high pulse repetition frequency can achieve thermal ablation at a low acoustic power using inertial cavitation. Because of its cavitation-dependent property, the therapeutic outcome is unreliable when the treatment zone lacks cavitation nuclei. To overcome this intrinsic limitation, we introduced perfluorocarbon nanodroplets as extra cavitation nuclei into short-pulsed HIFU-mediated thermal ablation. Two types of nanodroplets were used with perfluorohexane (PFH) as the core material coated with bovine serum albumin (BSA) or an anionic fluorosurfactant (FS) to demonstrate the feasibility of this study. The thermal ablation process was recorded by high-speed photography. The inertial cavitation activity during the ablation was revealed by sonoluminescence (SL). The high-speed photography results show that the thermal ablation volume increased by ∼643% and 596% with BSA-PFH and FS-PFH, respectively, than the short-pulsed HIFU alone at an acoustic power of 19.5 W. Using nanodroplets, much larger ablation volumes were created even at a much lower acoustic power. Meanwhile, the treatment time for ablating a desired volume significantly reduced in the presence of nanodroplets. Moreover, by adjusting the treatment time, lesion migration towards the HIFU transducer could also be avoided. The SL results show that the thermal lesion shape was significantly dependent on the inertial cavitation in this short-pulsed HIFU-mediated thermal ablation. The inertial cavitation activity became more predictable by using nanodroplets. Therefore, the introduction of PFH nanodroplets as extra cavitation nuclei made the short-pulsed HIFU thermal ablation more efficient by increasing the ablation volume and speed, and more controllable by reducing the acoustic power and preventing lesion migration. Copyright © 2018. Published by Elsevier B.V.
Thermophoretic transport of water nanodroplets conﬁned in carbon nanotubes: the role of friction
DEFF Research Database (Denmark)
Oyarzua, Elton; Walther, Jens Honore; Zambrano, Harvey
The development of eﬃcient nanoﬂuidic devices requires driving mechanisms that provide controlled transport of ﬂuids through nanoconduits. Temperature gradients have been proposed as a mechanism to drive particles, fullerenes and nanodroplets inside carbon nanotubes (CNTs). In this work, molecular...... dynamics (MD) simulations are conducted to study thermophoresis of water nanodroplets inside CNTs. To gain insight into the interplay between the thermophoretic force acting on the droplet and the retarding liquid-solid friction, sets of constrained and unconstrained MD simulations are conducted...
Lithium atoms on helium nanodroplets: Rydberg series and ionization dynamics
Lackner, Florian; Krois, Günter; Ernst, Wolfgang E.
2017-11-01
The electronic excitation spectrum of lithium atoms residing on the surface of helium nanodroplets is presented and analyzed employing a Rydberg-Ritz approach. Utilizing resonant two-photon ionization spectroscopy, two different Rydberg series have been identified: one assigned to the nS(Σ) series and the other with predominantly nP(Π) character. For high Rydberg states, which have been resolved up to n = 13, the surrounding helium effectively screens the valence electron from the Li ion core, as indicated by the apparent red-shift of Li transitions and lowered quantum defects on the droplet with respect to their free atom counterparts. For low n states, the screening effect is weakened and the prevailing repulsive interaction gives rise to strongly broadened and blue-shifted transitions. The red-shifts originate from the polarization of nearby He atoms by the positive Li ion core. As a consequence of this effect, the ionization threshold is lowered by 116 ± 10 cm-1 for Li on helium droplets with a radius of about 40 Å. Upon single-photon ionization, heavy complexes corresponding to Li ions attached to intact helium droplets are detected. We conclude that ionization close to the on-droplet ionization threshold triggers a dynamic process in which the Li ion core undergoes a transition from a surface site into the droplet.
Baghbani, Fatemeh; Chegeni, Mahdieh; Moztarzadeh, Fathollah; Hadian-Ghazvini, Samaneh; Raz, Majid
2017-05-01
Ultrasound-responsive nanodroplets are a class of new emerging smart drug delivery systems which provide image-guided nano-therapy of various diseases, especially cancers. Here, we developed multifunctional smart curcumin-loaded chitosan/perfluorohexane nanodroplets for contrast-ultrasound imaging and on-demand drug delivery. The nanodroplets were synthesized via nanoemulsion process. The optimal formulation with the size of 101.2nm and 77.8% curcumin entrapment was chosen for release study and cytotoxicity evaluation. Sonication at the frequency of 1MHz, 2W/cm 2 for 4min triggered the release of 63.5% of curcumin from optimal formulation (Cur-NDs-2). Ultrasound aided release study indicated that the concentration of perfluorohexane and the degree of acoustic droplet vaporization play important role in ultrasound-active drug release. B-mode ultrasound imaging confirmed strong ultrasound contrast of chitosan nanodroplets even at low concentrations via droplet to bubble transition. Finally, cytotoxicity of the ultrasound-responsive nanodroplets in the presence of ultrasound was evaluated in-vitro on 4T1 human breast cancer cells. Cell growth inhibitory effects of curcumin-loaded nanodroplets significantly increased by ultrasound exposure. According to the obtained results, these ultrasound responsive curcumin-loaded chitosan/perfluorohexane nanodroplets have a great potential for imaged-guided cancer therapy. Copyright © 2016 Elsevier B.V. All rights reserved.
Electron attachment and electron ionization of acetic acid clusters embedded in helium nanodroplets
da Silva, F. Ferreira; Jaksch, S.; Martins, G.; Dang, H. M.; Dampc, M.; Denifl, S.; Maerk, T. D.; Limao-Vieira, P.; Liu, J.; Yang, S.; Ellis, A. M.; Scheier, P.
2009-01-01
The effect of incident electrons on acetic acid clusters is explored for the first time. The acetic acid clusters are formed inside liquid helium nanodroplets and both cationic and anionic products ejected into the gas phase are detected by mass spectrometry. The cation chemistry (induced by
Two-pulse driving of D+D nuclear fusion within a single Coulomb exploding nanodroplet
International Nuclear Information System (INIS)
Last, Isidore; Jortner, Joshua; Peano, Fabio; Silva, Luis O.
2010-01-01
This paper presents a computational study of D+D fusion driven by Coulomb explosion (CE) within a single, homonuclear deuterium nanodroplet, subjected to double-pulse ultraintense laser irradiation. This irradiation scheme results in the attainment (by the first weaker pulse) of a transient inhomogeneous density profile, which serves as a target for the driving (by the second superintense pulse) of nonuniform CE that triggers overrun effects and induces intrananodroplet (INTRA) D+D fusion. Scaled electron and ion dynamics simulations were utilized to explore the INTRA D+D fusion yields for double-pulse, near-infrared laser irradiation of deuterium nanodroplets. The dependence of the INTRA yield on the nanodroplet size and on the parameters of the two laser pulses was determined, establishing the conditions for the prevalence of efficient INTRA fusion. The INTRA fusion yields are amenable to experimental observation within an assembly of nanodroplets. The INTRA D+D fusion can be distinguished from the concurrent internanodroplet D+D fusion reaction occurring in the macroscopic plasma filament and outside it in terms of the different energies of the neutrons produced in these two channels.
The effect of the molecular mass on the sputtering by electrosprayed nanodroplets
Energy Technology Data Exchange (ETDEWEB)
Borrajo-Pelaez, Rafael; Gamero-Castaño, Manuel, E-mail: mgameroc@uci.edu
2015-07-30
Highlights: • We study the effect of the molecular mass on nanodroplet sputtering of silicon. • The impact phenomenology is a strong function of the projectile’s molecular mass. • Nanodroplet sputtering intrinsically is a molecular scale phenomenon. - Abstract: Energetic bombardment of covalently bonded materials by electrosprayed nanodroplets causes sputtering and topographic changes on the surface of the target. This work investigates the influence of the projectile's molecular mass on these phenomena by sputtering single-crystal silicon wafers with a variety of liquids (molecular masses between 45.0 and 773.3 amu), and acceleration voltages. The electrosprays are characterized via time of flight to determine the charge to mass ratio of the nanodroplets which, together with the acceleration voltage, yield the impact velocity, the stagnation pressure, and the molecular kinetic energy of the projectile. The estimated range of droplet diameters is 20–79 nm, while the impact velocity, the stagnation pressure and the molecular kinetic energy range between 2.9–10 km/s, 4.7–63 GPa, and 2.1–98 eV. We find that the damage on the surface of the targets strongly depends on the molecular mass of the projectile: liquids with low molecular mass sputter significantly less and produce nanometric indentations and low surface roughness, the latter increasing moderately with stagnation pressure; in contrast, the roughness and sputtering caused by the impacts of droplets with larger molecular mass reach significantly higher values, and exhibit non-monotonic behaviors. The maximum sputtering yields for formamide, EAN, EMI-BF{sub 4}, EMI-Im, TES, and TPP are 0.20, 0.75, 1.20, 2.80, 4.00 and 2.90 silicon atoms per molecule in the projectile. These trends indicate that despite their rather large diameters, the sputtering by electrosprayed nanodroplets is intrinsically a molecular scale phenomenon.
Molecular rotation and dynamics in superfluid helium-4 nanodroplets
Callegari, Carlo
2000-11-01
Cavity-enhanced laser radiation, coupled to molecular- beam bolometric detection has been used to study the spectroscopy of acetylenic molecules embedded in helium nanodroplets. The 2ν1 transition (CH stretch overtone) of HCN, DCCH, NCCCH, CH3CCH, CF3CCH, (CH 3)3CCCH, (CH3)3SiCCH, has been investigated in the 1.5 μm spectral region by means of a color center laser coupled to a resonant build-up cavity, which enhances the laser power experienced by the molecules in the beam by up to a factor of 400, thus overcoming the weakness of the (dipole forbidden) transitions. All molecules are observed to rotate freely in the liquid cluster environment, with strongly enhanced moments of inertia, but with negligible matrix induced shifts (less than 1 cm-1). We show that this enhancement is largely accounted for by hydrodynamic effects, which we have modeled and numerically calculated. While in the gas phase the rotational lines have instrument-limited widths (a few MHZ), in the droplets we have observed linewidths ranging from 600 MHz for (CH3)3SiCCH to 2.8GHz for (CH3) 3CCCH. To investigate the nature of the broadening (which was widely believed to be homogeneous), we have performed a series of infrared (IR) saturation experiments on the 2ν1 transition. We have also thoroughly investigated NCCCH by means of microwave (MW) single-resonance experiments (on rotational transitions) and double-resonance (MW-MW and MW-IR) experiments. The results demonstrate that the spectral features of molecules in He droplets are inhomogeneously broadened, and allow an estimate of the importance of the different broadening contributions. In particular, MW-IR measurements show that the size of the cluster greatly affects the way rotational energy is relaxed. Large clusters seem to follow a ``strong collision model'' where memory of the initial rotational state is completely lost after each ``relaxation'' event, while for smaller clusters relaxation rates are probably affected by the lower
Molecular rotation and dynamics in superfluid ^4He nanodroplets
Callegari, Carlo
2001-05-01
Cavity-enhanced laser radiation, coupled to molecular-beam bolometric detection has been used to study the spectroscopy of acetylenic molecules embedded in helium nanodroplets. The 2ν1 transition (CH stretch overtone) of HCN, DCCH, NCCCH, CH_3CCH, CF_3CCH, (CH_3)_3CCCH, (CH_3)_3SiCCH, has been investigated in the 1.5 μm spectral region by means of a color center laser coupled to a resonant buildup cavity, which enhances the laser power experienced by the molecules in the beam by up to a factor of 400, thus overcoming the weakness of the (harmonically forbidden) transitions. All molecules are observed to rotate freely in the liquid cluster environment, with strongly enhanced moments of inertia, but with negligible matrix induced shifts (less than 1 cm-1). We show that this enhancement is largely accounted for by hydrodynamic effects, which we have modeled and numerically calculated. While in the gas phase the rotational lines have instrument-limited widths (a few MHz), in the droplets we have observed linewidths ranging from 600 MHz for (CH_3)_3SiCCH to 2.8 GHz for (CH_3)_3CCCH. To investigate the nature of the broadening (which was widely believed to be homogeneous), we have performed a series of infrared (IR) saturation experiments on the 2ν1 transition. We have also thoroughly investigated NCCCH by means of microwave (MW) single-resonance experiments (on rotational transitions) and double-resonance (MW-MW and MW-IR) experiments. The results demonstrate that the spectral features of molecules in He droplets are inhomogeneously broadened, and allow an estimate of the importance of the different broadening contributions. In particular, MW-IR measurements show that the size of the cluster greatly affects the way rotational energy is relaxed. Large clusters seem to follow a ``strong collision model'' where memory of the initial rotational state is completely lost after each ``relaxation'' event, while for smaller clusters relaxation rates are probably affected by
Kontrastide maa Brasiilia / Meelis Joost
Joost, Meelis
2011-01-01
Artikli autor kuulus Euroopa Majandus- ja Sotsiaalkomitee delegatsioon, mis külastas lihavõttenädalale järgneval nädalal Brasiilia Majandus– ja Sotsiaalnõukogu kutsel Brasiilia Föderatsiooni pealinna Brasíliat ning riigi esimest pealinna, praegust Bahia osariigi pealinna Salvadori, et osaleda 4. EL– Brasiilia kodanikuühiskonna ümarlaual
Wu, Shih-Ying; Fix, Samantha M.; Arena, Christopher B.; Chen, Cherry C.; Zheng, Wenlan; Olumolade, Oluyemi O.; Papadopoulou, Virginie; Novell, Anthony; Dayton, Paul A.; Konofagou, Elisa E.
2018-02-01
Focused ultrasound with nanodroplets could facilitate localized drug delivery after vaporization with potentially improved in vivo stability, drug payload, and minimal interference outside of the focal zone compared with microbubbles. While the feasibility of blood-brain barrier (BBB) opening using nanodroplets has been previously reported, characterization of the associated delivery has not been achieved. It was hypothesized that the outcome of drug delivery was associated with the droplet’s sensitivity to acoustic energy, and can be modulated with the boiling point of the liquid core. Therefore, in this study, octafluoropropane (OFP) and decafluorobutane (DFB) nanodroplets were used both in vitro for assessing their relative vaporization efficiency with high-speed microscopy, and in vivo for delivering molecules with a size relevant to proteins (40 kDa dextran) to the murine brain. It was found that at low pressures (300-450 kPa), OFP droplets vaporized into a greater number of microbubbles compared to DFB droplets at higher pressures (750-900 kPa) in the in vitro study. In the in vivo study, successful delivery was achieved with OFP droplets at 300 kPa and 450 kPa without evidence of cavitation damage using ¼ dosage, compared to DFB droplets at 900 kPa where histology indicated tissue damage due to inertial cavitation. In conclusion, the vaporization efficiency of nanodroplets positively impacted the amount of molecules delivered to the brain. The OFP droplets due to the higher vaporization efficiency served as better acoustic agents to deliver large molecules efficiently to the brain compared with the DFB droplets.
Interaction of SO2 with the Surface of a Water Nanodroplet.
Zhong, Jie; Zhu, Chongqin; Li, Lei; Richmond, Geraldine L; Francisco, Joseph S; Zeng, Xiao Cheng
2017-11-29
We present a comprehensive computational study of interaction of a SO 2 with water molecules in the gas phase and with the surface of various sized water nanodroplets to investigate the solvation behavior of SO 2 in different atmospheric environments. Born-Oppenheimer molecular dynamics (BOMD) simulation shows that, in the gas phase and at a temperature of 300 K, the dominant interaction between SO 2 and H 2 O is (SO 2 ) S···O (H 2 O) , consistent with previous density-functional theory (DFT) computation at 0 K. However, at the surface of a water nanodroplet, BOMD simulation shows that the hydrogen-bonding interaction of (SO 2 ) O···H (H 2 O) becomes increasingly important with the increase of droplet size, reflecting a marked effect of the water surface on the SO 2 solvation. This conclusion is in good accordance with spectroscopy evidence obtained previously (J. Am. Chem. Soc. 2005, 127, 16806; J. Am. Chem. Soc. 2006, 128, 3256). The prevailing interaction (SO 2 ) O···H (H 2 O) on a large droplet is mainly due to favorable exposure of H atoms of H 2 O at the air-water interface. Indeed, the conversion of the dominant interaction in the gas phase (SO 2 ) S···O (H 2 O) to the dominant interaction on the water nanodroplet (SO 2 ) O···H (H 2 O) may incur effects on the SO 2 chemistry in atmospheric aerosols because the solvation of SO 2 at the water surface can affect the reactive sites and electrophilicity of SO 2 . Hence, the solvation of SO 2 on the aerosol surface may have new implications when studying SO 2 chemistry in the aerosol-containing troposphere.
Technique to measure contact angle of micro/nanodroplets using atomic force microscopy
International Nuclear Information System (INIS)
Jung, Yong Chae; Bhushan, Bharat
2008-01-01
Contact angle is the primary parameter that characterizes wetting; however, the measurement techniques have been limited to droplets with a diameter as low as about 50 μm. The authors developed an atomic force microscopy-based technique to measure the contact angle of micro- and nanodroplets deposited using a modified nanoscale dispensing tip. The obtained contact angle results were compared with those of a macrodroplet (2.1 mm diameter). It was found that the contact angle on various surfaces decreases with decreasing the droplet size
International Nuclear Information System (INIS)
Lu, Gui; Hu, Han; Sun, Ying; Duan, Yuanyuan
2013-01-01
In this Letter, dynamic wetting of water nano-droplets containing non-surfactant gold nanoparticles on a gold substrate is examined via molecular dynamics simulations. The results show that the addition of non-surfactant nanoparticles hinders the nano-second droplet wetting process, attributed to the increases in both surface tension of the nanofluid and friction between nanofluid and substrate. The droplet wetting kinetics decreases with increasing nanoparticle loading and water-particle interaction energy. The observed wetting suppression and the absence of nanoparticle ordering near the contact line of nano-sized droplets differ from the wetting behaviors reported from nanofluid droplets of micron size or larger
Alignment and Imaging of the CS2 Dimer Inside Helium Nanodroplets
Pickering, James D.; Shepperson, Benjamin; Hübschmann, Bjarke A. K.; Thorning, Frederik; Stapelfeldt, Henrik
2018-03-01
The carbon disulphide (CS2) dimer is formed inside He nanodroplets and identified using fs laser-induced Coulomb explosion, by observing the CS2+ ion recoil velocity. It is then shown that a 160 ps moderately intense laser pulse can align the dimer in advantageous spatial orientations which allow us to determine the cross-shaped structure of the dimer by analysis of the correlations between the emission angles of the nascent CS2+ and S+ ions, following the explosion process. Our method will enable fs time-resolved structural imaging of weakly bound molecular complexes during conformational isomerization, including formation of exciplexes.
Communication: X-ray coherent diffractive imaging by immersion in nanodroplets
Directory of Open Access Journals (Sweden)
Rico Mayro P. Tanyag
2015-09-01
Full Text Available Lensless x-ray microscopy requires the recovery of the phase of the radiation scattered from a specimen. Here, we demonstrate a de novo phase retrieval technique by encapsulating an object in a superfluid helium nanodroplet, which provides both a physical support and an approximate scattering phase for the iterative image reconstruction. The technique is robust, fast-converging, and yields the complex density of the immersed object. Images of xenon clusters embedded in superfluid helium droplets reveal transient configurations of quantum vortices in this fragile system.
Foroutan, Masumeh; Fatemi, S. Mahmood; Esmaeilian, Farshad; Fadaei Naeini, Vahid; Baniassadi, Majid
2018-05-01
In the present work, the effect of temperature gradient on the behavior of a water nano-droplet resting on a suspended graphene was studied based on a non-equilibrium molecular dynamics simulation. The acquired results indicate that the applied temperature gradient to the suspended graphene drives the water nano-droplet to the colder region. The droplet accelerates its motion toward the cold reservoir as the temperature gradient is increased. In addition to the translational motion of the nano-droplet, the vortical motion of the water molecules was also observed. Contact angle analysis was also utilized to describe the directional motion of the nano-droplet. The translational motion of the droplet leads to the estimation of contact angle hysteresis through advancing and receding contact angles while the rotational motion resulted in the advancing and receding fronts being switched with one another through the simulation. The average displacement vector of the water molecules shows that parts of the droplet seem to stagnate while other parts rotate around them. The reason behind this particular behavior was studied based on interaction energy contours between a water molecule and the suspended graphene. The obtained data indicate that the rotational motion is in agreement with the migration of the water molecules to low interaction energy regions in order to avoid high interaction energy areas.
Chen, Cherry C; Sheeran, Paul S; Wu, Shih-Ying; Olumolade, Oluyemi O; Dayton, Paul A; Konofagou, Elisa E
2013-12-28
Focused ultrasound (FUS) in the presence of systemically administered microbubbles has been shown to locally, transiently and reversibly increase the permeability of the blood-brain barrier (BBB), thus allowing targeted delivery of therapeutic agents in the brain for the treatment of central nervous system diseases. Currently, microbubbles are the only agents that have been used to facilitate the FUS-induced BBB opening. However, they are constrained within the intravascular space due to their micron-size diameters, limiting the delivery effect at or near the microvessels. In the present study, acoustically-activated nanodroplets were used as a new class of contrast agents to mediate FUS-induced BBB opening in order to study the feasibility of utilizing these nanoscale phase-shift particles for targeted drug delivery in the brain. Significant dextran delivery was achieved in the mouse hippocampus using nanodroplets at clinically relevant pressures. Passive cavitation detection was used in the attempt to establish a correlation between the amount of dextran delivered in the brain and the acoustic emission recorded during sonication. Conventional microbubbles with the same lipid shell composition and perfluorobutane core as the nanodroplets were also used to compare the efficiency of an FUS-induced dextran delivery. It was found that nanodroplets had a higher BBB opening pressure threshold but a lower stable cavitation threshold than microbubbles, suggesting that contrast agent-dependent acoustic emission monitoring was needed. A more homogeneous dextran delivery within the targeted hippocampus was achieved using nanodroplets without inducing inertial cavitation or compromising safety. Our results offered a new means of developing the FUS-induced BBB opening technology for potential extravascular targeted drug delivery in the brain, extending the potential drug delivery region beyond the cerebral vasculature. © 2013.
Fragmentation dynamics of ionized neon trimer inside helium nanodroplets: a theoretical study.
Bonhommeau, David; Viel, Alexandra; Halberstadt, Nadine
2004-06-22
We report a theoretical study of the fragmentation dynamics of Ne(3) (+) inside helium nanodroplets, following vertical ionization of the neutral neon trimer. The motion of the neon atoms is treated classically, while transitions between the electronic states of the ionic cluster are treated quantum mechanically. A diatomics-in-molecules description of the potential energy surfaces is used, in a minimal basis set consisting of three effective p orbitals on each neon atom for the missing electron. The helium environment is modeled by a friction force acting on the neon atoms when their speed exceeds the Landau velocity. A reasonable range of values for the corresponding friction coefficient is obtained by comparison with existing experimental measurements. (c) 2004 American Institute of Physics.
Cremer, Johannes W.; Thaler, Klemens M.; Haisch, Christoph; Signorell, Ruth
2016-03-01
Photochemistry taking place in atmospheric aerosol droplets has a significant impact on the Earth's climate. Nanofocusing of electromagnetic radiation inside aerosols plays a crucial role in their absorption behaviour, since the radiation flux inside the droplet strongly affects the activation rate of photochemically active species. However, size-dependent nanofocusing effects in the photokinetics of small aerosols have escaped direct observation due to the inability to measure absorption signatures from single droplets. Here we show that photoacoustic measurements on optically trapped single nanodroplets provide a direct, broadly applicable method to measure absorption with attolitre sensitivity. We demonstrate for a model aerosol that the photolysis is accelerated by an order of magnitude in the sub-micron to micron size range, compared with larger droplets. The versatility of our technique promises broad applicability to absorption studies of aerosol particles, such as atmospheric aerosols where quantitative photokinetic data are critical for climate predictions.
Interaction of 3D dewetting nanodroplets on homogeneous and chemically heterogeneous substrates
International Nuclear Information System (INIS)
Asgari, M; Moosavi, A
2014-01-01
Long-time interaction of dewetting nanodroplets is investigated using a long-wave approximation method. Although three-dimensional (3D) droplets evolution dynamics exhibits qualitative behavior analogous to two-dimensional (2D) dynamics, there is an extensive quantitative difference between them. 3D dynamics is substantially faster than 2D dynamics. This can be related to the larger curvature and, as a consequence, the larger Laplace pressure difference between the droplets in 3D systems. The influence of various chemical heterogeneities on the behavior of droplets has also been studied. In the case of gradient surfaces, it is shown how the gradient direction could change the dynamics. For a chemical step located between the droplets, the dynamics is enhanced or weakened depending on the initial configuration of the system. (paper)
Molecular Dynamics Simulation of Water Nanodroplets on Silica Surfaces at High Air Pressures
DEFF Research Database (Denmark)
Zambrano, Harvey A; Jaffe, Richard Lawrence; Walther, Jens Honore
2010-01-01
e.g., nanobubbles. In the present work we study the role of air on the wetting of hydrophilic systems. We conduct molecular dynamics simulations of a water nanodroplet on an amorphous silica surface at different air pressures. The interaction potentials describing the silica, water, and air......Silicon dioxides-water systems are abundant in nature and play fundamental roles in a diversity of novel science and engineering applications. Although extensive research has been devoted to study the nature of the interaction between silica and water a complete understanding of the system has...... perform extensive simulations of the water- air equilibrium and calibrate the water-air interaction to match the experimental solubility of N2 and O2 in water. For the silica-water system we calibrate the water-silica interaction to match the experimental contact angle of 27º. We subsequently study...
Crystallization kinetics of Ga metallic nano-droplets under As flux
International Nuclear Information System (INIS)
Bietti, S; Somaschini, C; Sanguinetti, S
2013-01-01
We present an experimental investigation of the crystallization dynamics of Ga nano-droplets under As flux. The transformation of the metallic Ga contained in the droplets into a GaAs nano-island proceeds by increasing the size of a tiny ring of GaAs which is formed just after the Ga deposition at the rim of a droplet. The GaAs crystallization rate depends linearly on the liquid–solid interface area. The maximum growth rate is set by the As flux impinging on the droplet, thus showing an efficient As incorporation and transport despite the predicted low solubility of the As in metallic Ga at the crystallization temperatures. (paper)
Zhu, Ying; Piehowski, Paul D; Zhao, Rui; Chen, Jing; Shen, Yufeng; Moore, Ronald J; Shukla, Anil K; Petyuk, Vladislav A; Campbell-Thompson, Martha; Mathews, Clayton E; Smith, Richard D; Qian, Wei-Jun; Kelly, Ryan T
2018-02-28
Nanoscale or single-cell technologies are critical for biomedical applications. However, current mass spectrometry (MS)-based proteomic approaches require samples comprising a minimum of thousands of cells to provide in-depth profiling. Here, we report the development of a nanoPOTS (nanodroplet processing in one pot for trace samples) platform for small cell population proteomics analysis. NanoPOTS enhances the efficiency and recovery of sample processing by downscaling processing volumes to 3000 proteins are consistently identified from as few as 10 cells. Furthermore, we demonstrate quantification of ~2400 proteins from single human pancreatic islet thin sections from type 1 diabetic and control donors, illustrating the application of nanoPOTS for spatially resolved proteome measurements from clinical tissues.
Dynamics of solvation and desolvation of rubidium attached to He nanodroplets
International Nuclear Information System (INIS)
Vangerow, J. von; John, O.; Stienkemeier, F.; Mudrich, M.
2015-01-01
The real-time dynamics of photoexcited and photoionized rubidium (Rb) atoms attached to helium (He) nanodroplets is studied by femtosecond pump-probe mass spectrometry. While excited Rb atoms in the perturbed 6p-state (Rb * ) desorb off the He droplets, Rb + photoions tend to sink into the droplet interior when created near the droplet surface. The transition from Rb + solvation to full Rb * desorption is found to occur at a delay time τ ∼ 600 fs for Rb * in the 6pΣ-state and τ ∼ 1200 fs for the 6pΠ-state. Rb + He ions are found to be created by directly exciting bound Rb * He exciplex states as well as by populating bound Rb + He-states in a photoassociative ionization process
Dynamics of solvation and desolvation of rubidium attached to He nanodroplets
von Vangerow, J.; John, O.; Stienkemeier, F.; Mudrich, M.
2015-07-01
The real-time dynamics of photoexcited and photoionized rubidium (Rb) atoms attached to helium (He) nanodroplets is studied by femtosecond pump-probe mass spectrometry. While excited Rb atoms in the perturbed 6p-state (Rb*) desorb off the He droplets, Rb+ photoions tend to sink into the droplet interior when created near the droplet surface. The transition from Rb+ solvation to full Rb* desorption is found to occur at a delay time τ ˜ 600 fs for Rb* in the 6pΣ-state and τ ˜ 1200 fs for the 6pΠ-state. Rb+He ions are found to be created by directly exciting bound Rb*He exciplex states as well as by populating bound Rb+He-states in a photoassociative ionization process.
Dynamics of solvation and desolvation of rubidium attached to He nanodroplets
Energy Technology Data Exchange (ETDEWEB)
Vangerow, J. von; John, O.; Stienkemeier, F.; Mudrich, M., E-mail: mudrich@physik.uni-freiburg.de [Physikalisches Institut, Universität Freiburg, 79104 Freiburg (Germany)
2015-07-21
The real-time dynamics of photoexcited and photoionized rubidium (Rb) atoms attached to helium (He) nanodroplets is studied by femtosecond pump-probe mass spectrometry. While excited Rb atoms in the perturbed 6p-state (Rb{sup *}) desorb off the He droplets, Rb{sup +} photoions tend to sink into the droplet interior when created near the droplet surface. The transition from Rb{sup +} solvation to full Rb{sup *} desorption is found to occur at a delay time τ ∼ 600 fs for Rb{sup *} in the 6pΣ-state and τ ∼ 1200 fs for the 6pΠ-state. Rb{sup +}He ions are found to be created by directly exciting bound Rb{sup *}He exciplex states as well as by populating bound Rb{sup +}He-states in a photoassociative ionization process.
International Nuclear Information System (INIS)
Vespini, Veronica; Coppola, Sara; Grilli, Simonetta; Paturzo, Melania; Ferraro, Pietro
2013-01-01
Liquid handling at micron- and nano-scale is of paramount importance in many fields of application such as biotechnology and biochemistry. In fact, the microfluidics technologies play an important role in lab-on-a-chip devices and, in particular, the dispensing of liquid droplets is a required functionality. Different approaches have been developed for manipulating, dispensing and controlling nano-droplets under a wide variety of configurations. Here we demonstrate that nano-droplets can be drawn from liquid drop or film reservoirs through a sort of milking effect achieved by the absorption of IR laser radiation into a pyroelectric crystal. The generation of the pyroelectric field induced by the IR laser is calculated numerically and a specific experiment has been designed to visualize the electric field stream lines that are responsible for the liquid milking effect. The experiments performed are expected to open a new route for the visualization, measure and characterization procedures in the case of electrohydrodynamic applications. (paper)
International Nuclear Information System (INIS)
Droppelmann, G.
2005-09-01
In the framework of this thesis several aspects of the properties of helium nanodroplets and their dopings. The formation of the exciplexes RbHe and KHe on helium droplets was studied by means of pump-probe ionization in real time, whereby the main interest lied on the influence of the applied helium isotopes. The experiments with cesium atoms on the droplet surface aimed on the elucidation of the relaxation dynamics of the surface under regardment both of isotope and size effects. From the pump-probe measurements on the formation of the exciplex RbHe on helium nanodroplets performed in the framework of this thesis formation times of 8.5 ps for Rb 4 He and 11.6 ps for Rb 3 He resulted
Directory of Open Access Journals (Sweden)
Guo H
2017-06-01
Full Text Available Hao Guo,1 Ziming Wang,1 Quanyin Du,1 Pan Li,2 Zhigang Wang,2 Aimin Wang1 1Department of Orthopedics, Institute of Surgery Research, Daping Hospital, Third Military Medical University, Chongqing, China; 2Chongqing Key Laboratory of Ultrasound Molecular Imaging, Institute of Ultrasound Imaging, Second Affiliated Hospital of Chongqing Medical University, Chongqing, China Purpose: Bacterial biofilms on the surface of prostheses are becoming a rising concern in managing prosthetic joint infections. The inherent resistant features of biofilms render traditional antimicrobial therapy unproductive and revision surgery outcomes uncertain. This situation has prompted the exploration of novel antimicrobial strategies. The synergy of ultrasound microbubbles and vancomycin has been proposed as an efficient alternative for biofilm eradication. The purpose of this study was to evaluate the anti-biofilm effect of stimulated phase-shift acoustic nanodroplets (NDs combined with vancomycin.Materials and methods: We fabricated lipid phase-shift NDs with a core of liquid perfluoropentane. A new phase change mode for NDs incorporating an initial unfocused low-intensity pulsed ultrasound for 5 minutes and a subsequent incubation at 37°C into a 24-hour duration was developed. Methicillin-resistant Staphylococcus aureus (MRSA biofilms were incubated with vancomycin and NDs under the hybrid stimulation. Biofilm morphology following treatment was determined using confocal laser scanning microscopy and scanning electron microscopy. Resazurin assay was used to quantify bactericidal efficacy against MRSA biofilm bacteria.Results: NDs treated sequentially with ultrasound and heating at 37°C achieved gradual and substantial ND vaporization and cavitation in a successive process. NDs after stimulation were capable of generating stronger destruction on biofilm structure which was best characterized by residual circular arc margins and more dead bacteria. Furthermore, NDs
Energy Technology Data Exchange (ETDEWEB)
Saiz, Fernan [Department of Chemistry, Imperial College of Science, Technology and Medicine, South Kensington, London, SW7 2A7 (United Kingdom); Gamero-Castaño, Manuel, E-mail: mgameroc@uci.edu [Department of Mechanical and Aerospace Engineering, University of California, Irvine, California, 92697 (United States)
2016-06-15
The impact of electrosprayed nanodroplets on ceramics at several km/s alters the atomic order of the target, causing sputtering, surface amorphization and cratering. The molecular mass of the projectile is known to have a strong effect on the impact phenomenology, and this article aims to rationalize this dependency using molecular dynamics. To achieve this goal, the article models the impact of four projectiles with molecular masses between 45 and 391 amu, and identical diameters and kinetic energies, 10 nm and 63 keV, striking a silicon target. In agreement with experiments, the simulations show that the number of sputtered atoms strongly increases with molecular mass. This is due to the increasing intensity of collision cascades with molecular mass: when the fixed kinetic energy of the projectile is distributed among fewer, more massive molecules, their collisions with the target produce knock-on atoms with higher energies, which in turn generate more energetic and larger numbers of secondary and tertiary knock-on atoms. The more energetic collision cascades intensify both knock-on sputtering and, upon thermalization, thermal sputtering. Besides enhancing sputtering, heavier molecules also increase the fraction of the projectile’s energy that is transferred to the target, as well as the fraction of this energy that is dissipated.
Wetting and evaporation of salt-water nanodroplets: A molecular dynamics investigation.
Zhang, Jun; Borg, Matthew K; Sefiane, Khellil; Reese, Jason M
2015-11-01
We employ molecular dynamics simulations to study the wetting and evaporation of salt-water nanodroplets on platinum surfaces. Our results show that the contact angle of the droplets increases with the salt concentration. To verify this, a second simulation system of a thin salt-water film on a platinum surface is used to calculate the various surface tensions. We find that both the solid-liquid and liquid-vapor surface tensions increase with salt concentration and as a result these cause an increase in the contact angle. However, the evaporation rate of salt-water droplets decreases as the salt concentration increases, due to the hydration of salt ions. When the water molecules have all evaporated from the droplet, two forms of salt crystals are deposited, clump and ringlike, depending on the solid-liquid interaction strength and the evaporation rate. To form salt crystals in a ring, it is crucial that there is a pinned stage in the evaporation process, during which salt ions can move from the center to the rim of the droplets. With a stronger solid-liquid interaction strength, a slower evaporation rate, and a higher salt concentration, a complete salt crystal ring can be deposited on the surface.
Cracks and nanodroplets produced on tungsten surface samples by dense plasma jets
Ticoş, C. M.; Galaţanu, M.; Galaţanu, A.; Luculescu, C.; Scurtu, A.; Udrea, N.; Ticoş, D.; Dumitru, M.
2018-03-01
Small samples of 12.5 mm in diameter made from pure tungsten were exposed to a dense plasma jet produced by a coaxial plasma gun operated at 2 kJ. The surface of the samples was analyzed using a scanning electron microscope (SEM) before and after applying consecutive plasma shots. Cracks and craters were produced in the surface due to surface tensions during plasma heating. Nanodroplets and micron size droplets could be observed on the samples surface. An energy-dispersive spectroscopy (EDS) analysis revealed that the composition of these droplets coincided with that of the gun electrode material. Four types of samples were prepared by spark plasma sintering from powders with the average particle size ranging from 70 nanometers up to 80 μm. The plasma power load to the sample surface was estimated to be ≈4.7 MJ m-2 s-1/2 per shot. The electron temperature and density in the plasma jet had peak values 17 eV and 1.6 × 1022 m-3, respectively.
Ahadi, Elias; Konermann, Lars
2011-06-22
The ejection of solvated small ions from nanometer-sized droplets plays a central role during electrospray ionization (ESI). Molecular dynamics (MD) simulations can provide insights into the nanodroplet behavior. Earlier MD studies have largely focused on aqueous systems, whereas most practical ESI applications involve the use of organic cosolvents. We conduct simulations on mixed water/methanol droplets that carry excess NH(4)(+) ions. Methanol is found to compromise the H-bonding network, resulting in greatly increased rates of ion ejection and solvent evaporation. Considerable differences in the water and methanol escape rates cause time-dependent changes in droplet composition. Segregation occurs at low methanol concentration, such that layered droplets with a methanol-enriched periphery are formed. This phenomenon will enhance the partitioning of analyte molecules, with possible implications for their ESI efficiencies. Solvated ions are ejected from the tip of surface protrusions. Solvent bridging prior to ion secession is more extensive for methanol/water droplets than for purely aqueous systems. The ejection of solvated NH(4)(+) is visualized as diffusion-mediated escape from a metastable basin. The process involves thermally activated crossing of a ~30 kJ mol(-1) free energy barrier, in close agreement with the predictions of the classical ion evaporation model.
Application of Ultrasound to Selectively Localize Nanodroplets for Targeted Imaging and Therapy
Directory of Open Access Journals (Sweden)
Paul A. Dayton
2006-07-01
Full Text Available Lipid-coated perfluorocarbon nanodroplets are submicrometer-diameter liquid-filled droplets with proposed applications in molecularly targeted therapeutics and ultrasound (US imaging. Ultrasonic molecular imaging is unique in that the optimal application of these agents depends not only on the surface chemistry, but also on the applied US field, which can increase receptor-ligand binding and membrane fusion. Theory and experiments are combined to demonstrate the displacement of perfluorocarbon nanoparticles in the direction of US propagation, where a traveling US wave with a peak pressure on the order of megapascals and frequency in the megahertz range produces a particle translational velocity that is proportional to acoustic intensity and increases with increasing center frequency. Within a vessel with a diameter on the order of hundreds of micrometers or larger, particle velocity on the order of hundreds of micrometers per second is produced and the dominant mechanism for droplet displacement is shown to be bulk fluid streaming. A model for radiation force displacement of particles is developed and demonstrates that effective particle displacement should be feasible in the microvasculature. In a flowing system, acoustic manipulation of targeted droplets increases droplet retention. Additionally, we demonstrate the feasibility of US-enhanced particle internalization and therapeutic delivery.
Energy Technology Data Exchange (ETDEWEB)
Zhu, Ying; Piehowski, Paul D.; Zhao, Rui; Chen, Jing; Shen, Yufeng; Moore, Ronald J.; Shukla, Anil K.; Petyuk, Vladislav A.; Campbell-Thompson, Martha; Mathews, Clayton E.; Smith, Richard D.; Qian, Wei-Jun; Kelly, Ryan T.
2018-02-28
Nanoscale or single cell technologies are critical for biomedical applications. However, current mass spectrometry (MS)-based proteomic approaches require samples comprising a minimum of thousands of cells to provide in-depth profiling. Here, we report the development of a nanoPOTS (Nanodroplet Processing in One pot for Trace Samples) platform as a major advance in overall sensitivity. NanoPOTS dramatically enhances the efficiency and recovery of sample processing by downscaling processing volumes to <200 nL to minimize surface losses. When combined with ultrasensitive LC-MS, nanoPOTS allows identification of ~1500 to ~3,000 proteins from ~10 to ~140 cells, respectively. By incorporating the Match Between Runs algorithm of MaxQuant, >3000 proteins were consistently identified from as few as 10 cells. Furthermore, we demonstrate robust quantification of ~2400 proteins from single human pancreatic islet thin sections from type 1 diabetic and control donors, illustrating the application of nanoPOTS for spatially resolved proteome measurements from clinical tissues.
Dynamics of photoexcited Ba{sup +} cations in {sup 4}He nanodroplets
Energy Technology Data Exchange (ETDEWEB)
Leal, Antonio; Pi, Martí [Departament ECM, Facultat de Física, and IN" 2UB, Universitat de Barcelona, Diagonal 645, 08028 Barcelona (Spain); Zhang, Xiaohang; Drabbels, Marcel [Laboratoire de Chimie Physique Moléculaire, Swiss Federal Institute of Technology Lausanne (EPFL), CH-1015 Lausanne (Switzerland); Barranco, Manuel [Departament ECM, Facultat de Física, and IN" 2UB, Universitat de Barcelona, Diagonal 645, 08028 Barcelona (Spain); Laboratoire des Collisions, Agrégats, Réactivité, IRSAMC, UMR 5589, CNRS et Université Paul Sabatier-Toulouse 3, 118 route de Narbonne, F-31062 Toulouse Cedex 09 (France); Cargnoni, Fausto [Istituto di Scienze e Tecnologie Molecolari (ISTM), Consiglio Nazionale delle Ricerche, via Golgi 19, 20133 Milano (Italy); Hernando, Alberto [Social Thermodynamics Applied Research (SThAR), EPFL Innovation Park, Bâtiment C, CH-1015 Lausanne (Switzerland); Mateo, David [Department of Chemistry and Biochemistry, California State University at Northridge, Northridge, California 91330 (United States); Mella, Massimo [Dipartimento di Scienza ed Alta Tecnologia, Università degli Studi dell’Insubria, via Valleggio 11, 22100 Como (Italy)
2016-03-07
We present a joint experimental and theoretical study on the desolvation of Ba{sup +} cations in {sup 4}He nanodroplets excited via the 6p ← 6s transition. The experiments reveal an efficient desolvation process yielding mainly bare Ba{sup +} cations and Ba{sup +}He{sub n} exciplexes with n = 1 and 2. The speed distributions of the ions are well described by Maxwell-Boltzmann distributions with temperatures ranging from 60 to 178 K depending on the excitation frequency and Ba{sup +} He{sub n} exciplex size. These results have been analyzed by calculations based on a time-dependent density functional description for the helium droplet combined with classical dynamics for the Ba{sup +}. In agreement with experiment, the calculations reveal the dynamical formation of exciplexes following excitation of the Ba{sup +} cation. In contrast to experimental observation, the calculations do not reveal desolvation of excited Ba{sup +} cations or exciplexes, even when relaxation pathways to lower lying states are included.
International Nuclear Information System (INIS)
Saiz, Fernan; Gamero-Castaño, Manuel
2016-01-01
The impact of electrosprayed nanodroplets on ceramics at several km/s alters the atomic order of the target, causing sputtering, surface amorphization and cratering. The molecular mass of the projectile is known to have a strong effect on the impact phenomenology, and this article aims to rationalize this dependency using molecular dynamics. To achieve this goal, the article models the impact of four projectiles with molecular masses between 45 and 391 amu, and identical diameters and kinetic energies, 10 nm and 63 keV, striking a silicon target. In agreement with experiments, the simulations show that the number of sputtered atoms strongly increases with molecular mass. This is due to the increasing intensity of collision cascades with molecular mass: when the fixed kinetic energy of the projectile is distributed among fewer, more massive molecules, their collisions with the target produce knock-on atoms with higher energies, which in turn generate more energetic and larger numbers of secondary and tertiary knock-on atoms. The more energetic collision cascades intensify both knock-on sputtering and, upon thermalization, thermal sputtering. Besides enhancing sputtering, heavier molecules also increase the fraction of the projectile’s energy that is transferred to the target, as well as the fraction of this energy that is dissipated.
International Nuclear Information System (INIS)
Pentlehner, D.; Slenczka, A.
2015-01-01
Electronic spectra of organic molecules doped into superfluid helium nanodroplets show characteristic features induced by the helium environment. Besides a solvent induced shift of the electronic transition frequency, in many cases, a spectral fine structure can be resolved for electronic and vibronic transitions which goes beyond the expected feature of a zero phonon line accompanied by a phonon wing as known from matrix isolation spectroscopy. The spectral shape of the zero phonon line and the helium induced phonon wing depends strongly on the dopant species. Phonon wings, for example, are reported ranging from single or multiple sharp transitions to broad (Δν > 100 cm −1 ) diffuse signals. Despite the large number of example spectra in the literature, a quantitative understanding of the helium induced fine structure of the zero phonon line and the phonon wing is missing. Our approach is a systematic investigation of related molecular compounds, which may help to shed light on this key feature of microsolvation in superfluid helium droplets. This paper is part of a comparative study of the helium induced fine structure observed in electronic spectra of anthracene derivatives with particular emphasis on a spectrally sharp multiplet splitting at the electronic origin. In addition to previously discussed species, 9-cyanoanthracene and 9-chloroanthracene will be presented in this study for the first time
Energy Technology Data Exchange (ETDEWEB)
Douberly, Gary Elliott [Univ. of Georgia, Athens, GA (United States)
2017-11-16
The objective of our experimental research program is to isolate and stabilize transient intermediates and products of prototype combustion reactions. This will be accomplished by Helium Nanodroplet Isolation, a novel technique where liquid helium droplets freeze out high energy metastable configurations of a reacting system, permitting infrared spectroscopic characterizations of products and intermediates that result from hydrocarbon radical reactions with molecular oxygen and other small molecules relevant to combustion environments. The low temperature (0.4 K) and rapid cooling associated with He droplets provides a perfectly suited medium to isolate and probe a broad range of molecular radical and carbene systems important to combustion chemistry. The sequential addition of molecular species to He droplets often leads to the stabilization of high-energy, metastable cluster configurations that represent regions of the potential energy surface far from the global minimum. Single and double resonance IR laser spectroscopy techniques, along with Stark and Zeeman capabilities, are being used to probe the structural and dynamical properties of these systems.
Spectroscopy of Cold LiCa Molecules Formed on Helium Nanodroplets
2013-01-01
We report on the formation of mixed alkali–alkaline earth molecules (LiCa) on helium nanodroplets and present a comprehensive experimental and theoretical study of the ground and excited states of LiCa. Resonance enhanced multiphoton ionization time-of-flight (REMPI-TOF) spectroscopy and laser induced fluorescence (LIF) spectroscopy were used for the experimental investigation of LiCa from 15000 to 25500 cm–1. The 42Σ+ and 32Π states show a vibrational structure accompanied by distinct phonon wings, which allows us to determine molecular parameters as well as to study the interaction of the molecule with the helium droplet. Higher excited states (42Π, 52Σ+, 52Π, and 62Σ+) are not vibrationally resolved and vibronic transitions start to overlap. The experimental spectrum is well reproduced by high-level ab initio calculations. By using a multireference configuration interaction (MRCI) approach, we calculated the 19 lowest lying potential energy curves (PECs) of the LiCa molecule. On the basis of these calculations, we could identify previously unobserved transitions. Our results demonstrate that the helium droplet isolation approach is a powerful method for the characterization of tailor-made alkali–alkaline earth molecules. In this way, important contributions can be made to the search for optimal pathways toward the creation of ultracold alkali–alkaline earth ground state molecules from the corresponding atomic species. Furthermore, a test for PECs calculated by ab initio methods is provided. PMID:24028555
International Nuclear Information System (INIS)
Aleem, M. A.
2010-01-01
The present PhD thesis represents a broad range study of electron induced formation and stability of positive and negative ions in gas phase and superfluid helium nanodroplets. The molecules studied are of industrial, environmental, plasma and biological relevance. The knowledge obtained from the study provides new insight for the proper understanding and control on energetics and dynamics of the reactions involved in the formation and fragmentation processes of the studied molecules and clusters. The experiments are accomplished and investigated using mass spectrometric techniques for the formation of molecular and cluster ions using different mass spectrometers available in our laboratory. One part of the work is focused on electron-induced reactions of the molecules in gas phase. Especially focus is laid to electron attachment to the isomers of mononitrotolouene used as an additive to explosives. The fragile nature and high internal energy of these molecules has lead to extensive fragmentation following the ionisation process. Dissociative electron attachment to the three different isomers has shown different resonances and therefore this process can be utilized to explicitly distinguish these isomers. Anion efficiency curves of the isomers have been studied using effusive molecular beam source in combination with a hemispherical electron monochromator as well as a Nier-type ion source attached to a sector field mass spectrometer. The outcome of the experiment is a reliable and effective detection method highly desirable for environmental and security reasons. Secondly, dissociative electron ionization of acetylene and propene is studied and their data is directly related to the plasma modelling for plasma fusion and processing reactors. Temperature effects for dissociative electron attachment to halo-hydrocarbons are also measured using a trochoidal electron monochromator. The second part of the work is concerned with the investigation of electron
Joost ja Kotjuh said kultuuritegelase preemia
2011-01-01
President Toomas Hendrik Ilves andis 8. juunil 2011 üle SA Vabariigi Presidendi Kultuurirahastu noore kultuuritegelase preemia dirigent Risto Joostile ning eripreemia poeedile, esseistile ja tõlkijale Igor Kotjuhile
Electrospinning of poly(vinyl alcohol) nanofibers loaded with hexadecane nanodroplets.
Arecchi, A; Mannino, S; Weiss, J
2010-08-01
The feasibility of producing poly(vinyl alcohol) (PVA) nanofibers containing fine-disperse hexadecane droplets by electrospinning a blend of hexadecane-in-water emulsions and PVA was investigated. Hexadecane oil-in-water nanoemulsions (d(10)= 181.2 +/- 0.1 nm) were mixed with PVA at pH 4.5 to yield polymer-emulsion blends containing 0.5 to 1.5 wt% oil droplets and 8-wt% PVA. The solution properties of emulsions and emulsion-PVA blends (viscosity, conductivity, surface tension) were determined. Solutions were electrospun and the morphology and thermal properties of deposited fiber mats characterized by scanning electron microscopy and differential scanning calorimetry. Fiber mats were dissolved in buffer to liberate incorporated hexadecane droplets and the buffer solutions analyzed by optical microscopy, UV-spectroscopy, and light scattering. Analysis of dry fiber mats and their solutions showed that emulsion droplets were indeed part of the electrospun fiber structures. Depending on the concentration of hexadecane in the initial emulsion-polymer blends, droplets were dispersed in the fibers as individual droplets or in form of aggregated flocs of hexadecane droplets. Nanofibers with spindle-like perturbations or nanofibers containing bead-like structures with approximately 5 times larger than the size of droplets in the original nanoemulsion were obtained. Remarkably, incorporation of hexadecane droplets in fibers did not alter size of individual droplets, that is, no coalescence occurred. The manufacture of solid matrix containing nanodroplets could be of substantial interest for manufacturers wishing to develop encapsulation system for lipophilic functional compounds such as lipid-soluble flavors, antimicrobials, antioxidants, and bioactives with tailored release kinetics. Practical Applications: The paper describes the formation of electrospun nanofibers from hydrophilic polymers that contain fine-disperse emulsion droplets. By incorporating emulsion droplets, a
Nandi, Prithwish K.; Burnham, Christian J.; English, Niall J.
2018-01-01
Understanding water solidification, especially in "No Man's Land" (NML) (150 K < T < 235 K) is crucially important (e.g., upper-troposphere cloud processes) and challenging. A rather neglected aspect of tropospheric ice-crystallite formation is inevitably present electromagnetic fields' role. Here, we employ non-equilibrium molecular dynamics of aggressively quenched supercooled water nano-droplets in the gas phase under NML conditions, in externally applied electromagnetic (e/m) fields, elucidating significant differences between effects of static and oscillating fields: although static fields induce "electro-freezing," e/m fields exhibit the contrary - solidification inhibition. This anti-freeze action extends not only to crystal-ice formation but also restricts amorphisation, i.e., suppression of low-density amorphous ice which forms otherwise in zero-field NML environments. E/m-field applications maintain water in the deeply supercooled state in an "entropic trap," which is ripe for industrial impacts in cryo-freezing, etc.
International Nuclear Information System (INIS)
Droppelmann, G.; Buenermann, O.; Stienkemeier, F.; Schulz, C.P.
2004-01-01
Nanodroplets of either superfluid He 4 or normal fluid He 3 are doped with Rb atoms that are bound to the surface of the droplets. The formation of RbHe exciplexes upon 5P 3/2 excitation is monitored in real time by femtosecond pump-probe techniques. We find formation times of 8.5 and 11.6 ps for Rb He 4 and Rb He 3 , respectively. A comparison to calculations based on a tunneling model introduced for these systems by Reho et al. [J. Chem. Phys. 113, 9694 (2000)] shows that the proposed mechanism cannot account for our findings. Apparently, a different relaxation dynamics of the superfluid opposed to the normal fluid surface is responsible for the observed formation times
Fragmentation dynamics of ionized neon clusters (Ne(n), n=3-14) embedded in helium nanodroplets.
Bonhommeau, David; Halberstadt, Nadine; Viel, Alexandra
2006-01-14
We report a theoretical study of the nonadiabatic fragmentation dynamics of ionized neon clusters embedded in helium nanodroplets for cluster sizes up to n=14 atoms. The dynamics of the neon atoms is modeled using the molecular dynamics with quantum transitions method of Tully [J. Chem. Phys. 93, 1061 (1990)] with the nuclei treated classically and transitions between electronic states quantum mechanically. The potential-energy surfaces are derived from a diatomics-in-molecules model to which induced dipole-induced dipole interactions are added. The effect of the spin-orbit interaction is also discussed. The helium environment is modeled by a friction force acting on charged atoms whose speed exceeds the critical Landau velocity. The dependence of the fragment size distribution on the friction strength and on the initial nanodroplet size is investigated. By comparing with the available experimental data obtained for Ne3+ and Ne4+, a reasonable value for the friction coefficient, the only parameter of the model, is deduced. This value is then used to predict the effect of the helium environment on the dissociation dynamics of larger neon clusters, n=5-14. The results show stabilization of larger fragments than in the gas phase, but fragmentation is not completely caged. In addition, two types of dynamics are characterized for Ne4+: fast and explosive, therefore leaving no time for friction to cool down the process when dynamics starts on one of the highest electronic states, and slower, therefore leading to some stabilization by helium when it starts on one of the lowest electronic states.
Uras-Aytemiz, Nevin; Devlin, J. Paul
2013-07-01
Studies of catalyzed all-vapor gas-hydrate formation on a sub-second timescale have been extended with a special focus on liquid-droplet compositions at the instant of hydrate crystallization. This focus has been enabled by inclusion of methanol in the all-vapor mixture. This slows droplet to gas-hydrate conversion near 200 K to a time scale suited for standard FTIR sampling. Such droplet data are sought as a guide to ongoing efforts to reduce the amount of guest catalyst required for instant formation of the gas hydrates. For the same reason, all-vapor sampling has also been extended to the generation of long-lived liquid droplets with reduced or no water content. Observations of single-solvent droplets show that surprising quantities of gas molecules are trapped during rapid droplet growth. For example, CO2 is trapped at levels near 50 mol. % in droplets of acetone, tetrahydrofuran, or trimethylene oxide formed under CO2 pressures of several Torr in a cold-chamber at 170 K. Less but significant amounts of gas are trapped at higher temperatures, or in methanol or water-methanol droplets. The droplet metastability appears to commonly lead to formation of bubbles larger than the original nanodroplets. Besides serving as a guide for the all-vapor gas-hydrate studies, the semiquantitative evidence of extensive trapping of gases is expected to have a role in future studies of atmospheric aerosols.
International Nuclear Information System (INIS)
Khadjavi, Amina; Magnetto, Chiara; Panariti, Alice; Argenziano, Monica; Gulino, Giulia Rossana; Rivolta, Ilaria; Cavalli, Roberta; Giribaldi, Giuliana; Guiot, Caterina; Prato, Mauro
2015-01-01
Background: : In chronic wounds, efficient epithelial tissue repair is hampered by hypoxia, and balances between the molecules involved in matrix turn-over such as matrix metalloproteinases (MMPs) and tissue inhibitors of metalloproteinases (TIMPs) are seriously impaired. Intriguingly, new oxygenating nanocarriers such as 2H,3H-decafluoropentane-based oxygen-loaded nanodroplets (OLNs) might effectively target chronic wounds. Objective: : To investigate hypoxia and chitosan-shelled OLN effects on MMP/TIMP production by human keratinocytes. Methods: : HaCaT cells were treated for 24 h with 10% v/v OLNs both in normoxia or hypoxia. Cytotoxicity and cell viability were measured through biochemical assays; cellular uptake by confocal microscopy; and MMP and TIMP production by enzyme-linked immunosorbent assay or gelatin zymography. Results: : Normoxic HaCaT cells constitutively released MMP-2, MMP-9, TIMP-1 and TIMP-2. Hypoxia strongly impaired MMP/TIMP balances by reducing MMP-2, MMP-9, and TIMP-2, without affecting TIMP-1 release. After cellular uptake by keratinocytes, nontoxic OLNs abrogated all hypoxia effects on MMP/TIMP secretion, restoring physiological balances. OLN abilities were specifically dependent on time-sustained oxygen diffusion from OLN core. Conclusion: : Chitosan-shelled OLNs effectively counteract hypoxia-dependent dysregulation of MMP/TIMP balances in human keratinocytes. Therefore, topical administration of exogenous oxygen, properly encapsulated in nanodroplet formulations, might be a promising adjuvant approach to promote healing processes in hypoxic wounds. - Highlights: • Hypoxia impairs MMP9/TIMP1 and MMP2/TIMP2 balances in HaCaT human keratinocytes. • Chitosan-shelled oxygen-loaded nanodroplets (OLNs) are internalised by HaCaT cells. • OLNs are not toxic to HaCaT cells. • OLNs effectively counteract hypoxia effects on MMP/TIMP balances in HaCaT cells. • OLNs appear as promising and cost-effective therapeutic tools for hypoxic
Energy Technology Data Exchange (ETDEWEB)
Khadjavi, Amina [Dipartimento di Neuroscienze, Università di Torino, Torino (Italy); Magnetto, Chiara [Istituto Nazionale di Ricerca Metrologica (INRIM), Torino (Italy); Panariti, Alice [Dipartimento di Scienze della Salute, Università di Milano Bicocca, Monza (Italy); Argenziano, Monica [Dipartimento di Scienza e Tecnologia del Farmaco, Università di Torino, Torino (Italy); Gulino, Giulia Rossana [Dipartimento di Oncologia, Università di Torino, Torino (Italy); Rivolta, Ilaria [Dipartimento di Scienze della Salute, Università di Milano Bicocca, Monza (Italy); Cavalli, Roberta [Dipartimento di Scienza e Tecnologia del Farmaco, Università di Torino, Torino (Italy); Giribaldi, Giuliana [Dipartimento di Oncologia, Università di Torino, Torino (Italy); Guiot, Caterina [Dipartimento di Neuroscienze, Università di Torino, Torino (Italy); Prato, Mauro, E-mail: mauro.prato@unito.it [Dipartimento di Neuroscienze, Università di Torino, Torino (Italy); Dipartimento di Scienze della Sanità Pubblica e Pediatriche, Università di Torino, Torino (Italy)
2015-08-01
Background: : In chronic wounds, efficient epithelial tissue repair is hampered by hypoxia, and balances between the molecules involved in matrix turn-over such as matrix metalloproteinases (MMPs) and tissue inhibitors of metalloproteinases (TIMPs) are seriously impaired. Intriguingly, new oxygenating nanocarriers such as 2H,3H-decafluoropentane-based oxygen-loaded nanodroplets (OLNs) might effectively target chronic wounds. Objective: : To investigate hypoxia and chitosan-shelled OLN effects on MMP/TIMP production by human keratinocytes. Methods: : HaCaT cells were treated for 24 h with 10% v/v OLNs both in normoxia or hypoxia. Cytotoxicity and cell viability were measured through biochemical assays; cellular uptake by confocal microscopy; and MMP and TIMP production by enzyme-linked immunosorbent assay or gelatin zymography. Results: : Normoxic HaCaT cells constitutively released MMP-2, MMP-9, TIMP-1 and TIMP-2. Hypoxia strongly impaired MMP/TIMP balances by reducing MMP-2, MMP-9, and TIMP-2, without affecting TIMP-1 release. After cellular uptake by keratinocytes, nontoxic OLNs abrogated all hypoxia effects on MMP/TIMP secretion, restoring physiological balances. OLN abilities were specifically dependent on time-sustained oxygen diffusion from OLN core. Conclusion: : Chitosan-shelled OLNs effectively counteract hypoxia-dependent dysregulation of MMP/TIMP balances in human keratinocytes. Therefore, topical administration of exogenous oxygen, properly encapsulated in nanodroplet formulations, might be a promising adjuvant approach to promote healing processes in hypoxic wounds. - Highlights: • Hypoxia impairs MMP9/TIMP1 and MMP2/TIMP2 balances in HaCaT human keratinocytes. • Chitosan-shelled oxygen-loaded nanodroplets (OLNs) are internalised by HaCaT cells. • OLNs are not toxic to HaCaT cells. • OLNs effectively counteract hypoxia effects on MMP/TIMP balances in HaCaT cells. • OLNs appear as promising and cost-effective therapeutic tools for hypoxic
Kim, Byeonggon; Kim, Hyun Gyu; Shim, Gyu-Yeop; Park, Ji-Sub; Joo, Kyung-Il; Lee, Dong-Jin; Lee, Joun-Ho; Baek, Ji-Ho; Kim, Byeong Koo; Choi, Yoonseuk; Kim, Hak-Rin
2018-01-10
We proposed and analyzed an optically isotropic nano-droplet liquid crystal (LC) doped with high k nanoparticles (NPs), exhibiting enhanced Kerr effects, which could be operated with reduced driving voltages. For enhancing the contrast ratio together with the light efficiencies, the LC droplet sizes were adjusted to be shorter than the wavelength of visible light to reduce depolarization effects by optical scattering of the LC droplets. Based on the optical analysis of the depolarization effects, the influence of the relationship between the LC droplet size and the NP doping ratio on the Kerr effect change was investigated.
Faulkner, Ty; Miller, Isaac; Raston, Paul L.
2018-01-01
We report high-resolution infrared spectra of OCS isotopologues embedded in helium nanodroplets that were recorded with a newly built spectrometer. For the normal isotopologue, we observed the relatively weak third bending overtone band, in addition to new high J transitions in the C-O stretching fundamental, which has previously been investigated by diode laser spectroscopy [S. Grebenev et al., J. Chem. Phys. 112, 4485 (2000)]. Similar to the gas phase, the overtone band is (only) 45 cm-1 higher in energy than the fundamental, and this leads to additional broadening due to rapid vibrational relaxation that is accompanied by the creation of real/virtual phonon excitations. We also observed spectra in the C-O stretching fundamental for several minor isotopologues of OCS, including 18OCS, O13CS, and OC33S, in addition to some new peaks for OC34S. A rovibrational analysis allowed for determination of the moment of inertia of helium (ΔIHe) that couples to the rotation of OCS for each isotopologue. In the context of the adiabatic following approximation, the helium density structure that follows the rotation of OCS should essentially remain unchanged between the isotopologues, i.e., there should be no dependence of ΔIHe on the gas phase moment of inertia of OCS (IG). While this behavior was expected for the "heavy" OCS rotor investigated here, we instead found an approximately linear 1:1 relation between ΔIHe and IG, which suggests partial breakdown of the adiabatic following approximation, making OCS the heaviest molecule for which evidence for this effect has been obtained.
Energy Technology Data Exchange (ETDEWEB)
Ghosh, Deborin [Department of Chemistry, University College of Science & Technology, University of Calcutta, 92, A.P.C. Road, Kolkata 700 009 (India); Batuta, Shaikh; Begum, Naznin Ara [Bio-Organic Chemistry Lab, Department of Chemistry, Visva-Bharati University, Santiniketan 731 235 (India); Mandal, Debabrata, E-mail: dmandal.chemistry@gmail.com [Department of Chemistry, University College of Science & Technology, University of Calcutta, 92, A.P.C. Road, Kolkata 700 009 (India)
2017-04-15
The excited state intramolecular proton transfer (ESIPT) of the well-known fluorophore 4'-N,N-Dimethylamino-3-hydroxyflavone (DMA3HF) was studied in AOT/n-heptane/water reverse micelle solutions. For DMA3HF molecules located inside the AOT encapsulated polar nanodroplets, ESIPT from excited enol (E*) to tautomer (T*) forms was markedly inhibited, yielding time-constants of ≥100 ps, and followed the same trend as solvent relaxation when the ratio W= [H{sub 2}O]/[AOT] was varied. At W=0, the DMA3HF molecules were attached to the ionic AOT headgroups via strong intermolecular H-bonding, which hindered ESIPT. Addition of water changes the situation radically: water molecules form stronger H-bonds with AOT headgroups, displacing the DMA3HF, which are instead engaged in intermolecular H-bonded complexes of the type [DMA3HF···water]. ESIPT of these complex-bound fluorophores involves substantial rearrangement of H-bonding, and is coupled to solvation dynamics. With increasing W-value, solvation becomes faster, and so does ESIPT, reducing the yield of E* species. At the same time, the local environment within the nanodroplets become more more polar with gradual accumulation of water, which causes a monotonic red-shift of the E* emission peak.
McClements, Jake; Buffone, Cosimo; Shaver, Michael P; Sefiane, Khellil; Koutsos, Vasileios
2017-09-20
The self-assembly of poly(styrene-co-butadiene) random copolymers on mica surfaces was studied by varying solution concentrations and polymer molecular weights. Toluene solutions of the poly(styrene-co-butadiene) samples were spin coated onto a mica surface and the resulting polymer morphology was investigated by atomic force microscopy. At higher concentrations, thin films formed with varying thicknesses; some dewetting was observed which depended on the molecular weight. Total dewetting did not occur despite the polymer's low glass transition temperature. Instead, partial dewetting was observed suggesting that the polymer was in a metastable equilibrium state. At lower concentrations, spherical cap shaped nanodroplets formed with varying sizes from single polymer chains to aggregates containing millions of chains. As the molecular weight was increased, fewer aggregates were observed on the surface, albeit with larger sizes resulting from increased solution viscosities and more chain entanglements at higher molecular weights. The contact angles of the nanodroplets were shown to be size dependent. A minimum contact angle occurs for droplets with radii of 100-250 nm at each molecular weight. Droplets smaller than 100 nm showed a sharp increase in contact angle; attributed to an increase in the elastic modulus of the droplets, in addition, to a positive line tension value. Droplets larger than 250 nm also showed an increased contact angle due to surface heterogeneities which cannot be avoided for larger droplets. This increase in contact angle plateaus as the droplet size reaches the macroscopic scale.
Chen, Wei-Tsung; Kang, Shih-Tsung; Lin, Jian-Liang; Wang, Chung-Hsin; Chen, Ran-Chou; Yeh, Chih-Kuang
2015-01-01
In this study, we aimed to validate the feasibility of receptor-targeted tumor theranostics with folate-conjugated (FA) and camptothecin-loaded (CPT) acoustic nanodroplets (NDs) (collectively termed FA-CPT-NDs). The ND formulation was based on lipid-stabilized low-boiling perfluorocarbon that can undergo acoustic droplet vaporization (ADV) under ultrasound (US) exposure. Conjugation of folate enhanced the selective delivery to tumors expressing high levels of folate receptor (FR) under mediation by the enhanced permeability and retention effect. In vitro and in vivo studies were performed using FR-positive KB and FR-negative HT-1080 cell lines and mouse xenograft tumor models. Simultaneous therapy and imaging were conducted with a clinical US imaging system at mechanical indices of up to 1.4 at a center frequency of 10 MHz. The results demonstrated that FA-CPT-NDs selectively attached to KB cells, but not HT-1080 cells. The targeted ADV caused instant and delayed damage via mechanical disruption and chemical toxicity to decrease the viability of KB cells by up to 45%, a much higher decrease than that achieved by the NDs without folate conjugation. The in vivo experiments showed that FR-mediated targeting successfully enhanced the EPR of FA-CPT-NDs in KB tumors mainly on the tumor periphery as indicated by immunofluorescence microscopy and US B-mode imaging. Treatments with FA-CPT-NDs at a CPT dose of 50 μg/kg inhibited the growth of KB tumors for up to six weeks, whereas treatment with NDs lacking folate produced a 4.6-fold increase in tumor volume. For HT-1080 tumors, neither the treatments with FA-CPT-NDs nor those with the NDs lacking folate presented tumor growth inhibition. In summary, FR-targeted tumor theranostics has been successfully implemented with FA-CPT-NDs and a clinical US unit. The ligand-directed and EPR-mediated accumulation provides active and passive targeting capabilities, permitting the antitumor effects of FA-CPT-NDs to be exerted
Zhang, Siyuan; Cui, Zhiwei; Xu, Tianqi; Liu, Pan; Li, Dapeng; Shang, Shaoqiang; Xu, Ranxiang; Zong, Yujin; Niu, Gang; Wang, Supin; He, Xijing; Wan, Mingxi
2017-01-01
This paper compared the effects of flowing phase-shift nanodroplets (NDs) and lipid-shelled microbubbles (MBs) on subsequent cavitation during focused ultrasound (FUS) exposures. The cavitation activity was monitored using a passive cavitation detection method as solutions of either phase-shift NDs or lipid-shelled MBs flowed at varying velocities through a 5-mm diameter wall-less vessel in a transparent tissue-mimicking phantom when exposed to FUS. The intensity of cavitation for the phase-shift NDs showed an upward trend with time and cavitation for the lipid-shelled MBs grew to a maximum at the outset of the FUS exposure followed by a trend of decreases when they were static in the vessel. Meanwhile, the increase of cavitation for the phase-shift NDs and decrease of cavitation for the lipid-shelled MBs had slowed down when they flowed through the vessel. During two discrete identical FUS exposures, while the normalized inertial cavitation dose (ICD) value for the lipid-shelled MB solution was higher than that for the saline in the first exposure (p-value 0.95). Meanwhile, the normalized ICD value for the phase-shift NDs was 0.182 at a flow velocity of 5cm/s and increased to 0.188 at a flow velocity of 15cm/s. As the flow velocity increased to 20cm/s, the normalized ICD was 0.185 and decreased to 0.178 at a flow velocity of 30cm/s. At high acoustic power, the normalized ICD values for both the lipid-shelled MBs and the phase-shift NDs increased with increasing flow velocities from 5 to 30cm/s (r>0.95). The effects of the flowing phase-shift NDs vaporized into gas bubbles as cavitation nuclei on the subsequent cavitation were inverse to those of the flowing lipid-shelled MBs destroyed after focused ultrasound exposures. Copyright © 2016 Elsevier B.V. All rights reserved.
International Nuclear Information System (INIS)
Basilico, Nicoletta; Magnetto, Chiara; D'Alessandro, Sarah; Panariti, Alice; Rivolta, Ilaria; Genova, Tullio; Khadjavi, Amina; Gulino, Giulia Rossana; Argenziano, Monica; Soster, Marco
2015-01-01
In chronic wounds, hypoxia seriously undermines tissue repair processes by altering the balances between pro-angiogenic proteolytic enzymes (matrix metalloproteinases, MMPs) and their inhibitors (tissue inhibitors of metalloproteinases, TIMPs) released from surrounding cells. Recently, we have shown that in human monocytes hypoxia reduces MMP-9 and increases TIMP-1 without affecting TIMP-2 secretion, whereas in human keratinocytes it reduces MMP-2, MMP-9, and TIMP-2, without affecting TIMP-1 release. Provided that the phenotype of the cellular environment is better understood, chronic wounds might be targeted by new oxygenating compounds such as chitosan- or dextran-shelled and 2H,3H-decafluoropentane-cored oxygen-loaded nanodroplets (OLNs). Here, we investigated the effects of hypoxia and dextran-shelled OLNs on the pro-angiogenic phenotype and behavior of human dermal microvascular endothelium (HMEC-1 cell line), another cell population playing key roles during wound healing. Normoxic HMEC-1 constitutively released MMP-2, TIMP-1 and TIMP-2 proteins, but not MMP-9. Hypoxia enhanced MMP-2 and reduced TIMP-1 secretion, without affecting TIMP-2 levels, and compromised cell ability to migrate and invade the extracellular matrix. When taken up by HMEC-1, nontoxic OLNs abrogated the effects of hypoxia, restoring normoxic MMP/TIMP levels and promoting cell migration, matrix invasion, and formation of microvessels. These effects were specifically dependent on time-sustained oxygen diffusion from OLN core, since they were not achieved by oxygen-free nanodroplets or oxygen-saturated solution. Collectively, these data provide new information on the effects of hypoxia on dermal endothelium and support the hypothesis that OLNs might be used as effective adjuvant tools to promote chronic wound healing processes. - Highlights: • Hypoxia enhances MMP-2 and reduces TIMP-1 secretion by dermal HMEC-1 cell line. • Hypoxia compromises migration and matrix invasion abilities of
Energy Technology Data Exchange (ETDEWEB)
Basilico, Nicoletta, E-mail: nicoletta.basilico@unimi.it [Dipartimento di Scienze Biomediche, Chirurgiche e Odontoiatriche, Università di Milano, via Pascal 36, 20133 Milano (Italy); Magnetto, Chiara, E-mail: c.magnetto@inrim.it [Istituto Nazionale di Ricerca Metrologica (INRIM), Strada delle Cacce, 91, 10135 Torino (Italy); D' Alessandro, Sarah, E-mail: sarah.dalessandro@unimi.it [Dipartimento di Scienze Farmacologiche e Biomolecolari, Università di Milano, via Pascal 36, 20133 Milano (Italy); Panariti, Alice, E-mail: alice.panariti@mail.mcgill.ca [Dipartimento di Scienze della Salute, Università di Milano Bicocca, Via Cadore 48, 20900 Monza (Italy); Rivolta, Ilaria, E-mail: ilaria.rivolta@unimib.it [Dipartimento di Scienze della Salute, Università di Milano Bicocca, Via Cadore 48, 20900 Monza (Italy); Genova, Tullio, E-mail: tullio.genova@unito.it [Dipartimento di Scienze della Vita e Biologia dei Sistemi, Via Accademia Albertina 13, 10123 Torino (Italy); Khadjavi, Amina, E-mail: amina.khadjavi@unito.it [Dipartimento di Neuroscienze, Università di Torino, Corso Raffaello 30, 10125 Torino (Italy); Gulino, Giulia Rossana, E-mail: giuliarossana.gulino@unito.it [Dipartimento di Oncologia, Università di Torino, Via Santena 5 bis, 10126 Torino (Italy); Argenziano, Monica, E-mail: monica.argenziano@unito.it [Dipartimento di Scienza e Tecnologia del Farmaco, Università di Torino, Via Giuria, 9, 10125 Torino (Italy); Soster, Marco, E-mail: marco.soster@unito.it [Dipartimento di Scienza e Tecnologia del Farmaco, Università di Torino, Via Giuria, 9, 10125 Torino (Italy); and others
2015-11-01
In chronic wounds, hypoxia seriously undermines tissue repair processes by altering the balances between pro-angiogenic proteolytic enzymes (matrix metalloproteinases, MMPs) and their inhibitors (tissue inhibitors of metalloproteinases, TIMPs) released from surrounding cells. Recently, we have shown that in human monocytes hypoxia reduces MMP-9 and increases TIMP-1 without affecting TIMP-2 secretion, whereas in human keratinocytes it reduces MMP-2, MMP-9, and TIMP-2, without affecting TIMP-1 release. Provided that the phenotype of the cellular environment is better understood, chronic wounds might be targeted by new oxygenating compounds such as chitosan- or dextran-shelled and 2H,3H-decafluoropentane-cored oxygen-loaded nanodroplets (OLNs). Here, we investigated the effects of hypoxia and dextran-shelled OLNs on the pro-angiogenic phenotype and behavior of human dermal microvascular endothelium (HMEC-1 cell line), another cell population playing key roles during wound healing. Normoxic HMEC-1 constitutively released MMP-2, TIMP-1 and TIMP-2 proteins, but not MMP-9. Hypoxia enhanced MMP-2 and reduced TIMP-1 secretion, without affecting TIMP-2 levels, and compromised cell ability to migrate and invade the extracellular matrix. When taken up by HMEC-1, nontoxic OLNs abrogated the effects of hypoxia, restoring normoxic MMP/TIMP levels and promoting cell migration, matrix invasion, and formation of microvessels. These effects were specifically dependent on time-sustained oxygen diffusion from OLN core, since they were not achieved by oxygen-free nanodroplets or oxygen-saturated solution. Collectively, these data provide new information on the effects of hypoxia on dermal endothelium and support the hypothesis that OLNs might be used as effective adjuvant tools to promote chronic wound healing processes. - Highlights: • Hypoxia enhances MMP-2 and reduces TIMP-1 secretion by dermal HMEC-1 cell line. • Hypoxia compromises migration and matrix invasion abilities of
Energy Technology Data Exchange (ETDEWEB)
Droppelmann, G.
2005-09-15
In the framework of this thesis several aspects of the properties of helium nanodroplets and their dopings. The formation of the exciplexes RbHe and KHe on helium droplets was studied by means of pump-probe ionization in real time, whereby the main interest lied on the influence of the applied helium isotopes. The experiments with cesium atoms on the droplet surface aimed on the elucidation of the relaxation dynamics of the surface under regardment both of isotope and size effects. From the pump-probe measurements on the formation of the exciplex RbHe on helium nanodroplets performed in the framework of this thesis formation times of 8.5 ps for Rb{sup 4}He and 11.6 ps for Rb{sup 3}He resulted.
Zhang, Siyuan; Cui, Zhiwei; Li, Chong; Zhou, Fanyu; Zong, Yujin; Wang, Supin; Wan, Mingxi
2017-03-01
Cavitation and heating are the primary mechanisms of numerous therapeutic applications of ultrasound. Various encapsulated microbubbles (MBs) and phase-shift nanodroplets (NDs) have been used to enhance local cavitation and heating, creating interests in developing ultrasound therapy using these encapsulated MBs and NDs. This work compared the efficiency of flowing polymer- and lipid-shelled MBs and phase-shift NDs in cavitation and heating during focused ultrasound (FUS) exposures. Cavitation activity and temperature were investigated when the solution of polymer- and lipid-shelled MBs and NDs flowed through the vessel in a tissue-mimicking phantom with varying flow velocities when exposed to FUS at various acoustic power levels. The inertial cavitation dose (ICD) for the encapsulated MBs and NDs were higher than those for the saline. Temperature initially increased with increasing flow velocities of the encapsulated MBs, followed by a decrease of the temperature with increasing flow velocities when the velocity was much higher. Meanwhile, ICD showed a trend of increases with increasing flow velocity. For the phase-shift NDs, ICD after the first FUS exposure was lower than those after the second FUS exposure. For the encapsulated MBs, ICD after the first FUS exposure was higher than those after the second FUS exposure. Further studies are necessary to investigate the treatment efficiency of different encapsulated MBs and phase-shift NDs in cavitation and heating.
Zhu, Chongqin; Gao, Yurui; Li, Hui; Meng, Sheng; Li, Lei; Francisco, Joseph S; Zeng, Xiao Cheng
2016-11-15
Hydrophobicity of macroscopic planar surface is conventionally characterized by the contact angle of water droplets. However, this engineering measurement cannot be directly extended to surfaces of proteins, due to the nanometer scale of amino acids and inherent nonplanar structures. To measure the hydrophobicity of side chains of proteins quantitatively, numerous parameters were developed to characterize behavior of hydrophobic solvation. However, consistency among these parameters is not always apparent. Herein, we demonstrate an alternative way of characterizing hydrophobicity of amino acid side chains in a protein environment by constructing a monolayer of amino acids (i.e., artificial planar peptide network) according to the primary and the β-sheet secondary structures of protein so that the conventional engineering measurement of the contact angle of a water droplet can be brought to bear. Using molecular dynamics simulations, contact angles θ of a water nanodroplet on the planar peptide network, together with excess chemical potentials of purely repulsive methane-sized Weeks-Chandler-Andersen solute, are computed. All of the 20 types of amino acids and the corresponding planar peptide networks are studied. Expectedly, all of the planar peptide networks with nonpolar amino acids are hydrophobic due to θ [Formula: see text] 90°, whereas all of the planar peptide networks of the polar and charged amino acids are hydrophilic due to θ [Formula: see text] 90°. Planar peptide networks of the charged amino acids exhibit complete-wetting behavior due to θ [Formula: see text] 0°. This computational approach for characterization of hydrophobicity can be extended to artificial planar networks of other soft matter.
de Lara-Castells, María Pilar; Stoll, Hermann; Civalleri, Bartolomeo; Causà, Mauro; Voloshina, Elena; Mitrushchenkov, Alexander O; Pi, Martí
2014-10-21
In this work we propose a general strategy to calculate accurate He-surface interaction potentials. It extends the dispersionless density functional approach recently developed by Pernal et al. [Phys. Rev. Lett. 103, 263201 (2009)] to adsorbate-surface interactions by including periodic boundary conditions. We also introduce a scheme to parametrize the dispersion interaction by calculating two- and three-body dispersion terms at coupled cluster singles and doubles and perturbative triples (CCSD(T)) level via the method of increments [H. Stoll, J. Chem. Phys. 97, 8449 (1992)]. The performance of the composite approach is tested on (4)He/graphene by determining the energies of the low-lying selective adsorption states, finding an excellent agreement with the best available theoretical data. Second, the capability of the approach to describe dispersionless correlation effects realistically is used to extract dispersion effects in time-dependent density functional simulations on the collision of (4)He droplets with a single graphene sheet. It is found that dispersion effects play a key role in the fast spreading of the (4)He nanodroplet, the evaporation-like process of helium atoms, and the formation of solid-like helium structures. These characteristics are expected to be quite general and highly relevant to explain experimental measurements with the newly developed helium droplet mediated deposition technique.
Energy Technology Data Exchange (ETDEWEB)
Lara-Castells, María Pilar de, E-mail: Pilar.deLara.Castells@csic.es [Instituto de Física Fundamental (C.S.I.C.), Serrano 123, E-28006 Madrid (Spain); Stoll, Hermann [Institut für Theoretische Chemie, Universität Stuttgart, D-70550 Stuttgart (Germany); Civalleri, Bartolomeo [Dipartimento di Chimica e Centro Interdipartimentale NIS, Universitá di Torino, Via P. Giuria 7, 10125 Torino (Italy); Causà, Mauro [Dipartimento di Ingegneria Chimica, dei Materiali e delle Produzioni Industriali, Universiá di Napoli Federico II, Piazzale Tecchio, 80126 Napoli (Italy); Voloshina, Elena [Humboldt-Universität zu Berlin, Institut für Chemie, Brook-Taylor-Str. 2, 12489 Berlin (Germany); Mitrushchenkov, Alexander O. [Université Paris-Est, Laboratoire Modélisation et Simulation Multi Echelle, MSME UMR 8208 CNRS, 5 bd Descartes, 77454 Marne-la-Vallée (France); Pi, Martí [Department ECM, Facultat de Física, and IN" 2UB, Universitat de Barcelona, Diagonal 645, E-08028 Barcelona (Spain)
2014-10-21
In this work we propose a general strategy to calculate accurate He–surface interaction potentials. It extends the dispersionless density functional approach recently developed by Pernal et al. [Phys. Rev. Lett. 103, 263201 (2009)] to adsorbate-surface interactions by including periodic boundary conditions. We also introduce a scheme to parametrize the dispersion interaction by calculating two- and three-body dispersion terms at coupled cluster singles and doubles and perturbative triples (CCSD(T)) level via the method of increments [H. Stoll, J. Chem. Phys. 97, 8449 (1992)]. The performance of the composite approach is tested on {sup 4}He/graphene by determining the energies of the low-lying selective adsorption states, finding an excellent agreement with the best available theoretical data. Second, the capability of the approach to describe dispersionless correlation effects realistically is used to extract dispersion effects in time-dependent density functional simulations on the collision of {sup 4}He droplets with a single graphene sheet. It is found that dispersion effects play a key role in the fast spreading of the {sup 4}He nanodroplet, the evaporation-like process of helium atoms, and the formation of solid-like helium structures. These characteristics are expected to be quite general and highly relevant to explain experimental measurements with the newly developed helium droplet mediated deposition technique.
Alternative Hamiltonian for molecular dynamics simulations in the grand canonical ensemble
International Nuclear Information System (INIS)
Lo, C.; Palmer, B.
1995-01-01
An alternative to the Hamiltonian of Cagin and Pettitt for performing molecular dynamics simulations in the grand canonical ensemble is presented and used as the basis for a new algorithm. The algorithm is tested on the ideal gas and the truncated and shifted Lennard-Jones fluid. Simulations are used to calculate the vapor--liquid coexistence points for the Lennard-Jones system and are found to be in agreement with previous calculations using Gibbs ensemble calculations and with the Nicolas equation of state. Simulations are also performed on the Lennard-Jones solid
Adhesive contact: from atomistic model to continuum model
International Nuclear Information System (INIS)
Fan Kang-Qi; Jia Jian-Yuan; Zhu Ying-Min; Zhang Xiu-Yan
2011-01-01
Two types of Lennard-Jones potential are widely used in modeling adhesive contacts. However, the relationships between the parameters of the two types of Lennard-Jones potential are not well defined. This paper employs a self-consistent method to derive the Lennard-Jones surface force law from the interatomic Lennard-Jones potential with emphasis on the relationships between the parameters. The effect of using correct parameters in the adhesion models is demonstrated in single sphere-flat contact via continuum models and an atomistic model. Furthermore, the adhesion hysteresis behaviour is investigated, and the S-shaped force-distance relation is revealed by the atomistic model. It shows that the adhesion hysteresis loop is generated by the jump-to-contact and jump-off-contact, which are illustrated by the S-shaped force-distance curve. (atomic and molecular physics)
A free energy study of the liquid-liquid phase transition of the Jagla ...
Indian Academy of Sciences (India)
Appendix” preliminary free energy surface calculations for select parameterizations of the generalized family of Jagla potentials spanning from the original (anomalous,water-like) Jagla model to the Lennard-Jones model. These calculations ...
Diffusion processes and memory effects
International Nuclear Information System (INIS)
Mokshin, Anatolii V; Yulmetyev, Renat M; Haenggi, Peter
2005-01-01
We report the results of the numerical estimation of statistical memory effects in diffusion for two various systems: Lennard-Jones fluids and the model of the Brownian particle in a one-dimensional harmonic lattice. We have found the relation between the diffusion coefficient and the non-Markovity parameter, which is linear for the Lennard-Jones systems in liquid state. The relation between the memory measure and the excess entropy is also discussed here
Addendum to ''Density fluctuations in liquid rubidium''
International Nuclear Information System (INIS)
Haan, S.W.; Mountain, R.D.; Hsu, C.S.; Rahman, A.
1980-01-01
We performed molecular-dynamics simulations of liquid rubidium and the Lennard-Jones fluid at several densities and temperatures, and of a system whose pair potential is the repulsive core of the rubidium potential. In all cases, propagating density fluctuations occurred in the rubidiumlike systems at much shorter wavelengths than in the Lennard-Jones system. This indicates that the repulsive part of the pair potential is the dominant factor in determining the relaxation of short-wavelength density fluctuations
Method and Apparatus for Forming Nanodroplets
Ackley, Donald; Forster, Anita
2011-01-01
This innovation uses partially miscible fluids to form nano- and microdroplets in a microfluidic droplet generator system. Droplet generators fabricated in PDMS (polydimethylsiloxane) are currently being used to fabricate engineered nanoparticles and microparticles. These droplet generators were first demonstrated in a T-junction configuration, followed by a cross-flow configuration. All of these generating devices have used immiscible fluids, such as oil and water. This immiscible fluid system can produce mono-dispersed distributions of droplets and articles with sizes ranging from a few hundred nanometers to a few hundred microns. For applications such as drug delivery, the ability to encapsulate aqueous solutions of drugs within particles formed from the droplets is desirable. Of particular interest are non-polar solvents that can dissolve lipids for the formation of liposomes in the droplet generators. Such fluids include ether, cyclohexane, butanol, and ethyl acetate. Ethyl acetate is of particular interest for two reasons. It is relatively nontoxic and it is formed from ether and acetic acid, and maybe broken down into its constituents at relatively low concentrations.
Biomolecular ions in superfluid helium nanodroplets
International Nuclear Information System (INIS)
Gonzalez Florez, Ana Isabel
2016-01-01
The function of a biological molecule is closely related to its structure. As a result, understanding and predicting biomolecular structure has become the focus of an extensive field of research. However, the investigation of molecular structure can be hampered by two main difficulties: the inherent complications that may arise from studying biological molecules in their native environment, and the potential congestion of the experimental results as a consequence of the large number of degrees of freedom present in these molecules. In this work, a new experimental setup has been developed and established in order to overcome the afore mentioned limitations combining structure-sensitive gas-phase methods with superfluid helium droplets. First, biological molecules are ionised and brought into the gas phase, often referred to as a clean-room environment, where the species of interest are isolated from their surroundings and, thus, intermolecular interactions are absent. The mass-to-charge selected biomolecules are then embedded inside clusters of superfluid helium with an equilibrium temperature of ∝0.37 K. As a result, the internal energy of the molecules is lowered, thereby reducing the number of populated quantum states. Finally, the local hydrogen bonding patterns of the molecules are investigated by probing specific vibrational modes using the Fritz Haber Institute's free electron laser as a source of infrared radiation. Although the structure of a wide variety of molecules has been studied making use of the sub-Kelvin environment provided by superfluid helium droplets, the suitability of this method for the investigation of biological molecular ions was still unclear. However, the experimental results presented in this thesis demonstrate the applicability of this experimental approach in order to study the structure of intact, large biomolecular ions and the first vibrational spectrum of the protonated pentapeptide leu-enkephalin embedded in helium droplets has been recorded. The experimental results show well resolved spectra, which are in good agreement with theoretical calculations. Moreover, the weakly interacting nature of helium droplets is confirmed by the excellent agreement obtained with the available gas-phase data. Using standard gas-phase mass spectrometry techniques allows to study the molecular ions as a function of charge state. As a result, the role of the interplay between Coulomb repulsion and hydrogen bonding in the secondary structure of the target molecules can be investigated. For this purpose, the infrared spectra of the proteins ubiquitin and cytochrome c embedded in helium droplets were recorded. The experimental results are interpreted in terms of a charge induced unzipping of the proteins, where a structural transition from helical into extended C 5 -type hydrogen bonded structures occurs. This interpretation is supported by simple energy considerations, as well as by quantum chemical calculations on model peptides. The transition in secondary structure observed here is most likely universal for isolated proteins in the gas phase. Embedding positively charged ions inside helium droplets also offers the possibility to directly investigate the intrinsic properties of helium droplets. One fundamental characteristic of helium droplets is their unique ability to pick up the species with which they collide. In order to gain more insight into this process, the presence of an electrical charge was used to accelerate and detect the ion-doped droplets as a function of the mass and size of the dopant. A systematic investigation of the pick-up probability demonstrates the existence of a dopant dependent minimum droplet size below which no pick-up occurs. As a result, different hypotheses and theoretical models are proposed and discussed in order to shed more light into the constraints and limitations of the pick-up process.
Acoustic Studies on Nanodroplets, Microbubbles and Liposomes
Kumar, Krishna Nandan
Microbubbles and droplets are nanometer to micron size biocompatible particles which are primarily used for drug delivery and contrast imaging. Our aim is to broaden the use of microbubbles from contrast imaging to other applications such as measuring blood pressure. The other goal is to develop in situ contrast agents (phase shift droplets) which can be used for applications such as cancer tumor imaging. Therefore, the focus is on developing and validating the concept using experimental and theoretical methods. Below is an overview of each of the projects performed on droplets and microbubbles. Phase shift droplets vaporizable by acoustic stimulation offer many advantages over microbubbles as contrast agents due to their higher stability and possibility of smaller sizes. In this study, the acoustic droplet vaporization (ADV) threshold of a suspension of PFP droplets (400-3000nm) was acoustically measured as a function of the excitation frequency by examining the scattered signals, fundamental, sub- and second-harmonic. This work presents the experimental methodology to determine ADV threshold. The threshold increases with frequency: 1.25 MPa at 2.25 MHz, 2.0 MPa at 5 MHz and 2.5 MPa at 10 MHz. The scattered response from droplets was also found to match well with that of independently prepared lipid-coated microbubble suspension in magnitude as well as trends above the threshold value. Additionally, we have employed classical nucleation theory (CNT) to investigate the ADV, specifically the threshold value of the peak negative pressure required for vaporization. The theoretical analysis predicts that the ADV threshold increases with increasing surface tension of the droplet core and frequency of excitation, while it decreases with increasing temperature and droplet size. The predictions are in qualitative agreement with experimental observations. A technique to measure the ambient pressure using microbubbles was developed. Here we are presenting the results of an in vitro study aimed at developing an ultrasound-aided noninvasive pressure estimation technique using contrast agents-DefinityRTM, a lipid coated microbubble, and an experimental PLA (Poly lactic acid) microbubbles. Scattered responses from these bubbles have been measured in vitro as a function of ambient pressure using a 3.5 MHz acoustic excitation of varying amplitude. At an acoustic pressure of 670 kPa, Definity RTM microbubbles showed a linear decrease in subharmonic signal with increasing ambient pressure, registering a 12dB reduction at an overpressure of 120 mm Hg. Ultrasound contrast microbubbles experience widely varying ambient blood pressure in different organs, which can also change due to diseases. Pressure change can alter the material properties of the encapsulation of these microbubbles. Here the characteristic rheological parameters of contrast agent Definity and Targestar are determined by varying the ambient pressure (in a physiologically relevant range 0-200 mmHg). Four different interfacial rheological models are used to characterize the microbubbles. Both the contrast agents show an increase in their interfacial dilatational viscosity and interfacial dilatational elasticity with ambient pressure. It has been well established that liposomes prepared following a careful multi-step procedure can be made echogenic. Our group as well as others experimentally demonstrated that freeze-drying in the presence of mannitol is a crucial component to ensure echogenicity. Here, we showed that freeze-dried aqueous solutions of excipients such as mannitol, meso-erythritol, glycine, and glucose that assume a crystalline state, when dispersed in water creates bubbles and are echogenic even without any lipids. We also present an explanation for the bubble generation process because of dissolution of mannitol.
Surface Impact Simulations of Helium Nanodroplets
2015-06-30
distorted hcp-like cages at three different target densities: 22.6 nm−3, 27.8 nm−3, and 34.8 nm−3. These densities are respectively 3%, 28%, and 59% higher...M. Lindsay, J. Phys. Chem. C 117, 2358 (2013). [9] A. Boatwright, C. Feng, D. Spence, E. Latimer, C. Binns, A. M. Ellis, and S. Yang, Faraday Discuss...displacement u2 (bohr2) Fig. 3: Probability distributions for the mean squared displacement 〈u2〉 for He atoms in distorted hcp-like cages . The en- semble of
Biomolecular ions in superfluid helium nanodroplets
Energy Technology Data Exchange (ETDEWEB)
Gonzalez Florez, Ana Isabel
2016-07-01
The function of a biological molecule is closely related to its structure. As a result, understanding and predicting biomolecular structure has become the focus of an extensive field of research. However, the investigation of molecular structure can be hampered by two main difficulties: the inherent complications that may arise from studying biological molecules in their native environment, and the potential congestion of the experimental results as a consequence of the large number of degrees of freedom present in these molecules. In this work, a new experimental setup has been developed and established in order to overcome the afore mentioned limitations combining structure-sensitive gas-phase methods with superfluid helium droplets. First, biological molecules are ionised and brought into the gas phase, often referred to as a clean-room environment, where the species of interest are isolated from their surroundings and, thus, intermolecular interactions are absent. The mass-to-charge selected biomolecules are then embedded inside clusters of superfluid helium with an equilibrium temperature of ∝0.37 K. As a result, the internal energy of the molecules is lowered, thereby reducing the number of populated quantum states. Finally, the local hydrogen bonding patterns of the molecules are investigated by probing specific vibrational modes using the Fritz Haber Institute's free electron laser as a source of infrared radiation. Although the structure of a wide variety of molecules has been studied making use of the sub-Kelvin environment provided by superfluid helium droplets, the suitability of this method for the investigation of biological molecular ions was still unclear. However, the experimental results presented in this thesis demonstrate the applicability of this experimental approach in order to study the structure of intact, large biomolecular ions and the first vibrational spectrum of the protonated pentapeptide leu-enkephalin embedded in helium droplets has been recorded. The experimental results show well resolved spectra, which are in good agreement with theoretical calculations. Moreover, the weakly interacting nature of helium droplets is confirmed by the excellent agreement obtained with the available gas-phase data. Using standard gas-phase mass spectrometry techniques allows to study the molecular ions as a function of charge state. As a result, the role of the interplay between Coulomb repulsion and hydrogen bonding in the secondary structure of the target molecules can be investigated. For this purpose, the infrared spectra of the proteins ubiquitin and cytochrome c embedded in helium droplets were recorded. The experimental results are interpreted in terms of a charge induced unzipping of the proteins, where a structural transition from helical into extended C{sub 5}-type hydrogen bonded structures occurs. This interpretation is supported by simple energy considerations, as well as by quantum chemical calculations on model peptides. The transition in secondary structure observed here is most likely universal for isolated proteins in the gas phase. Embedding positively charged ions inside helium droplets also offers the possibility to directly investigate the intrinsic properties of helium droplets. One fundamental characteristic of helium droplets is their unique ability to pick up the species with which they collide. In order to gain more insight into this process, the presence of an electrical charge was used to accelerate and detect the ion-doped droplets as a function of the mass and size of the dopant. A systematic investigation of the pick-up probability demonstrates the existence of a dopant dependent minimum droplet size below which no pick-up occurs. As a result, different hypotheses and theoretical models are proposed and discussed in order to shed more light into the constraints and limitations of the pick-up process.
Critical Landau Velocity in Helium Nanodroplets
Brauer, N.B.; Smolarek, S.; Loginov, E.; Mateo, D.; Hernando, A.; Pi, M.; Barranco, M.; Buma, W.J.; Drabbels, M.
2013-01-01
The best-known property of superfluid helium is the vanishing viscosity that objects experience while moving through the liquid with speeds below the so-called critical Landau velocity. This critical velocity is generally considered a macroscopic property as it is related to the collective
Interatomic Coulombic decay in helium nanodroplets
DEFF Research Database (Denmark)
Shcherbinin, Mykola; Laforge, Aaron; Sharma, Vandana
2017-01-01
, or in the droplet interior. ICD at the surface gives rise to energetic He+ ions as previously observed for free He dimers. ICD deeper inside leads to the ejection of slow He+ ions due to Coulomb explosion delayed by elastic collisions with neighboring He atoms, and to the formation of Hek+ complexes....
ÜRO säästva arengu eesmärgid aastaks 2030 / Meelis Joost
Joost, Meelis
2016-01-01
ÜRO liikmesriikide juhid leppisid 25.‒27. septembril 2015 New Yorgis kokku säästva arengu eesmärkides, mis tuleb saavutada 2030. aastaks. Säästva arengu eesmärgid on kaudselt seotud ka puuetega inimestega. Eesti Puuetega Inimeste Koda huvitab, kuivõrd ligipääsetavus, puuetega inimeste elukvaliteet, kasvav kaasatus ühiskonda ning puuetega inimestele osutatavate sotsiaalteenuste kvaliteet leiab kajastamist säästva arengu tegevuskava elluviimises
Gurjanova, Ilona, 1958-
2016-01-01
Intervjuu Design Management OÜ disaineri ja juhataja, Eesti Disainerite Liidu esimehe, Eesti Disaini Maja endise juhi ja Disainiöö peakorraldaja Ilona Gurjanovaga universaalsest disainist ja selle näidetest
Dynamical phases of attractive particles sliding on a structured surface
International Nuclear Information System (INIS)
Hasnain, J; Jungblut, S; Dellago, C
2015-01-01
Inspired by experiments on quartz crystal microbalance setups, we study the mobility of a monolayer of Lennard-Jones particles driven over a hexagonal external potential. We pay special attention to the changes in the dynamical phases that arise when the lattice constant of the external substrate potential and the Lennard-Jones interaction are mismatched. We find that if the average particle separation is such that the particles repel each other, or interact harmonically, the qualitative behavior of the system is akin to that of a monolayer of purely repulsive Yukawa particles. On the other hand, if the particles typically attract each other, the ensuing dynamical states are determined entirely by the relative strength of the Lennard-Jones interaction with respect to that of the external potential. (paper)
Low pressure broadening and shift of the 540.06 nm line of neon
International Nuclear Information System (INIS)
Bielski, A.; Dokurno, W.; Szudy, J.; Wolnikowski, J.
1980-01-01
The collision broadening and shift of the 540.06 nm line of neon emitted from a low pressure glow discharge in pure neon and a neon-helium mixture have been measured. The values of the broadening and shift coefficients were determined and compared with the results of calculations based on the Lindholm-Foley impact theory assuming a Lennard-Jones potential. The results for pure neon demonstrate the inadequacy of the Lennard-Jones potential for the Ne-Ne interaction. (orig.)
International Nuclear Information System (INIS)
Palmer, B.J.
1994-01-01
A method to calculate the thermal diffusivity D T from spontaneous fluctuations in the local heat energy density is presented. Calculations of the thermal diffusivity are performed for the Lennard-Jones fluid, carbon dioxide, and water. The results for the Lennard-Jones fluid are in agreement with calculations of the thermal conductivity using Green-Kubo relations and nonequilibrium molecular-dynamics techniques. The results for carbon dioxide and water give thermal diffusivities within a factor of 2 of the experimental values
1981-07-01
inverted by the first, i.e., at the moment of time t = T, such that i = (2n+)lT, where 0 is the Rabi frequency (Oraevski et al., 1976). . classical... anisotropic molecule present. CW HeNe, Ar+ and Kr+ lasers are used, and the filter method is necessary because of time-scales lo8 - 10ll Hz. Some general...e.g., truncated harmonic oscillator, square well, spherically symmetric Morse or Lennard-Jones, anisotropic (angle-dependent) Morse or Lennard-Jones
Equation of state of a hard core fluid with a two-Yukawa tail: toward a simple analytic theory
International Nuclear Information System (INIS)
Jedrzejek, C.
1980-01-01
Thermodynamic properties of simple fluids are calculated using variational theory for a system of hard-core potential with a two-Yukawa tail. Likewise one Yukawa-tail case the working formulas are analytic. Five parameters of the two Yukawa system are chosen so as to get the best fit to a real argon potential or an ''argon-like'' Lennard-Jones potential. The results are fairly good in light of the extreme simplicity of the method. The discrepancies result from using the variational method and a different shape of Yukawa type potential in comparision to the real argon and Lennard-Jones potentials. (author)
Atomic and Molecular Dynamics on and in Superfluid Helium Nanodroplets
Lehmann, Kevin K.
2003-03-01
Studies of intramolecular and intermolecular dynamics is at the core of Molecular Spectroscopic research several decades. Gas phase, particularly molecular beam, studies have greatly illuminated these processes in isolated molecules, bimolecular collisions, or small covalent and van der Waals complexes. Parallel to this effort have been studies in condensed phases, but there has unfortunately been little intellectual contact between these. The recent development of Helium Nanodropet Isolation Spectroscopy is providing an intellectual bridge between gas phase and condensed phase spectroscopy. While droplets of 10,000 He atoms are effectively a condensed phase, their low temperature ( 0.4 K) and ultralow heat capacities combined with their superfluid state make them an almost ideal matrix in which to study both molecular dynamics, including solute induced relaxations. The nsec times scales for many of the relaxation events, orders of magnitude slower than in classical liquids, results in spectra with unprecedented resolution for the liquid state. In this talk, studies of the Princeton group will be highlighted, with particular emphasis on those for which a combination of theory and experiment have combined to reveal dynamics in this unique Quantum Fluid.
Ordered alternating binary polymer nanodroplet array by sequential spin dewetting.
Bhandaru, Nandini; Das, Anuja; Salunke, Namrata; Mukherjee, Rabibrata
2014-12-10
We report a facile technique for fabricating an ordered array of nearly equal-sized mesoscale polymer droplets of two constituent polymers (polystyrene, PS and poly(methyl methacrylate), PMMA) arranged in an alternating manner on a topographically patterned substrate. The self-organized array of binary polymers is realized by sequential spin dewetting. First, a dilute solution of PMMA is spin-dewetted on a patterned substrate, resulting in an array of isolated PMMA droplets arranged along the substrate grooves due to self-organization during spin coating itself. The sample is then silanized with octadecyltrichlorosilane (OTS), and subsequently, a dilute solution of PS is spin-coated on to it, which also undergoes spin dewetting. The spin-dewetted PS drops having a size nearly equal to the pre-existing PMMA droplets position themselves between two adjacent PMMA drops under appropriate conditions, forming an alternating binary polymer droplet array. The alternating array formation takes place for a narrow range of solution concentration for both the polymers and depends on the geometry of the substrate. The size of the droplets depends on the extent of confinement, and droplets as small as 100 nm can be obtained by this method, on a suitable template. The findings open up the possibility of creating novel surfaces having ordered multimaterial domains with a potential multifunctional capability.
Femtosecond vibrational dynamics in water nano-droplets
Cringus, Gheorghe Dan
2008-01-01
Water is probably the most researched substance on Earth. The interest in water, and redominantly in liquid water, is due to its importance on both macro- and microscopic scales. Although people have been trying to understand water for centuries, this ubiquitous liquid is still surrounded by mystery
Molecular Dynamics Simulations of Water Nanodroplets on Silica Surfaces
DEFF Research Database (Denmark)
Zambrano, Harvey A; Walther, Jens Honore; Jaffe, Richard L.
2009-01-01
and DNA microarrays technologies.4,5,6,7,8 Although extensive experimental, theoretical and computational work has been devoted to study the nature of the interaction between silica and water,2,9-16 at the molecular level a complete understanding of silica-water systems has not been reached. Contact angle...... computations of water droplets on silica surfaces offers a useful fundamental and quantitative measurement in order to study chemical and physical properties of water-silica systems.3,16,17,18 For hydrophobic systems the static and dynamic properties of the fluid-solid interface are influenced by the presence...
Van der Waals Attraction and Coalescence of Aqueous Salt Nanodroplets
Czech Academy of Sciences Publication Activity Database
Jungwirth, Pavel; Buch, V.
2003-01-01
Roč. 68, č. 12 (2003), s. 2283-2291 ISSN 0010-0765 R&D Projects: GA MŠk LN00A032 Institutional research plan: CEZ:AV0Z4040901 Keywords : van der Waals interactions * aqueous droplets * coalescence Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 1.041, year: 2003
International Nuclear Information System (INIS)
Bickes, R.W. Jr.; Scoles, G.; Smith, K.M.
1974-01-01
Differential elastic scattering cross sections with well resolved quantum oscillations have been measuremed for the systems H 2 +NH 3 and H 2 +H 2 O. Assuming a spherically symmetric interaction the data show that a simple spherical potential (i.e. Lennard-Jones) does not properly describe the scattering
Contact angle dependence on the fluid-wall dispersive energy
Horsch, M.; Heitzig, M.; Dan, C.M.; Harting, J.D.R.; Hasse, H.; Vrabec, J.
2010-01-01
Menisci of the truncated and shifted Lennard-Jones fluid between parallel planar walls are investigated by molecular dynamics simulation. Thereby, the characteristic energy of the unlike dispersive interaction between fluid molecules and wall atoms is systematically varied to determine its influence
Elastic properties of surfactant monolayers at liquid-liquid interfaces: A molecular dynamics study
DEFF Research Database (Denmark)
Laradji, Mohamed; Mouritsen, Ole G.
2000-01-01
Using a simple molecular model based on the Lennard-Jones potential, we systematically study the elastic properties of liquid-liquid interfaces containing surfactant molecules by means of extensive and large-scale molecular dynamics simulations. The main elastic constants of the interface, corres...
Some aspects of equations of state
International Nuclear Information System (INIS)
Frisch, H.L.
1979-02-01
Some elementary properties of the equation of state of molecules repulsing each other as point centers of force are developed briefly. An inequality for the Lennard--Jones gas is presented. The scaled particle theory equation of state of hard spheres is also reviewed briefly. Means of possibly applying these concepts to represent thermodynamic data on model detonating gases are suggested
DEFF Research Database (Denmark)
Toxværd, Søren; Dyre, J. C.
2011-01-01
. Lett. 103, 170601 (2009);10.1103/PhysRevLett.103.170601 J. Chem. Phys. 134, 214503 (2011)10.1063/1.3592709] . We present simulations of the standard Lennard-Jones liquid at several condensed-fluid state points, including a fairly low density state and a very high density state, as well as simulations...
Switching Between the NVT and NpT Ensembles Using the Reweighting and Reconstruction Scheme
Kadoura, Ahmad Salim; Salama, Amgad; Sun, Shuyu
2015-01-01
thermodynamic conditions from a single MC Markov chain. The latter scheme, was first developed to extrapolate quantities in NV T ensemble for struc- tureless Lennard-Jones particles. However, it is evident that for most real life applications the NpT ensemble
Validity of the Rosenfeld relationship: A comparative study of the ...
Indian Academy of Sciences (India)
ATREYEE BANERJEE
we find that the NTW model has mixed characteristics of simple liquids and ionic melts. Our study further ... and the value of the Rosenfeld exponents are differ- ent from that found for ..... Lennard-Jones chains J. Chem. Phys. 129 164904. 4.
Stochasticity thresholds in the Fermi-Pasta-Ulam model
International Nuclear Information System (INIS)
Callegari, B.; Galgani, L.; Milan Univ.
1979-01-01
The authors consider the celebrated model of Fermi, Pasta and Ulam and give a numerical estimate for its thresholds of stochasticity, thus determining a critical energy as a function of the frequency of the corresponding oscillators. The results turn out to be qualitatively similar to those already obtained for a chain of particles with nearest-neighbour Lennard-Jones interaction potential. (author)
Stochasticity thresholds in the Fermi-Pasta-Ulam model
Energy Technology Data Exchange (ETDEWEB)
Callegari, B [Ferrara Univ. (Italy). Ist. di Matematica; Carotta, M C; Ferrario, C [Ferrara Univ. (Italy). Ist. di Fisica; Lo Vecchio, G [Ferrara Univ. (Italy). Ist. di Fisica; Gruppo Nazionale di Struttura della Materia, Ferrara (Italy)); Galgani, L [Milan Univ. (Italy). Ist. di Fisica; Milan Univ. (Italy). Ist. di Matematica)
1979-12-11
The authors consider the celebrated model of Fermi, Pasta and Ulam and give a numerical estimate for its thresholds of stochasticity, thus determining a critical energy as a function of the frequency of the corresponding oscillators. The results turn out to be qualitatively similar to those already obtained for a chain of particles with nearest-neighbour Lennard-Jones interaction potential.
Pramana – Journal of Physics | Indian Academy of Sciences
Indian Academy of Sciences (India)
Home; Journals; Pramana – Journal of Physics. O akinlade. Articles written in Pramana – Journal of Physics. Volume 64 Issue 2 February 2005 pp 269-279 Research Articles. Structures and autocorrelation functions of liquid Al and Mg modelled via Lennard-Jones potential from molecular dynamics simulation.
Growing correlation length on cooling below the onset of caging in a simulated glass-forming liquid
DEFF Research Database (Denmark)
Lačević, N.; Starr, F. W.; Schrøder, Thomas
2002-01-01
We present a calculation of a fourth-order, time-dependent density correlation function that measures higher-order spatiotemporal correlations of the density of a liquid. From molecular dynamics simulations of a glass-forming Lennard-Jones liquid, we find that the characteristic length scale...... of the dynamics of the liquid in the alpha-relaxation regime....
Gas Enrichment at Liquid-Wall Interfaces
Dammer, S.M.; Lohse, Detlef
2006-01-01
Molecular dynamics simulations of Lennard-Jones systems are performed to study the effects of dissolved gas on liquid-wall and liquid-gas interfaces. Gas enrichment at walls, which for hydrophobic walls can exceed more than 2 orders of magnitude when compared to the gas density in the bulk liquid,
Indian Academy of Sciences (India)
Home; Journals; Pramana – Journal of Physics. G A Adebayo. Articles written in Pramana – Journal of Physics. Volume 64 Issue 2 February 2005 pp 269-279 Research Articles. Structures and autocorrelation functions of liquid Al and Mg modelled via Lennard-Jones potential from molecular dynamics simulation.
Density scaling and quasiuniversality of flow-event statistics for athermal plastic flows
Lerner, E.; Bailey, N.P.; Dyre, J.C.
2014-01-01
Athermal steady-state plastic flows were simulated for the Kob-Andersen binary Lennard-Jones system and its repulsive version in which the sign of the attractive terms is changed to a plus. Properties evaluated include the distributions of energy drops, stress drops, and strain intervals between the
Density-scaling exponents and virial potential-energy correlation ...
Indian Academy of Sciences (India)
This paper investigates the relation between the density-scaling exponent γ and the virial potential energy correlation coefficient R at several thermodynamic state points in three dimensions for the generalized (2n, n) Lennard-Jones (LJ) system for n = 4, 9, 12, 18, as well as for the standard n = 6 LJ system in two,three, and ...
Pramana – Journal of Physics | Indian Academy of Sciences
Indian Academy of Sciences (India)
Home; Journals; Pramana – Journal of Physics. L A Hussain. Articles written in Pramana – Journal of Physics. Volume 64 Issue 2 February 2005 pp 269-279 Research Articles. Structures and autocorrelation functions of liquid Al and Mg modelled via Lennard-Jones potential from molecular dynamics simulation.
Study of structure and spectroscopy of water–hydroxide ion clusters ...
Indian Academy of Sciences (India)
Experimen- talists are interested in determining the bonding,1–18 structure and spectroscopy of these systems and the- oreticians have contributed to the logical explanation of experimental findings. There are different types of systems ranging from atomic clusters, especially noble gas clusters (modelled by Lennard Jones ...
Calculation of Liquid Water-Hydrate-Methane Vapor Phase Equilibria from Molecular Simulations
DEFF Research Database (Denmark)
Jensen, Lars; Thomsen, Kaj; von Solms, Nicolas
2010-01-01
using the TIP4P/ice potential and a united-atom Lennard-Jones potential. respectively. The equilibrium calculation method for this system has three components, (i) thermodynamic integration from a supercritical ideal gas to obtain the fluid-phase chemical potentials. (ii) calculation of the chemical...
Calculation of partial enthalpies in argon-krypton mixtures by NPT molecular dynamics
Sindzingre, P.; Massobrio, C.; Ciccotti, G.; Frenkel, D.
1989-01-01
In an earlier paper, we have indicated how, by using a particle-insertion technique, partial molar enthalpies and related quantities can be evaluated from simulations on a single state point. In the present paper we apply this method to a Lennard-Jones argon-krypton mixture. For this particular
Boundary layer energies for nonconvex discrete systems
Scardia, L.; Schlömerkemper, A.; Zanini, C.
2011-01-01
In this work we consider a one-dimensional chain of atoms which interact through nearest and next-to-nearest neighbour interactions of Lennard-Jones type. We impose Dirichlet boundary conditions and in addition prescribe the deformation of the second and last but one atoms of the chain. This
HNC variational calculations of boson matter
International Nuclear Information System (INIS)
Lantto, L.J.; Jackson, A.D.; Siemens, P.J.
1977-01-01
A simple and reliable numerical technique is given for determining the two-body distribution function which minimizes the HNC energy of boson matter. Numerical results are presented for the neutron matter homework problem and the 4 He Lennard-Jones potential. The resulting distribution function is found to have proper asymptotic behaviour and yields reasonable binding energies. (Auth.)
Joost, Meelis
2015-01-01
21.–27. juulil 2015 osales EPIKoja 2-liikmeline meeskond koolitusel Venemaal Nižni Novgorodis, mille korraldas Austria organisatsioon Grenzenlos koostöös Venemaa organisatsiooniga SFERA. Koolituse eesmärgiks oli selgitada, kuidas Euroopa Liidu erinevatesse programmidesse on võimalik paremini kaasata erivajadustega inimesi
Group leaders optimization algorithm
Daskin, Anmer; Kais, Sabre
2011-03-01
We present a new global optimization algorithm in which the influence of the leaders in social groups is used as an inspiration for the evolutionary technique which is designed into a group architecture. To demonstrate the efficiency of the method, a standard suite of single and multi-dimensional optimization functions along with the energies and the geometric structures of Lennard-Jones clusters are given as well as the application of the algorithm on quantum circuit design problems. We show that as an improvement over previous methods, the algorithm scales as N 2.5 for the Lennard-Jones clusters of N-particles. In addition, an efficient circuit design is shown for a two-qubit Grover search algorithm which is a quantum algorithm providing quadratic speedup over the classical counterpart.
NVU dynamics. II. Comparing to four other dynamics
DEFF Research Database (Denmark)
Ingebrigtsen, Trond; Toxværd, Søren; Schrøder, Thomas
2011-01-01
-potential-energy hypersurface. Here, simulations of NVU dynamics are compared to results for four other dynamics, both deterministic and stochastic. First, NVU dynamics is compared to the standard energy-conserving Newtonian NVE dynamics by simulations of the Kob-Andersen binary Lennard-Jones liquid, its WCA version (i.......e., with cut-off's at the pair potential minima), and the Lennard-Jones Gaussian liquid. We find identical results for all quantities probed: radial distribution functions, incoherent intermediate scattering functions, and mean-square displacement as function of time. Arguments are presented...... on the constant-potential-energy hypersurface, and to Nos-Hoover NVT dynamics. If time is scaled for the two stochastic dynamics to make single-particle diffusion constants identical to that of NVE dynamics, the simulations show that all five dynamics are equivalent at low temperatures except at short times....
International Nuclear Information System (INIS)
Bertagnolli, H.
1978-01-01
For the case of special molecular models representing the acetonitrile molecule the expansion coefficients of the molecular par distribution function are calculated by use of pertubation theory. These results are used to get theoretical access to scattering intensities in the frame of several approximations. The first model describes the molecule by three hard spheres and uses a hard sphere liquid as reference. In the second cast the calculations are based on an anisotropic Lennard-Jones potential by application of a model of overlapping ellipsoids and by use of a Lennard-Jones liquid as a reference system. In the third model dipolar attractive forces are taken into account with an anisotropic hard-sphere liquid as a reference. In the third model dipolar attractive forces are taken into account with an anisotropic hard-sphere liquid as a reference. Finally all the calculations with different intermolecular potentials are compared with neutron scattering experiments. (orig.) 891 HK [de
On the equivalence of continuum and lattice models for fluids
International Nuclear Information System (INIS)
Panagiotopoulos, Athanassios Z.
2000-01-01
It was demonstrated that finely discretized lattice models for fluids with particles interacting via Lennard-Jones or exponential-6 potentials have essentially identical thermodynamic and structural properties to their continuum counterparts. Grand canonical histogram reweighting Monte Carlo calculations were performed for systems with repulsion exponents between 11 and 22. Critical parameters were determined from mixed-field finite-size scaling methods. Numerical equivalence of lattice and continuous space models, within simulation uncertainties, was observed for lattices with ratio of particle diameter σ to grid spacing of 10. The lattice model calculations were more efficient computationally by factors between 10 and 20. It was also shown that Lennard-Jones and exponential-6 based models with identical critical properties can be constructed by appropriate choice of the repulsion exponent. (c) 2000 American Institute of Physics
Graphene on Cu(111) at the nonzero temperatures: Molecular dynamic simulation
Sidorenkov, A. V.; Kolesnikov, S. V.; Saletsky, A. M.
2017-11-01
We present results of molecular dynamic simulation of continuous graphene monolayer on Cu(111). In this paper, we investigate the dependencies of the average binding energy and the average binding distance on the temperature. The interaction between carbon and copper atoms was described by Lennard-Jones potential. It is shown that the binding energy practically remains constant in a wide range of temperatures 0-800 K. However, in the same temperature range, the binding distance of graphene on Cu(111) surface has a linear dependence on temperature. The dependence of the linear thermal expansion coefficient of the binding distance on Lennard-Jones parameters has been calculated. We suggest a simple theoretical model to explain this dependence qualitatively.
Dislocation-like Structures in a Simulated Liquid
DEFF Research Database (Denmark)
Cotterill, Rodney M J
1979-01-01
The free-volume distribution in a simulated Lennard-Jones liquid is heterogeneous. Chains of holes, appearing as segments rather than a continuous network, have lifetimes that are brief compared with the mean vibration period of the atoms. Larger isolated holes persist for longer times. If the ch......The free-volume distribution in a simulated Lennard-Jones liquid is heterogeneous. Chains of holes, appearing as segments rather than a continuous network, have lifetimes that are brief compared with the mean vibration period of the atoms. Larger isolated holes persist for longer times....... If the chains are interpreted as dislocation cores, the observed dislocation density is 1.0×1014 cm-2, but the actual density is probably higher....
Koperwas, K.; Affouard, F.; Gerges, J.; Valdes, L.-C.; Adrjanowicz, K.; Paluch, M.
2017-12-01
In this paper, we examine, in terms of the classical nucleation theory, how the strengthening of the attractive intermolecular interactions influences the crystallization process for systems like Lennard-Jones at different isobaric conditions. For this purpose, we modify the standard Lennard-Jones potential, and as a result, we obtain three different systems characterized by various strengths of attractive potentials occurring between molecules, which are in direct relationship to the physical quantities describing molecules, e.g., its polarizability or dipole moment. Based on performed analysis, we demonstrate that the molecular attraction primarily impacts the thermodynamics of the interface between liquid and crystal. This is reflected in the behavior of nucleation and overall crystallization rates during compression of the system.
Phononless soliton waves as early forerunners of crystalline material fracture
International Nuclear Information System (INIS)
Dubovskij, O.A.; Orlov, A.V.
2007-01-01
Phononless soliton waves of compression are shown to generate at a critical tension of crystals featuring real Lennard-Jones potential of interatomic interaction just before their fracture. A new method of nonlinear micro dynamics was applied to define the initial atomic displacements at high excitation energies. A solution is found that corresponds to a soliton wave running before the front of fracture. In a bounded crystal, the soliton being reflected from the crystal boundary passes the front of fracture and deforms while moving in the opposite direction. The amplitude and spectral characteristics of that type of soliton waves in crystals with a modified Lennard-Jones potential have been investigated. An approximate analytical solution was found for the soliton waves [ru
International Nuclear Information System (INIS)
Jakubov, T.S.; Mainwaring, D.E.
2006-01-01
In the present work a generalized Kelvin equation for a fluid confined in thick-walled cylindrical capillary is developed. This has been accomplished by including the potential energy function for interaction between a solid wall of a capillary and a confined fluid into the Kelvin equation. Using the Lennard-Jones 12-6 potential, an explicit form of the potential energy functions as expressed by hypergeometrical functions have been derived-firstly, for the interaction between a solid wall and a test atom placed at an arbitrary point in a long open-end capillary, and thereafter for the body-body interaction between the solid wall and a confined Lennard-Jones fluid. Further, this generalized Kelvin equation has been applied to detailed description hysteresis phenomena in such capillaries. All numerical calculations have been carried out for the model argon-graphite system at 90 K
Shear-induced phase changes in mixtures
International Nuclear Information System (INIS)
Romig, K.D.; Hanley, H.J.M.
1986-01-01
A thermodynamic theory to account for the behavior of liquid mixtures exposed to a shear is developed. One consequence of the theory is that shear-induced phase changes are predicted. The theory is based on a thermodynamics that includes specifically the shear rate in the formalism and is applied to mixtures by a straightforward modification of the corresponding states, conformalsolution approach. The approach is general but is used here for a mixture of Lennard-Jones particles with a Lennard-Jones equation of state as a reference fluid. The results are discussed in the context of the Scott and Van Konynenberg phase classification. It is shown that the influence of a shear does affect substantially the type of the phase behavior. Results from the model mixture are equated loosely with those from real polymeric liquids
International Nuclear Information System (INIS)
Fay, P.J.; Ray, J.R.; Wolf, R.J.
1994-01-01
We present a new, nondestructive, method for determining chemical potentials in Monte Carlo and molecular dynamics simulations. The method estimates a value for the chemical potential such that one has a balance between fictitious successful creation and destruction trials in which the Monte Carlo method is used to determine success or failure of the creation/destruction attempts; we thus call the method a detailed balance method. The method allows one to obtain estimates of the chemical potential for a given species in any closed ensemble simulation; the closed ensemble is paired with a ''natural'' open ensemble for the purpose of obtaining creation and destruction probabilities. We present results for the Lennard-Jones system and also for an embedded atom model of liquid palladium, and compare to previous results in the literature for these two systems. We are able to obtain an accurate estimate of the chemical potential for the Lennard-Jones system at higher densities than reported in the literature
Kinetic energy of solid and liquid para-hydrogen: a path integral Monte Carlo simulation
International Nuclear Information System (INIS)
Zoppi, M.; Neumann, M.
1992-01-01
The translational (center of mass) kinetic energy of solid and liquid para-hydrogen have been recently measured by means of Deep Inelastic Neutron Scattering. We have evaluated the same quantity, in similar thermodynamic conditions, by means of Path Integral Monte Carlo computer simulation, modelling the system as composed of a set of spherical molecules interacting through a pairwise additive Lennard-Jones potential. In spite of the crude approximations on the interaction potential, the agreement is excellent. The pressure was also computed by means of the same simulations. This quantity, compared with the equation of state for solid para-hydrogen given by Driessen and Silvera, gives an agreement of a lesser quality and a negative value for the liquid state. We attribute this discrepancy to the limitations of the Lennard-Jones potential. (orig.)
Molecular dynamic simulation of Copper and Platinum nanoparticles Poiseuille flow in a nanochannels
Toghraie, Davood; Mokhtari, Majid; Afrand, Masoud
2016-10-01
In this paper, simulation of Poiseuille flow within nanochannel containing Copper and Platinum particles has been performed using molecular dynamic (MD). In this simulation LAMMPS code is used to simulate three-dimensional Poiseuille flow. The atomic interaction is governed by the modified Lennard-Jones potential. To study the wall effects on the surface tension and density profile, we placed two solid walls, one at the bottom boundary and the other at the top boundary. For solid-liquid interactions, the modified Lennard-Jones potential function was used. Velocity profiles and distribution of temperature and density have been obtained, and agglutination of nanoparticles has been discussed. It has also shown that with more particles, less time is required for the particles to fuse or agglutinate. Also, we can conclude that the agglutination time in nanochannel with Copper particles is faster that in Platinum nanoparticles. Finally, it is demonstrated that using nanoparticles raises thermal conduction in the channel.
Equilibrium properties of dense hydrogen isotope gases based on the theory of simple fluids.
Kowalczyk, Piotr; MacElroy, J M D
2006-08-03
We present a new method for the prediction of the equilibrium properties of dense gases containing hydrogen isotopes. The proposed approach combines the Feynman-Hibbs effective potential method and a deconvolution scheme introduced by Weeks et al. The resulting equations of state and the chemical potentials as functions of pressure for each of the hydrogen isotope gases depend on a single set of Lennard-Jones parameters. In addition to its simplicity, the proposed method with optimized Lennard-Jones potential parameters accurately describes the equilibrium properties of hydrogen isotope fluids in the regime of moderate temperatures and pressures. The present approach should find applications in the nonlocal density functional theory of inhomogeneous quantum fluids and should also be of particular relevance to hydrogen (clean energy) storage and to the separation of quantum isotopes by novel nanomaterials.
Isomorph invariance of Couette shear flows simulated by the SLLOD equations of motion
DEFF Research Database (Denmark)
Separdar, Leila; Bailey, Nicholas; Schrøder, Thomas
2013-01-01
fluctuations of virial and potential energy. Such systems have good isomorphs (curves in the thermodynamic phase diagram along which structural, dynamical, and some thermodynamic quantities are invariant when expressed in reduced units). The SLLOD equations of motion were used to simulate Couette shear flows......Non-equilibrium molecular dynamics simulations were performed to study the thermodynamic, structural, and dynamical properties of the single-component Lennard-Jones and the Kob-Andersen binary Lennard-Jones liquids. Both systems are known to have strong correlations between equilibrium thermal...... of the two systems. We show analytically that these equations are isomorph invariant provided the reduced strain rate is fixed along the isomorph. Since isomorph invariance is generally only approximate, a range of strain rates were simulated to test for the predicted invariance, covering both the linear...
Effective diameters and corresponding states of fluids
Del Río, Fernando
Effective hard-sphere diameters of fluids with purely repulsive interactions are derived from a generalized corresponding-states principle of Leland, Rowlinson and coworkers. Various alternative definitions are discussed and related. Virial expansions of the effective diameters and their corresponding volumes are obtained and compared with results of perturbation theory. Applications are made to inverse-power potentials, the repulsive part of the Lennard-Jones potential and hard spherocylinders and dumbells.
Cluster pair correlation function of simple fluids: energetic connectivity criteria
Pugnaloni, Luis A.; Zarragoicoechea, Guillermo J.; Vericat, Fernando
2006-01-01
We consider the clustering of Lennard-Jones particles by using an energetic connectivity criterion proposed long ago by T.L. Hill [J. Chem. Phys. 32, 617 (1955)] for the bond between pairs of particles. The criterion establishes that two particles are bonded (directly connected) if their relative kinetic energy is less than minus their relative potential energy. Thus, in general, it depends on the direction as well as on the magnitude of the velocities and positions of the particles. An integ...
SIMPLE FLUID IN AN ATTRACTIVE, DISORDERED POLYDISPERSE MATRIX
Directory of Open Access Journals (Sweden)
T.Patsahan
2004-01-01
Full Text Available The extension of the replica Ornstein-Zernike (ROZ equations is applied to the study of the structural properties of a Lennard-Jones fluid confined in an attractive polydisperse disordered matrix. The ROZ equations in combination with the orthogonal polynomial expansions for the correlation functions are used. The radial distribution functions are calculated for the adsorbed fluid at different temperatures. The effect of matrix polydispersity on the excess internal energy is considered in our study as well.
Microcanonical Monte Carlo approach for computing melting curves by atomistic simulations
Davis, Sergio; Gutiérrez, Gonzalo
2017-01-01
We report microcanonical Monte Carlo simulations of melting and superheating of a generic, Lennard-Jones system starting from the crystalline phase. The isochoric curve, the melting temperature $T_m$ and the critical superheating temperature $T_{LS}$ obtained are in close agreement (well within the microcanonical temperature fluctuations) with standard molecular dynamics one-phase and two-phase methods. These results validate the use of microcanonical Monte Carlo to compute melting points, a ...
1992-11-01
is more compact relative to that in the [001] direction. Detailed MD studies (De Lorenzi, Jacucci, and Pontikis 1982), using Lennard-Jones...Jacucci, and Pontikis 1982) have shown that the predominance of the adatom exchange mechanism results in nearly isotropic diffusion which is further...G., G. Jacucci, and V. Pontikis . Surface Science, vol. 116, p. 391, 1982. Doll, J. D., and A. F. Voter. Ann. Rev. Phys. Chem., vol. 38, p. 413, 1987
The second virial coefficients of some halogenated ethanes
Kohler, Friedrich; van Nhu, Nguyen
The second virial coefficients of 1,1-difluoroethane, 1,1,1-trifluoroethane, 1,1,1,2-tetrafluoroethane and 1-chloro-1,1-difluoroethane have been calculated on the basis of two-centre-Lennard-Jones + superimposed dipole model potentials and compared with experimental results. These can be explained taking into account the reduced dipole moments and the angle between dipole moment and molecular axis.
DEFF Research Database (Denmark)
Galliero, Guillaume; Medvedev, Oleg; Shapiro, Alexander
2005-01-01
A 322 (2004) 151). In the current study, a fast molecular dynamics scheme has been developed to determine the values of the penetration lengths in Lennard-Jones binary systems. Results deduced from computations provide a new insight into the concept of penetration lengths. It is shown for four different...... fluctuation theory and molecular dynamics scheme exhibit consistent trends and average deviations from experimental data around 10-20%. (c) 2004 Elsevier B.V. All rights reserved....
Molecular dynamics study of vacancy-like defects in a model glass : static behaviour
Delaye, J. M.; Limoge, Y.
1993-10-01
The possibility of defining vacancy-like defects in a Lennard-Jones glass is searched for in a systematic manner. Considering different relaxation levels of the same system, as well as different external pressures, we use a Molecular Dynamics simulation method, to study at constant volume or external pressure, the relaxation of a “piece” of glass, after the sudden removal of an atom. Three typical kinds of behaviour can be observed: the persistence of the empty volume left by the missing atom, its migration by clearly identifiable atomic jumps and the dissipation “on the spot”. A careful analysis of the probabilities of these three kinds of behaviour shows that a meaningful definition of vacancy-like defects can be given in a Lennard-Jones glass. Dans cet article, nous nous penchons de façon systématique sur la possibilité de définir des défauts de type lacunaire dans un verre de Lennard-Jones, à différents niveaux de relaxation et de pression, par une méthode de simulation numérique en dynamique moléculaire à volume ou à pression constants. Le défaut est créé en supprimant un atome et en suivant la réponse du système. Nous observons trois comportements typiques : la persistance sur place du “trou” laissé par l'atome supprimé, sa migration par des sauts atomiques clairement identifiés et enfin sa dissipation sur place. Une analyse détaillée de ces trois comportements montre qu'il est possible dans un verre de Lennard-Jones de définir des défauts de type lacunaire.
First order phase transition of expanding matter and its fragmentation
International Nuclear Information System (INIS)
Chikazumi, Shinpei; Iwamoto, Akira
2002-01-01
Using an expanding matter model with a Lennard-Jones potential, the instability of the expanding system is investigated. The pressure, the temperature, and the density fluctuations are calculated as functions of density during the time evolution of the expanding matter, which are compared to the coexistence curve calculated by the Gibbs ensemble. The expanding matter undergoes the first order phase transition in the limit of the quasistatic expansion. The resultant fragment mass distributions are also investigated. (author)
Condensation and Evaporation Transitions in Deep Capillary Grooves
Malijevský, A. (Alexandr); Parry, A.O.
2014-01-01
We study the order of capillary condensation and evaporation transitions of a simple fluid adsorbed in a deep capillary groove using a fundamental measure density functional theory (DFT). The walls of the capillary interact with the fluid particles via long-ranged, dispersion, forces while the fluid-fluid interaction is modelled as a truncated Lennard-Jones-like potential. We find that below the wetting temperature $T_w$ condensation is first-order and evaporation is continuous with the metas...
Resolving dispersion and induction components for polarisable molecular simulations of ionic liquids
Pádua, Agílio A. H.
2017-05-01
One important development in interaction potential models, or atomistic force fields, for molecular simulation is the inclusion of explicit polarisation, which represents the induction effects of charged or polar molecules on polarisable electron clouds. Polarisation can be included through fluctuating charges, induced multipoles, or Drude dipoles. This work uses Drude dipoles and is focused on room-temperature ionic liquids, for which fixed-charge models predict too slow dynamics. The aim of this study is to devise a strategy to adapt existing non-polarisable force fields upon addition of polarisation, because induction was already contained to an extent, implicitly, due to parametrisation against empirical data. Therefore, a fraction of the van der Waals interaction energy should be subtracted so that the Lennard-Jones terms only account for dispersion and the Drude dipoles for induction. Symmetry-adapted perturbation theory is used to resolve the dispersion and induction terms in dimers and to calculate scaling factors to reduce the Lennard-Jones terms from the non-polarisable model. Simply adding Drude dipoles to an existing fixed-charge model already improves the prediction of transport properties, increasing diffusion coefficients, and lowering the viscosity. Scaling down the Lennard-Jones terms leads to still faster dynamics and densities that match experiment extremely well. The concept developed here improves the overall prediction of density and transport properties and can be adapted to other models and systems. In terms of microscopic structure of the ionic liquids, the inclusion of polarisation and the down-scaling of Lennard-Jones terms affect only slightly the ordering of the first shell of counterions, leading to small decreases in coordination numbers. Remarkably, the effect of polarisation is major beyond first neighbours, significantly weakening spatial correlations, a structural effect that is certainly related to the faster dynamics of
Molecular dynamics simulation of a chemical reaction
International Nuclear Information System (INIS)
Gorecki, J.; Gryko, J.
1988-06-01
Molecular dynamics is used to study the chemical reaction A+A→B+B. It is shown that the reaction rate constant follows the Arrhenius law both for Lennard-Jones and hard sphere interaction potentials between substrate particles. A. For the denser systems the reaction rate is proportional to the value of the radial distribution function at the contact point of two hard spheres. 10 refs, 4 figs
International Nuclear Information System (INIS)
Kumar, P. V.; Maroncelli, M.
2000-01-01
Simulations of the time-dependent friction controlling rotational, translational, and vibrational motions of dipolar diatomic solutes in acetonitrile and methanol have been used to examine the nature of ''dielectric'' friction. The way in which electrical interactions increase the friction beyond that present in nonpolar systems is found to be rather different than what is anticipated by most theories of dielectric friction. Long-range electrostatic forces do not simply add an independent contribution to the friction due to short-ranged or ''mechanical'' sources (modeled here in terms of Lennard-Jones forces). Rather, the electrical and Lennard-Jones contributions are found to be strongly anticorrelated and not separable in any useful way. For some purposes, the mechanism by which electrical interactions increase friction is better viewed as a static electrostriction effect: electrical forces cause a subtle increase in atomic density in the solute's first solvation shell, which increases the amplitude of the force fluctuations derived from the Lennard-Jones interactions, i.e., the mechanical friction. However, electrical interactions also modify the dynamics of the friction, typically adding a long-time tail, which significantly increases the integral friction. Both of these effects must be included in a correct description of friction in the presence of polar interactions. (c) 2000 American Institute of Physics
Adsorption of metal atoms at a buckled graphene grain boundary using model potentials
International Nuclear Information System (INIS)
Helgee, Edit E.; Isacsson, Andreas
2016-01-01
Two model potentials have been evaluated with regard to their ability to model adsorption of single metal atoms on a buckled graphene grain boundary. One of the potentials is a Lennard-Jones potential parametrized for gold and carbon, while the other is a bond-order potential parametrized for the interaction between carbon and platinum. Metals are expected to adsorb more strongly to grain boundaries than to pristine graphene due to their enhanced adsorption at point defects resembling those that constitute the grain boundary. Of the two potentials considered here, only the bond-order potential reproduces this behavior and predicts the energy of the adsorbate to be about 0.8 eV lower at the grain boundary than on pristine graphene. The Lennard-Jones potential predicts no significant difference in energy between adsorbates at the boundary and on pristine graphene. These results indicate that the Lennard-Jones potential is not suitable for studies of metal adsorption on defects in graphene, and that bond-order potentials are preferable
Phase transitions of quadrupolar fluids
International Nuclear Information System (INIS)
OShea, S.F.; Dubey, G.S.; Rasaiah, J.C.
1997-01-01
Gibbs ensemble simulations are reported for Lennard-Jones particles with embedded quadrupoles of strength Q * =Q/(εσ 5 ) 1/2 =2.0 where ε and σ are the Lennard-Jones parameters. Calculations revealing the effect of the dispersive forces on the liquid endash vapor coexistence were carried out by scaling the attractive r -6 term in the Lennard-Jones pair potential by a factor λ ranging from 0 to 1. Liquid endash vapor coexistence is observed for all values of λ including λ=0 for Q * =2.0, unlike the corresponding dipolar fluid studied by van Leeuwen and Smit et al. [Phys. Rev. Lett. 71, 3991 (1993)] which showed no phase transition below λ=0.35 when the reduced dipole moment μ * =2.0. The simulation data are analyzed to estimate the critical properties of the quadrupolar fluid and their dependence on the strength λ of the dispersive force. The critical temperature and pressure show a clear quadratic dependence on λ, while the density is less confidently identified as being linear in λ. The compressibility is roughly linear in λ. copyright 1997 American Institute of Physics
Parsing partial molar volumes of small molecules: a molecular dynamics study.
Patel, Nisha; Dubins, David N; Pomès, Régis; Chalikian, Tigran V
2011-04-28
We used molecular dynamics (MD) simulations in conjunction with the Kirkwood-Buff theory to compute the partial molar volumes for a number of small solutes of various chemical natures. We repeated our computations using modified pair potentials, first, in the absence of the Coulombic term and, second, in the absence of the Coulombic and the attractive Lennard-Jones terms. Comparison of our results with experimental data and the volumetric results of Monte Carlo simulation with hard sphere potentials and scaled particle theory-based computations led us to conclude that, for small solutes, the partial molar volume computed with the Lennard-Jones potential in the absence of the Coulombic term nearly coincides with the cavity volume. On the other hand, MD simulations carried out with the pair interaction potentials containing only the repulsive Lennard-Jones term produce unrealistically large partial molar volumes of solutes that are close to their excluded volumes. Our simulation results are in good agreement with the reported schemes for parsing partial molar volume data on small solutes. In particular, our determined interaction volumes() and the thickness of the thermal volume for individual compounds are in good agreement with empirical estimates. This work is the first computational study that supports and lends credence to the practical algorithms of parsing partial molar volume data that are currently in use for molecular interpretations of volumetric data.
Energy Technology Data Exchange (ETDEWEB)
Claas, P.
2006-01-15
In the present thesis first studies on the short-time dynamics in alkali dimers and microclusters, which were bound on the surface of superfluid helium droplets, were presented. The experiments comprehended pump-probe measurements on the fs scale on the vibration dynamics on the dimers and on the fragmentation dynamics on the clusters. Generally by the studies it was shown that such extremely short slopes can also be observed on helium droplets by means of the femtosecond spectroscopy.
Vapor-Liquid-Solid Etch of Semiconductor Surface Channels by Running Gold Nanodroplets.
Nikoobakht, Babak; Herzing, Andrew; Muramoto, Shin; Tersoff, Jerry
2015-12-09
We show that Au nanoparticles spontaneously move across the (001) surface of InP, InAs, and GaP when heated in the presence of water vapor. As they move, the particles etch crystallographically aligned grooves into the surface. We show that this process is a negative analogue of the vapor-liquid-solid (VLS) growth of semiconductor nanowires: the semiconductor dissolves into the catalyst and reacts with water vapor at the catalyst surface to create volatile oxides, depleting the dissolved cations and anions and thus sustaining the dissolution process. This VLS etching process provides a new tool for directed assembly of structures with sublithographic dimensions, as small as a few nanometers in diameter. Au particles above 100 nm in size do not exhibit this process but remain stationary, with oxide accumulating around the particles.
Generation of micro- and nano-droplets containing immiscible solutions in view of optical studies
Nastasa, V.; Karapantsios, T.; Samaras, K.; Dafnopatidou, E.; Pradines, V.; Miller, R.; Pascu, M. L.
2010-08-01
The multiple resistances to treatment, developed by bacteria and malignant tumors require finding alternatives to the existing medicines and treatment procedures. One of them is strengthening the effects of cytostatics by improving the delivery method. Such a method is represented by the use of medicines as micro/nano-droplets. This method can reduce the substance consumption by generating drug micro-droplets incorporated in substances that can favour a faster localization, than the classical mode of medicine administration, to the tumor tissues. This paper contains the results concerning the generation and study of micro/nano-droplets and the generation of micro-droplets with an inner core (medicine) and a thin layer covering it. We have measured the surface tension at water/air interface and water/oil interface for a medicine (Vancomycin) and we have generated and measured droplets of medicine containing a layer of Vitamin A by using a double capillary system. The micro/nano-droplets may be produced by mixing of two immiscible solutions in particular conditions (high rotating speed and/or high pressure difference). For this we have studied the generation of emulsions of vitamin A diluted in sunflower oil and a solution of a surfactant Tween 80 in distilled water. The concentration of surfactant in water was typically 4*10-5M. We have studied in a batch stirred tank system the dependence of the droplet dimensions in emulsion, function of the mixing rotation speed, agitation time and components ratio. The droplet diameters were measured using a Malvern light scattering instrument type Mastersizer Hydro 2000M. We have obtained droplets with diameters smaller than 100 nm; the diameters distribution exhibited a peak at 65 nm.
Atomistic Simulations of Thermophoretic Motion of water Nanodroplets in Carbon Nanotubes
DEFF Research Database (Denmark)
Zambrano, Harvey A; Walther, Jens Honore; Koumoutsakos, Petros
2008-01-01
Open-ended nanotubes offer unique possibilities as fluid conduits with applications ranging from molecule separation devices in biocatalysis to encapsulation media for drug storage and delivery. Liquids and solids in nanochannels may be driven by electrophoresis, osmosis, gradients in the surface......-1925 for thermodiffusion in gases. Ibbs found that the coefficient of thermal diffusion is more sensitive than any of the other transport coefficients to the nature of the intermolecular forces.1 Thus, a complete understanding of the thermal diffusion could provide a powerful means of investigation of forces between...... molecules. Although the theoretical explanation of thermodiffusion for molecules in liquids is still under debate, the investigation of its practical usability is motivated by potential applications in nanotechnology. Hence, thermodiffusion was recently used as the driving mechanism in artificially...
A Polar Isomer of Formic Acid Dimer Formed in Helium Nanodroplets
Czech Academy of Sciences Publication Activity Database
Madeja, F.; Havenith, M.; Nauta, K.; Miller, R. E.; Chocholoušová, Jana; Hobza, Pavel
2004-01-01
Roč. 120, č. 22 (2004), s. 10554-10560 ISSN 0021-9606 R&D Projects: GA MŠk LN00A032 Institutional research plan: CEZ:AV0Z4040901 Keywords : resolution infrared - spectroscopy * double-resonance spectroscopy * ab initio calculations Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.105, year: 2004
Energy Technology Data Exchange (ETDEWEB)
Kavadiya, Shalinee; Raliya, Ramesh; Schrock, Michael; Biswas, Pratim, E-mail: pbiswas@wustl.edu [Washington University in St. Louis, Aerosol and Air Quality Research Laboratory, Department of Energy, Environmental and Chemical Engineering (United States)
2017-02-15
Restacking of graphene oxide (GO) nanosheets results in loss of surface area and creates limitations in its widespread use for applications. Previously, two-dimensional (2D) GO sheets have been crumpled into 3D structures to prevent restacking using different techniques. However, synthesis of nanometer size crumpled graphene particles and their direct deposition onto a substrate have not been demonstrated under room temperature condition so far. In this work, the evaporative crumpling of GO sheets into very small size (<100 nm) crumpled structures using an electrohydrodynamic atomization technique is described. Systematic study of the effect of different electrohydrodynamic atomization parameters, such as (1) substrate-to-needle distance, (2) GO concentration in the precursor solution, and (3) flow rate (droplet size) on the GO crumpling, is explored. Crumpled GO (CGO) particles are characterized online using a scanning mobility particle sizer (SMPS) and off-line using electron microscopy. The relation between the confinement force and the factors affecting the crumpled structure is established. Furthermore, to expand the application horizons of the structure, crumpled GO–TiO{sub 2} nanocomposites are synthesized. The method described here allows a simple and controlled production of graphene-based particles/composites with direct deposition onto any kind of substrate for a variety of applications.
Structure and phase behavior of a confined nanodroplet composed of the flexible chain molecules.
Kim, Soon-Chul; Kim, Eun-Young; Seong, Baek-Seok
2011-04-28
A polymer density functional theory has been employed for investigating the structure and phase behaviors of the chain polymer, which is modelled as the tangentially connected sphere chain with an attractive interaction, inside the nanosized pores. The excess free energy of the chain polymer has been approximated as the modified fundamental measure-theory for the hard spheres, the Wertheim's first-order perturbation for the chain connectivity, and the mean-field approximation for the van der Waals contribution. For the value of the chemical potential corresponding to a stable liquid phase in the bulk system and a metastable vapor phase, the flexible chain molecules undergo the liquid-vapor transition as the pore size is reduced; the vapor is the stable phase at small volume, whereas the liquid is the stable phase at large volume. The wide liquid-vapor coexistence curve, which explains the wide range of metastable liquid-vapor states, is observed at low temperature. The increase of temperature and decrease of pore size result in a narrowing of liquid-vapor coexistence curves. The increase of chain length leads to a shift of the liquid-vapor coexistence curve towards lower values of chemical potential. The coexistence curves for the confined phase diagram are contained within the corresponding bulk liquid-vapor coexistence curve. The equilibrium capillary phase transition occurs at a higher chemical potential than in the bulk phase.
Magnetic Dichroism of Potassium Atoms on the Surface of Helium Nanodroplets
International Nuclear Information System (INIS)
Nagl, Johann; Auboeck, Gerald; Callegari, Carlo; Ernst, Wolfgang E.
2007-01-01
The population ratio of Zeeman sublevels of atoms on the surface of superfluid helium droplets (T=0.37 K) has been measured. Laser induced fluorescence spectra of K atoms are measured in the presence of a moderately strong magnetic field (2.9 kG). The relative difference between the two states of circular polarization of the exciting laser is used to determine the electron spin polarization of the ensemble. Equal fluorescence levels indicate that the two spin sublevels of the ground-state K atom are equipopulated, within 1%. Thermalization to 0.37 K would give a population ratio of 0.35. We deduce that the rate of spin relaxation induced by the droplet must be 2 triplet dimer we find instead full thermalization of the spin
Alfè, D; Bartók, A P; Csányi, G; Gillan, M J
2013-06-14
We show the feasibility of using quantum Monte Carlo (QMC) to compute benchmark energies for configuration samples of thermal-equilibrium water clusters and the bulk liquid containing up to 64 molecules. Evidence that the accuracy of these benchmarks approaches that of basis-set converged coupled-cluster calculations is noted. We illustrate the usefulness of the benchmarks by using them to analyze the errors of the popular BLYP approximation of density functional theory (DFT). The results indicate the possibility of using QMC as a routine tool for analyzing DFT errors for non-covalent bonding in many types of condensed-phase molecular system.
Zong, Diyuan; Yang, Zhen; Duan, Yuanyuan
2017-10-01
Wetting kinetics of water droplets on substrates with lyophilic nanopillars was investigated using molecular dynamics simulations. Early spreading of the droplet is hindered by the nanopillars because of the penetration of the liquid which induce an extra dissipation in the droplet. Droplet spreading is mainly controlled by liquid viscosity and surface tension and not dependent on solid wettability. Propagation of the fringe film is hindered by the enhanced solid wettability because of the energy barrier introduced by the interaction between water molecules and nanopillars which increase with solid wettability.
Thermal motion in proteins: Large effects on the time-averaged interaction energies
International Nuclear Information System (INIS)
Goethe, Martin; Rubi, J. Miguel; Fita, Ignacio
2016-01-01
As a consequence of thermal motion, inter-atomic distances in proteins fluctuate strongly around their average values, and hence, also interaction energies (i.e. the pair-potentials evaluated at the fluctuating distances) are not constant in time but exhibit pronounced fluctuations. These fluctuations cause that time-averaged interaction energies do generally not coincide with the energy values obtained by evaluating the pair-potentials at the average distances. More precisely, time-averaged interaction energies behave typically smoother in terms of the average distance than the corresponding pair-potentials. This averaging effect is referred to as the thermal smoothing effect. Here, we estimate the strength of the thermal smoothing effect on the Lennard-Jones pair-potential for globular proteins at ambient conditions using x-ray diffraction and simulation data of a representative set of proteins. For specific atom species, we find a significant smoothing effect where the time-averaged interaction energy of a single atom pair can differ by various tens of cal/mol from the Lennard-Jones potential at the average distance. Importantly, we observe a dependency of the effect on the local environment of the involved atoms. The effect is typically weaker for bulky backbone atoms in beta sheets than for side-chain atoms belonging to other secondary structure on the surface of the protein. The results of this work have important practical implications for protein software relying on free energy expressions. We show that the accuracy of free energy expressions can largely be increased by introducing environment specific Lennard-Jones parameters accounting for the fact that the typical thermal motion of protein atoms depends strongly on their local environment.
Thermal motion in proteins: Large effects on the time-averaged interaction energies
Energy Technology Data Exchange (ETDEWEB)
Goethe, Martin, E-mail: martingoethe@ub.edu; Rubi, J. Miguel [Departament de Física Fonamental, Universitat de Barcelona, Martí i Franquès 1, 08028 Barcelona (Spain); Fita, Ignacio [Institut de Biologia Molecular de Barcelona, Baldiri Reixac 10, 08028 Barcelona (Spain)
2016-03-15
As a consequence of thermal motion, inter-atomic distances in proteins fluctuate strongly around their average values, and hence, also interaction energies (i.e. the pair-potentials evaluated at the fluctuating distances) are not constant in time but exhibit pronounced fluctuations. These fluctuations cause that time-averaged interaction energies do generally not coincide with the energy values obtained by evaluating the pair-potentials at the average distances. More precisely, time-averaged interaction energies behave typically smoother in terms of the average distance than the corresponding pair-potentials. This averaging effect is referred to as the thermal smoothing effect. Here, we estimate the strength of the thermal smoothing effect on the Lennard-Jones pair-potential for globular proteins at ambient conditions using x-ray diffraction and simulation data of a representative set of proteins. For specific atom species, we find a significant smoothing effect where the time-averaged interaction energy of a single atom pair can differ by various tens of cal/mol from the Lennard-Jones potential at the average distance. Importantly, we observe a dependency of the effect on the local environment of the involved atoms. The effect is typically weaker for bulky backbone atoms in beta sheets than for side-chain atoms belonging to other secondary structure on the surface of the protein. The results of this work have important practical implications for protein software relying on free energy expressions. We show that the accuracy of free energy expressions can largely be increased by introducing environment specific Lennard-Jones parameters accounting for the fact that the typical thermal motion of protein atoms depends strongly on their local environment.
Põneva kappkemmerguga mõisahoones hakkab sõitma lift / Vilja Kohler
Kohler, Vilja, 1966-
2005-01-01
Tartumaal asuva Tammistu mõisa rekonstrueerimisest, projekt AS Restor arhitektidelt Mart Keskkülalt ja Reet Saluverelt. Peahoonesse tuleb puuetega laste rehabilitatsioonikeskus. Kommenteerib Meelis Joost
Communication: An exact bound on the bridge function in integral equation theories.
Kast, Stefan M; Tomazic, Daniel
2012-11-07
We show that the formal solution of the general closure relation occurring in Ornstein-Zernike-type integral equation theories in terms of the Lambert W function leads to an exact relation between the bridge function and correlation functions, most notably to an inequality that bounds possible bridge values. The analytical results are illustrated on the example of the Lennard-Jones fluid for which the exact bridge function is known from computer simulations under various conditions. The inequality has consequences for the development of bridge function models and rationalizes numerical convergence issues.
Time-dependent friction and solvation time correlation function
International Nuclear Information System (INIS)
Samanta, Alok; Ali, Sk Musharaf; Ghosh, Swapan K
2005-01-01
We have derived a new relation between the time-dependent friction and solvation time correlation function (STCF) for non-polar fluids. The friction values calculated using this relation and simulation results on STCF for a Lennard-Jones fluid are shown to have excellent agreement with the same obtained through mode-coupling theory. Also derived is a relation between the time-dependent dielectric friction and STCF for polar fluids. Routes are thus provided to obtain the time-dependent friction (non-polar as well as dielectric) from an experimentally measured quantity like STCF, even if the interparticle interaction potential is not known
The heat current density correlation function: sum rules and thermal conductivity
International Nuclear Information System (INIS)
Singh, Shaminder; Tankeshwar, K; Pathak, K N; Ranganathan, S
2006-01-01
Expressions for the second and fourth sum rules of the heat current density correlation function have been derived in an appropriate ensemble. The thermal conductivity of Lennard-Jones fluids has been calculated using these sum rules for the heat current density correlation function and the Gaussian form of the memory function. It is found that the results obtained for the thermal conductivity are in good agreement with the molecular dynamics simulation results over a wide range of densities and temperatures. Earlier results obtained using the energy current density correlation function are also discussed
The heat current density correlation function: sum rules and thermal conductivity
Energy Technology Data Exchange (ETDEWEB)
Singh, Shaminder [Department of Physics, Panjab University, Chandigarh-160 014 (India); Tankeshwar, K [Department of Physics, Panjab University, Chandigarh-160 014 (India); Pathak, K N [Department of Physics, Panjab University, Chandigarh-160 014 (India); Ranganathan, S [Department of Physics, Royal Military College, Kingston, ON, K7K 7B4 (Canada)
2006-02-01
Expressions for the second and fourth sum rules of the heat current density correlation function have been derived in an appropriate ensemble. The thermal conductivity of Lennard-Jones fluids has been calculated using these sum rules for the heat current density correlation function and the Gaussian form of the memory function. It is found that the results obtained for the thermal conductivity are in good agreement with the molecular dynamics simulation results over a wide range of densities and temperatures. Earlier results obtained using the energy current density correlation function are also discussed.
Exponential and Bessel fitting methods for the numerical solution of the Schroedinger equation
International Nuclear Information System (INIS)
Raptis, A.D.; Cash, J.R.
1987-01-01
A new method is developed for the numerical integration of the one dimensional radial Schroedinger equation. This method involves using different integration formulae in different parts of the range of integration rather than using the same integration formula throughout. Two new integration formulae are derived, one which integrates Bessel and Neumann functions exactly and another which exactly integrates certain exponential functions. It is shown that, for large r, these new formulae are much more accurate than standard integration methods for the Schroedinger equation. The benefit of using this new approach is demonstrated by considering some numerical examples based on the Lennard-Jones potential. (orig.)
Phase equilibria of binary mixtures by molecular simulation and cubic equations of state
Directory of Open Access Journals (Sweden)
Cabral V.F.
2001-01-01
Full Text Available Molecular simulation data were used to study the performance of equations of state (EoS and combining rules usually employed in thermodynamic property calculations. The Monte Carlo method and the Gibbs ensemble technique were used for determining composition and densities of vapor and liquid phases in equilibrium for binary mixtures of Lennard-Jones fluids. Simulation results are compared to data in the literature and to those calculated by the t-PR-LJ EoS. The use of adequate combining rules has been shown to be very important for the satisfactory representation of molecular simulation data.
Communication: Simple liquids' high-density viscosity
Costigliola, Lorenzo; Pedersen, Ulf R.; Heyes, David M.; Schrøder, Thomas B.; Dyre, Jeppe C.
2018-02-01
This paper argues that the viscosity of simple fluids at densities above that of the triple point is a specific function of temperature relative to the freezing temperature at the density in question. The proposed viscosity expression, which is arrived at in part by reference to the isomorph theory of systems with hidden scale invariance, describes computer simulations of the Lennard-Jones system as well as argon and methane experimental data and simulation results for an effective-pair-potential model of liquid sodium.
Isomorphs in the phase diagram of a model liquid without inverse power law repulsion
DEFF Research Database (Denmark)
Veldhorst, Arnold Adriaan; Bøhling, Lasse; Dyre, J. C.
2012-01-01
scattering function are calculated. The results are shown to reflect a hidden scale invariance; despite its exponential repulsion the Buckingham potential is well approximated by an inverse power-law plus a linear term in the region of the first peak of the radial distribution function. As a consequence...... the dynamics of the viscous Buckingham liquid is mimicked by a corresponding model with purely repulsive inverse-power-law interactions. The results presented here closely resemble earlier results for Lennard-Jones type liquids, demonstrating that the existence of strong correlations and isomorphs does...... not depend critically on the mathematical form of the repulsion being an inverse power law....
Algebraic relaxation of a time correlation function
International Nuclear Information System (INIS)
Srivastava, S.; Kumar, C.N.; Tankeshwar, K.
2004-06-01
A second order non-linear differential equation obtained from Mori's integro- differential equation is shown to transform to another form which provides algebraic decay to a time correlation function. Involved parameters in algebraic formula are related to exact properties of the corresponding correlation function. The model has been used to study a sol-gel system which is known, experimentally, to exhibit a power law decay to stress auto-correlation function. The expression obtained for the viscosity shows a logarithmic divergence at some critical value of the parameter. Some features of the model have also been tested using available information about Lennard-Jones fluids. (author)
Solitons on H bonds in proteins
DEFF Research Database (Denmark)
d'Ovidio, F.; Bohr, H.G.; Lindgård, Per-Anker
2003-01-01
system shows that the solitons are spontaneously created and are stable and moving along the helix axis. A perturbation on one of the three H-bond lines forms solitons on the other H bonds as well. The robust solitary wave may explain very long-lived modes in the frequency range of 100 cm(-1) which...... are found in recent x-ray laser experiments. The dynamics parameters of the Toda lattice are in accordance with the usual Lennard-Jones parameters used for realistic H-bond potentials in proteins....
Theory of warm ionized gases: equation of state and kinetic Schottky anomaly.
Capolupo, A; Giampaolo, S M; Illuminati, F
2013-10-01
Based on accurate Lennard-Jones-type interaction potentials, we derive a closed set of state equations for the description of warm atomic gases in the presence of ionization processes. The specific heat is predicted to exhibit peaks in correspondence to single and multiple ionizations. Such kinetic analog in atomic gases of the Schottky anomaly in solids is enhanced at intermediate and low atomic densities. The case of adiabatic compression of noble gases is analyzed in detail and the implications on sonoluminescence are discussed. In particular, the predicted plasma electron density in a sonoluminescent bubble turns out to be in good agreement with the value measured in recent experiments.
Free energy evaluation in polymer translocation via Jarzynski equality
Energy Technology Data Exchange (ETDEWEB)
Mondaini, Felipe, E-mail: fmondaini@if.ufrj.br [Centro Federal de Educação Tecnológica Celso Suckow da Fonseca, Petrópolis, 25.620-003, RJ (Brazil); Moriconi, L., E-mail: moriconi@if.ufrj.br [Instituto de Física, Universidade Federal do Rio de Janeiro, C.P. 68528, 21945-970, Rio de Janeiro, RJ (Brazil)
2014-05-01
We perform, with the help of cloud computing resources, extensive Langevin simulations, which provide free energy estimates for unbiased three-dimensional polymer translocation. We employ the Jarzynski equality in its rigorous setting, to compute the variation of the free energy in single monomer translocation events. In our three-dimensional Langevin simulations, the excluded-volume and van der Waals interactions between beads (monomers and membrane atoms) are modeled through a repulsive Lennard-Jones (LJ) potential and consecutive monomers are subject to the Finite-Extension Nonlinear Elastic (FENE) potential. Analysing data for polymers with different lengths, the free energy profile is noted to have interesting finite-size scaling properties.
Free energy evaluation in polymer translocation via Jarzynski equality
International Nuclear Information System (INIS)
Mondaini, Felipe; Moriconi, L.
2014-01-01
We perform, with the help of cloud computing resources, extensive Langevin simulations, which provide free energy estimates for unbiased three-dimensional polymer translocation. We employ the Jarzynski equality in its rigorous setting, to compute the variation of the free energy in single monomer translocation events. In our three-dimensional Langevin simulations, the excluded-volume and van der Waals interactions between beads (monomers and membrane atoms) are modeled through a repulsive Lennard-Jones (LJ) potential and consecutive monomers are subject to the Finite-Extension Nonlinear Elastic (FENE) potential. Analysing data for polymers with different lengths, the free energy profile is noted to have interesting finite-size scaling properties.
Note: Nonpolar solute partial molar volume response to attractive interactions with water.
Williams, Steven M; Ashbaugh, Henry S
2014-01-07
The impact of attractive interactions on the partial molar volumes of methane-like solutes in water is characterized using molecular simulations. Attractions account for a significant 20% volume drop between a repulsive Weeks-Chandler-Andersen and full Lennard-Jones description of methane interactions. The response of the volume to interaction perturbations is characterized by linear fits to our simulations and a rigorous statistical thermodynamic expression for the derivative of the volume to increasing attractions. While a weak non-linear response is observed, an average effective slope accurately captures the volume decrease. This response, however, is anticipated to become more non-linear with increasing solute size.
Effect of pairwise additivity on finite-temperature behavior of classical ideal gas
Shekaari, Ashkan; Jafari, Mahmoud
2018-05-01
Finite-temperature molecular dynamics simulations have been applied to inquire into the effect of pairwise additivity on the behavior of classical ideal gas within the temperature range of T = 250-4000 K via applying a variety of pair potentials and then examining the temperature dependence of a number of thermodynamical properties. Examining the compressibility factor reveals the most deviation from ideal-gas behavior for the Lennard-Jones system mainly due to the presence of both the attractive and repulsive terms. The systems with either attractive or repulsive intermolecular potentials are found to present no resemblance to real gases, but the most similarity to the ideal one as temperature rises.
Chemical potential calculations in dense liquids using metadynamics
Perego, C.; Giberti, F.; Parrinello, M.
2016-10-01
The calculation of chemical potential has traditionally been a challenge in atomistic simulations. One of the most used approaches is Widom's insertion method in which the chemical potential is calculated by periodically attempting to insert an extra particle in the system. In dense systems this method fails since the insertion probability is very low. In this paper we show that in a homogeneous fluid the insertion probability can be increased using metadynamics. We test our method on a supercooled high density binary Lennard-Jones fluid. We find that we can obtain efficiently converged results even when Widom's method fails.
Note: Nonpolar solute partial molar volume response to attractive interactions with water
Energy Technology Data Exchange (ETDEWEB)
Williams, Steven M.; Ashbaugh, Henry S., E-mail: hanka@tulane.edu [Department of Chemical and Biomolecular Engineering, Tulane University, New Orleans, Louisiana 70118 (United States)
2014-01-07
The impact of attractive interactions on the partial molar volumes of methane-like solutes in water is characterized using molecular simulations. Attractions account for a significant 20% volume drop between a repulsive Weeks-Chandler-Andersen and full Lennard-Jones description of methane interactions. The response of the volume to interaction perturbations is characterized by linear fits to our simulations and a rigorous statistical thermodynamic expression for the derivative of the volume to increasing attractions. While a weak non-linear response is observed, an average effective slope accurately captures the volume decrease. This response, however, is anticipated to become more non-linear with increasing solute size.
Geysermans, P; Elyeznasni, N; Russier, V
2005-11-22
We present a study of the structure in the interface between two immiscible liquids by density-functional theory and molecular-dynamics calculations. The liquids are modeled by Lennard-Jones potentials, which achieve immiscibility by suppressing the attractive interaction between unlike particles. The density profiles of the liquids display oscillations only in a limited part of the simple liquid-phase diagram (rho,T). When approaching the liquid-vapor coexistence, a significant depletion appears while the layering behavior of the density profile vanishes. By analogy with the liquid-vapor interface and the analysis of the adsorption this behavior is suggested to be strongly related to the drying transition.
DEFF Research Database (Denmark)
Toxværd, Søren
2016-01-01
temperature Ttr.p. crystallizes via a liquid droplet is an example of Ostwald's step rule. The homogeneous nucleation in the supersaturated gas is not to a crystal, but to a liquid-like critical nucleus. We have for the first time performed constant energy (NVE) Molecular Dynamics (MD) of homogeneous...... nucleation without the use of a thermostat. The simulations of homogeneous nucleation in a Lennard-Jones system from supersaturated vapor at temperatures below Ttr.p. reveals that the nucleation to a liquid-like critical nucleus is initiated by a small cold cluster [S. Toxvaerd, J. Chem. Phys. \\textbf{143...
On the sighting of unicorns: A variational approach to computing invariant sets in dynamical systems
Junge, Oliver; Kevrekidis, Ioannis G.
2017-06-01
We propose to compute approximations to invariant sets in dynamical systems by minimizing an appropriate distance between a suitably selected finite set of points and its image under the dynamics. We demonstrate, through computational experiments, that this approach can successfully converge to approximations of (maximal) invariant sets of arbitrary topology, dimension, and stability, such as, e.g., saddle type invariant sets with complicated dynamics. We further propose to extend this approach by adding a Lennard-Jones type potential term to the objective function, which yields more evenly distributed approximating finite point sets, and illustrate the procedure through corresponding numerical experiments.
Recasting a model atomistic glassformer as a system of icosahedra
Energy Technology Data Exchange (ETDEWEB)
Pinney, Rhiannon [HH Wills Physics Laboratory, Tyndall Avenue, Bristol BS8 1TL (United Kingdom); Bristol Centre for Complexity Science, University of Bristol, Bristol BS8 1TS (United Kingdom); Liverpool, Tanniemola B. [School of Mathematics, University of Bristol, Bristol BS8 1TW (United Kingdom); Royall, C. Patrick, E-mail: paddy.royall@bristol.ac.uk [HH Wills Physics Laboratory, Tyndall Avenue, Bristol BS8 1TL (United Kingdom); School of Chemistry, University of Bristol, Cantock Close, Bristol BS8 1TS (United Kingdom); Centre for Nanoscience and Quantum Information, Tyndall Avenue, Bristol BS8 1FD (United Kingdom)
2015-12-28
We consider a binary Lennard-Jones glassformer whose super-Arrhenius dynamics are correlated with the formation of icosahedral structures. Upon cooling, these icosahedra organize into mesoclusters. We recast this glassformer as an effective system of icosahedra which we describe with a population dynamics model. This model we parameterize with data from the temperature regime accessible to molecular dynamics simulations. We then use the model to determine the population of icosahedra in mesoclusters at arbitrary temperature. Using simulation data to incorporate dynamics into the model, we predict relaxation behavior at temperatures inaccessible to conventional approaches. Our model predicts super-Arrhenius dynamics whose relaxation time remains finite for non-zero temperature.
Variation along liquid isomorphs of the driving force for crystallization
DEFF Research Database (Denmark)
Pedersen, Ulf Rørbæk; Adrjanowicz, Karolina; Niss, Kristine
2017-01-01
at a reference temperature. More general analysis allows interpretation of experimental data for molecular liquids such as dimethyl phthalate and indomethacin, and suggests that the isomorph scaling exponent γ in these cases is an increasing function of density, although this cannot be seen in measurements......We investigate the variation of the driving force for crystallization of a supercooled liquid along isomorphs, curves along which structure and dynamics are invariant. The variation is weak, and can be predicted accurately for the Lennard-Jones fluid using a recently developed formalism and data...
Estimating the density-scaling exponent of a monatomic liquid from its pair potential
DEFF Research Database (Denmark)
Bøhling, Lasse; Bailey, Nicholas; Schrøder, Thomas
2014-01-01
This paper investigates two conjectures for calculating the density dependence of the density-scaling exponent γ of a single-component, pair-potential liquid with strong virial potential-energy correlations. The first conjecture gives an analytical expression for γ directly in terms of the pair...... potential. The second conjecture is a refined version of this involving the most likely nearest-neighbor distance determined from the pair-correlation function. The conjectures are tested by simulations of three systems, one of which is the standard Lennard-Jones liquid. While both expressions give...
Role of attractive forces in determining the equilibrium structure and dynamics of simple liquids
DEFF Research Database (Denmark)
Toxværd, Søren
2015-01-01
Molecular Dynamics simulations of a Lennard-Jones system with different range of attraction show that the attractive forces modify the radial distribution of the particles. For condensed liquids only, the forces within the the first coordination shell (FCS) are important, but for gases and moderate...... condensed fluids, even the attractive forces outside the FCS play a role. The changes in the distribution caused by neglecting the attractive forces, lead to a too high pressure. The weak long-range attractions damp the dynamics and the diffusion of the particles in gas-, super critical fluid- and in liquid...
Computer simulation of the thermal pressure in solids and the equation of state
International Nuclear Information System (INIS)
Welch, D.O.; Dienes, G.J.; Paskin, A.
1976-01-01
The equation of state of solids was investigated with molecular dynamics techniques by obtaining the pressure as a function of temperature over a wide range of compressions. Data were obtained for fcc crystals with Lennard--Jones interactions and for bcc crystals with Morse interactions. The results were analyzed in terms of the Mie--Gruneisen equation of state. The Gruneisen constant at zero temperature is found to be essentially that obtained from the volume dependence of the mean-squared lattice vibration frequency, and its temperature dependence can be approximated well with a self-consistent cell model. Calculated results are compared with experimental data for argon along the melting line
Communication: Simple liquids' high-density viscosity.
Costigliola, Lorenzo; Pedersen, Ulf R; Heyes, David M; Schrøder, Thomas B; Dyre, Jeppe C
2018-02-28
This paper argues that the viscosity of simple fluids at densities above that of the triple point is a specific function of temperature relative to the freezing temperature at the density in question. The proposed viscosity expression, which is arrived at in part by reference to the isomorph theory of systems with hidden scale invariance, describes computer simulations of the Lennard-Jones system as well as argon and methane experimental data and simulation results for an effective-pair-potential model of liquid sodium.
Thermodynamical Properties of the Solidified Rare Gases
Energy Technology Data Exchange (ETDEWEB)
Ebbsjoe, I
1971-12-15
Lattice parameter, isothermal bulk modulus and specific heat at constant volume are calculated from Helmholtz free energy for solid Ne, Ar, Kr and Xe. The lattice potential energy is expanded to the fourth order in the nuclear displacements. A perturbation treatment in the quasi harmonic approximation of the partition function includes the cubic anharmonic term to second order and the quartic to first order. Detailed numerical calculations are presented for two interatomic pair potentials, the Lennard-Jones (12,6) and the (exp,a,6). The three nearest neighbours have been taken into account. It is shown that earlier nearest neighbour calculations exaggerate the breakdown of the theory at higher temperatures
Identifying Structural Flow Defects in Disordered Solids Using Machine-Learning Methods
Cubuk, E. D.; Schoenholz, S. S.; Rieser, J. M.; Malone, B. D.; Rottler, J.; Durian, D. J.; Kaxiras, E.; Liu, A. J.
2015-03-01
We use machine-learning methods on local structure to identify flow defects—or particles susceptible to rearrangement—in jammed and glassy systems. We apply this method successfully to two very different systems: a two-dimensional experimental realization of a granular pillar under compression and a Lennard-Jones glass in both two and three dimensions above and below its glass transition temperature. We also identify characteristics of flow defects that differentiate them from the rest of the sample. Our results show it is possible to discern subtle structural features responsible for heterogeneous dynamics observed across a broad range of disordered materials.
Oscillations of spherical fullerenes interacting with graphene sheet
Energy Technology Data Exchange (ETDEWEB)
Ghavanloo, Esmaeal, E-mail: ghavanloo@shirazu.ac.ir; Fazelzadeh, S. Ahmad
2017-01-01
In the present study, the oscillations of spherical fullerenes in the vicinity of a fully constrained graphene sheet are investigated. Using the continuous approximation and Lennard-Jones potential, the van der Waals (vdW) potential energy and interaction forces are obtained. The equation of motion is derived and directly solved based on the actual force distribution between the fullerene molecules and the graphene sheet. Numerical results are obtained and shown that the oscillation is sensitive to the size of the fullerene as well as the distance between the center of the fullerene and the graphene sheet.
Cluster structures influenced by interaction with a surface.
Witt, Christopher; Dieterich, Johannes M; Hartke, Bernd
2018-05-30
Clusters on surfaces are vitally important for nanotechnological applications. Clearly, cluster-surface interactions heavily influence the preferred cluster structures, compared to clusters in vacuum. Nevertheless, systematic explorations and an in-depth understanding of these interactions and how they determine the cluster structures are still lacking. Here we present an extension of our well-established non-deterministic global optimization package OGOLEM from isolated clusters to clusters on surfaces. Applying this approach to intentionally simple Lennard-Jones test systems, we produce a first systematic exploration that relates changes in cluster-surface interactions to resulting changes in adsorbed cluster structures.
Markov state modeling and dynamical coarse-graining via discrete relaxation path sampling.
Fačkovec, B; Vanden-Eijnden, E; Wales, D J
2015-07-28
A method is derived to coarse-grain the dynamics of complex molecular systems to a Markov jump process (MJP) describing how the system jumps between cells that fully partition its state space. The main inputs are relaxation times for each pair of cells, which are shown to be robust with respect to positioning of the cell boundaries. These relaxation times can be calculated via molecular dynamics simulations performed in each cell separately and are used in an efficient estimator for the rate matrix of the MJP. The method is illustrated through applications to Sinai billiards and a cluster of Lennard-Jones discs.
2011-03-01
have been developed ranging from measuring surface details to modifying surface structures . This chapter focuses on aspects of AFM modeling the- ory and...how far apart they are. An example of a poten- tial function is the Lennard-Jones potential, which is also called the 6-12 potential. It can be...γ1 + γ2 + γ12, (31) where γ1 and γ2 are the surface energies of the two adhering spheres, and γ12 is the interfacial energy between the two spheres
Note: Modification of the Gay-Berne potential for improved accuracy and speed
Persson, Rasmus A. X.
2012-06-01
A modification of the Gay-Berne (GB) potential is proposed which is about 10% to 20% more speed efficient and statistically more accurate in reproducing the energy of interaction of two linear Lennard-Jones tetratomics when averaged over all orientations. For the special cases of end-to-end and side-by-side configurations, the new potential is equivalent to the GB one. A simple generalization to dissimilar particles of D∞h symmetry is presented but does not retain the superior agreement with respect to its GB counterpart, except at close range.
International Nuclear Information System (INIS)
Vallee, O.; Ranson, P.; Chapelle, J.
1977-01-01
AI line broadening was studied from collisions between neutral argon atoms (3p 5 4p-3p 5 4s transitions) in a weakly ionised plasma jet (neutral atoms temperature T 0 approximately 4000K, electrons temperature Tsub(e) approximately 6000K, electronic density Nsub(e) 15 cm -3 , ionisation rate α -4 , and pressure range from 1 to 3 kg/cm 2 ). A satisfactory description of Van der Waals broadened lines is obtained by means of a Lennard-Jones potential. Measurement of line widths whose corresponding transitions occur on resonant levels, gives with relatively good accuracy the oscillator strength of the argon resonance lines [fr
International Nuclear Information System (INIS)
Neimark, Alexander V; Ravikovitch, Peter I; Vishnyakov, Aleksey
2003-01-01
With the example of the capillary condensation of Lennard-Jones fluid in nanopores ranging from 1 to 10 nm, we show that the non-local density functional theory (NLDFT) with properly chosen parameters of intermolecular interactions bridges the scale gap from molecular simulations to macroscopic thermodynamics. On the one hand, NLDFT correctly approximates the results of Monte Carlo simulations (shift of vapour-liquid equilibrium, spinodals, density profiles, adsorption isotherms) for pores wider than about 2 nm. On the other hand, NLDFT smoothly merges (above 7-10 nm) with the Derjaguin-Broekhoff-de Boer equations which represent augmented Laplace-Kelvin equations of capillary condensation and desorption
Capillary condensation in pores with rough walls: a density functional approach.
Bryk, P; Rzysko, W; Malijevsky, Al; Sokołowski, S
2007-09-01
The effect of surface roughness of slit-like pore walls on the capillary condensation of a spherical particles and short chains is studied. The gas molecules interact with the substrate by a Lennard-Jones (9,3) potential. The rough layer at each pore wall has a variable thickness and density and consists of a disordered quenched matrix of spherical particles. The system is described in the framework of a density functional approach and using computer simulations. The contribution due to attractive van der Waals interactions between adsorbate molecules is described by using first-order mean spherical approximation and mean-field approximation.
Modulation of capillary condensation by trace component
Directory of Open Access Journals (Sweden)
Shiqi Zhou
2011-06-01
Full Text Available Impact of trace component on capillary condensation (CC is investigated systematically using a classical density functional theory. It is discovered that (i presence of the trace component makes the CC to occur at much lower condensation pressure than when its absence; (ii Lennard-Jones potential parameters like size parameter and energy parameter of the trace component, and its concentration in the bulk adsorption system, show their effects the most remarkably within a particular range beyond which the effects eventually become insignificant. The present discoveries have implications in low pressure storage of gases, separation and enrichment of low concentration component, and easy control of CC transition, etc.
Similarity Laws for the Lines of Ideal Free Energy and Chemical Potential in Supercritical Fluids.
Apfelbaum, E M; Vorob'ev, V S
2017-09-21
We have found the curves on the density-temperature plane, along which the values of free energy and chemical potential correspond to ideal gas quantities. At first, we have applied the van der Waals equation to construct them and to derive their equations. Then we have shown that the same lines for real substances (Ar, N 2 , CH 4 , SF 6 , H 2 , H 2 O) and for the model Lennard-Jones system constructed on the basis of the measurements data and calculations are well matched with the derived equations. The validity and deviations from the obtained similarity laws are discussed.
Analysis of bound-state spectra near the threshold of neutral particle interaction potentials
International Nuclear Information System (INIS)
Ou Fang; Cao Zhuangqi; Chen Jianping; Xu Junjie
2006-01-01
It is understood that conventional semiclassical approximations deteriorate towards threshold in a typical neutral particle interaction potential which is important for the study of ultra-cold atoms and molecules. In this Letter we give an example of the Lennard-Jones potential with tuning of the strength parameter on the basis of the analytical transfer matrix (ATM) method. Highly accurate quantum mechanical results, such as number of the bound states, energy level density and the eigenvalues with extremely low energies have been derived
Microscopic theory of warm ionized gases: equation of state and kinetic Schottky anomaly
International Nuclear Information System (INIS)
Capolupo, A; Giampaolo, S M; Illuminati, F
2013-01-01
Based on accurate Lennard-Jones type interaction potentials, we derive a closed set of state equations for the description of warm atomic gases in the presence of ionization processes. The specific heat is predicted to exhibit peaks in correspondence to single and multiple ionizations. Such kinetic analogue in atomic gases of the Schottky anomaly in solids is enhanced at intermediate and low atomic densities. The case of adiabatic compression of noble gases is analyzed in detail and the implications on sonoluminescence are discussed.
Experimental studies of the NaRb ground-state potential up to the v''=76 level
International Nuclear Information System (INIS)
Docenko, O.; Nikolayeva, O.; Tamanis, M.; Ferber, R.; Pazyuk, E.A.; Stolyarov, A.V.
2002-01-01
Laser induced fluorescence spectra of the C 1 Σ + -X 1 Σ + system of 23 Na 85 Rb and 23 Na 87 Rb have allowed vibrational levels of the electronic ground state up to v '' =76, spanning 99.85% of the potential well to be observed. The ground-state term values have been fitted to a Dunham polynomial expansion, and also to a direct modified Lennard-Jones (MLJ) potential. The analytical MLJ construction allowed us to match previous measured term values for v '' ≤30 with long-range behavior of the potential through the intermediate internuclear distance region covered by the present investigation
Theoretical Assessment of Compressibility Factor of Gases by Using Second Virial Coefficient
Mamedov, Bahtiyar A.; Somuncu, Elif; Askerov, Iskender M.
2018-01-01
We present a new analytical approximation for determining the compressibility factor of real gases at various temperature values. This algorithm is suitable for the accurate evaluation of the compressibility factor using the second virial coefficient with a Lennard-Jones (12-6) potential. Numerical examples are presented for the gases H2, N2, He, CO2, CH4 and air, and the results are compared with other studies in the literature. Our results showed good agreement with the data in the literature. The consistency of the results demonstrates the effectiveness of our analytical approximation for real gases.
Cluster growing process and a sequence of magic numbers
DEFF Research Database (Denmark)
Solov'yov, Ilia; Solov'yov, Andrey V.; Greiner, Walter
2003-01-01
demonstrate that in this way all known global minimum structures of the Lennard-Jones (LJ) clusters can be found. Our method provides an efficient tool for the calculation and analysis of atomic cluster structure. With its use we justify the magic number sequence for the clusters of noble gas atoms......We present a new theoretical framework for modeling the cluster growing process. Starting from the initial tetrahedral cluster configuration, adding new atoms to the system, and absorbing its energy at each step, we find cluster growing paths up to the cluster sizes of more than 100 atoms. We...
International Nuclear Information System (INIS)
Lamb, W.E. Jr.
1978-07-01
The molecule SF 6 is treated as a classical dynamical system obeying Newton's laws of motion. This report describes how the current SF 6 potential is determined. The initial approach is described in terms of a pair of Lennard--Jones potential functions with arbitrary coefficients. A method for determining the potential constants is developed. The SF 6 spectrum was reproduced by including three-body forces. By specifying certain parameters such as the 1/r 6 F-F constant and the total dissociation energy of the molecule, a satisfactory global potential was obtained. The laser-molecule interaction energy was developed
Feasibility of a single-parameter description of equilibrium viscous liquid dynamics
DEFF Research Database (Denmark)
Pedersen, Ulf Rørbæk; Christensen, Tage Emil; Schrøder, Thomas
2008-01-01
Molecular dynamics results for the dynamic Prigogine-Defay ratio are presented for two glass-forming liquids, thus evaluating the experimentally relevant quantity for testing whether metastable-equilibrium liquid dynamics is described by a single parameter to a good approximation. For the Kob......-Andersen binary Lennard-Jones mixture as well as for an asymmetric dumbbell model liquid, a single-parameter description works quite well. This is confirmed by time-domain results where it is found that energy and pressure fluctuations are strongly correlated on the alpha time scale in the constant...
International Nuclear Information System (INIS)
Brooks, R.; Porter, R.A.R.; Kalos, F.; Grosser, A.E.
1975-01-01
A velocity selected molecular beam of D 2 O was crossed with a nozzle beam of Ar and the angular distribution of the scattered D 2 O was measured mass spectrometrically. By varying the velocity of the D 2 O beam, the differential cross section was measured at two collision energies. The experimental results were compared with synthetic differential cross sections calculated from Lennard-Jones and Kihara-Stockmayer trial potentials to determine potential parameters. Implications for the H 2 O pair potential are discussed
Density scaling and quasiuniversality of flow-event statistics for athermal plastic flows
DEFF Research Database (Denmark)
Lerner, Edan; Bailey, Nicholas; Dyre, J. C.
2014-01-01
Athermal steady-state plastic flows were simulated for the Kob-Andersen binary Lennard-Jones system and its repulsive version in which the sign of the attractive terms is changed to a plus. Properties evaluated include the distributions of energy drops, stress drops, and strain intervals between...... the flow events. We show that simulations at a single density in conjunction with an equilibrium-liquid simulation at the same density allow one to predict the plastic flow-event statistics at other densities. This is done by applying the recently established “hidden scale invariance” of simple liquids...
Chaotic dynamics in dense fluids
International Nuclear Information System (INIS)
Posch, H.A.; Hoover, W.G.
1987-09-01
We present calculations of the full spectra of Lyapunov exponents for 8- and 32-particle systems with periodic boundary conditions and interacting with the repulsive part of a Lennard-Jones potential both in equilibrium and nonequilibrium steady states. Lyapunov characteristic exponents λ/sub n/ describe the mean exponential rates of divergence and convergence of neighbouring trajectories in phase-space. They are useful in characterizing the stochastic properties of a dynamical system. A new algorithm for their calculation is presented which incorporates ideas from control theory and constraint nonequilibrium molecular dynamics. 4 refs., 1 fig
A new shared-memory programming paradigm for molecular dynamics simulations on the Intel Paragon
International Nuclear Information System (INIS)
D'Azevedo, E.F.; Romine, C.H.
1994-12-01
This report describes the use of shared memory emulation with DOLIB (Distributed Object Library) to simplify parallel programming on the Intel Paragon. A molecular dynamics application is used as an example to illustrate the use of the DOLIB shared memory library. SOTON-PAR, a parallel molecular dynamics code with explicit message-passing using a Lennard-Jones 6-12 potential, is rewritten using DOLIB primitives. The resulting code has no explicit message primitives and resembles a serial code. The new code can perform dynamic load balancing and achieves better performance than the original parallel code with explicit message-passing
Um modelo para a superfície líquida no estudo da dinâmica do espalhamento de Xe e Ne pelo esqualano
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Leal Alexandre S.
2004-01-01
Full Text Available In this work we present a theoretical model to investigate the scattering of Xe and Ne by a liquid squalane surface. The liquid surface is modeled as a grid of harmonic oscillators with frequencies adjusted to experimental vibration as frequencies of the liquid squalane and the atom-surface interaction potential is modeled by a Lennard-Jones function. The three dimensional description of the dynamics of the process which occurs at the gas-liquid interface is obtained by the classical trajectory method. The general characteristics of the dynamics of the scattering process are in good agreement with experimental data.
Complexity, rate of energy exchanges and stochasticity
International Nuclear Information System (INIS)
Casartelli, M.; Sello, S.
1987-01-01
The complexity of trajectories in the phase of anharmonic crystal (mostly a Lennard-Jones chain) is analysed by the variance of microcanonical density and by new parameters P and chi defined, respectively, as the mean value of the time averages and the relative variance of the absolute exchange rate of energies among the normal modes. Evidence is given to the trapping action of residual invariant surfaces in low stochastic regime of motion. The parameter chi, moreover, proves efficient in exploring the border of stochasticity. A simple power law for P vs. the specific energy is obtained and proved to be independent of stochasticity and of the type of anharmonic potential
She, Zimin; Ghosh, Debasis; Pope, Michael A
2017-10-24
A major stumbling block in the development of high energy density graphene-based supercapacitors has been maintaining high ion-accessible surface area combined with high electrode density. Herein, we develop an ionic liquid (IL)-surfactant microemulsion system that is found to facilitate the spontaneous adsorption of IL-filled micelles onto graphene oxide (GO). This adsorption distributes the IL over all available surface area and provides an aqueous formulation that can be slurry cast onto current collectors, leaving behind a dense nanocomposite film of GO/IL/surfactant. By removing the surfactant and reducing the GO through a low-temperature (360 °C) heat treatment, the IL plays a dual role of spacer and electrolyte. We study the effect of IL content and operating temperature on the performance, demonstrating a record high gravimetric capacitance (302 F/g at 1 A/g) for 80 wt % IL composites. At 60 wt % IL, combined high capacitance and bulk density (0.76 g/cm 3 ), yields one of the highest volumetric capacitances (218 F/cm 3 , at 1 A/g) ever reported for a high-voltage IL-based supercapacitor. While achieving promising rate performance and cycle-life, the approach also eliminates the long and costly electrolyte imbibition step of cell assembly as the electrolyte is cast directly with the electrode material.
2013-09-01
Isolated Ion- Pair 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide Emmanuel I. Obi†, Christopher M. Leavitt†, Paul L. Raston... Christopher P. Moradi†, Steven D. Flynn†, Jerry A. Boatz§,*, Steven D. Chambreau‡,* and Gary E. Douberly†,* †Department of Chemistry, University of...Windus, T. L.; Dupuis , M.; Montgomery, J. A. General Atomic and Molecular Electronic-Structure System. J. Comput. Chem. 1993, 14, 1347-1363
A study on the contact angles of a water droplet on smooth and rough solid surfaces
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Park, Ju Young; Ha, Man Yeong; Choi, Ho Jin; Hong, Seung Do; Yoon, Hyun Sik
2011-01-01
We investigated the wetting characteristics such as contact angle, wetting radius and topography of water droplets on smooth and random solid surfaces. Molecular dynamic simulation is employed to analyze the wetting behavior of water droplets on smooth and rough surfaces by considering different potential energy models of bond, angle, Lennard-Jones and Coulomb to calculate the interacting forces between water molecules. The Lennard-Jones potential energy model is adopted as an interaction model between water molecules and solid surface atoms. The randomly rough surface is generated by changing the standard deviation of roughness height from 1 A to 3 A with the fixed autocorrelation length. The size of water droplet considered is in the range from 2,000 to 5,000 molecules. The contact angles increase generally with increasing number of water molecules. For a hydrophobic surface whose characteristic energy is 0.1 kcal/mol, the contact angles depend rarely on the standard deviation of the roughness height. However, when the surface energy is 0.5 and 1.0 kcal/mol, the contact angles depend on both the roughness height of surfaces and droplet size
Combination Rules for Morse-Based van der Waals Force Fields.
Yang, Li; Sun, Lei; Deng, Wei-Qiao
2018-02-15
In traditional force fields (FFs), van der Waals interactions have been usually described by the Lennard-Jones potentials. Conventional combination rules for the parameters of van der Waals (VDW) cross-termed interactions were developed for the Lennard-Jones based FFs. Here, we report that the Morse potentials were a better function to describe VDW interactions calculated by highly precise quantum mechanics methods. A new set of combination rules was developed for Morse-based FFs, in which VDW interactions were described by Morse potentials. The new set of combination rules has been verified by comparing the second virial coefficients of 11 noble gas mixtures. For all of the mixed binaries considered in this work, the combination rules work very well and are superior to all three other existing sets of combination rules reported in the literature. We further used the Morse-based FF by using the combination rules to simulate the adsorption isotherms of CH 4 at 298 K in four covalent-organic frameworks (COFs). The overall agreement is great, which supports the further applications of this new set of combination rules in more realistic simulation systems.
Heat conduction in diatomic chains with correlated disorder
Savin, Alexander V.; Zolotarevskiy, Vadim; Gendelman, Oleg V.
2017-01-01
The paper considers heat transport in diatomic one-dimensional lattices, containing equal amounts of particles with different masses. Ordering of the particles in the chain is governed by single correlation parameter - the probability for two neighboring particles to have the same mass. As this parameter grows from zero to unity, the structure of the chain varies from regular staggering chain to completely random configuration, and then - to very long clusters of particles with equal masses. Therefore, this correlation parameter allows a control of typical cluster size in the chain. In order to explore different regimes of the heat transport, two interatomic potentials are considered. The first one is an infinite potential wall, corresponding to instantaneous elastic collisions between the neighboring particles. In homogeneous chains such interaction leads to an anomalous heat transport. The other one is classical Lennard-Jones interatomic potential, which leads to a normal heat transport. The simulations demonstrate that the correlated disorder of the particle arrangement does not change the convergence properties of the heat conduction coefficient, but essentially modifies its value. For the collision potential, one observes essential growth of the coefficient for fixed chain length as the limit of large homogeneous clusters is approached. The thermal transport in these models remains superdiffusive. In the Lennard-Jones chain the effect of correlation appears to be not monotonous in the limit of low temperatures. This behavior stems from the competition between formation of long clusters mentioned above, and Anderson localization close to the staggering ordered state.
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Wu, Xia; Wu, Genhua
2014-01-01
Highlights: • A high efficient method for optimization of atomic clusters is developed. • Its performance is studied by optimizing Lennard-Jones clusters and Ag clusters. • The method is proved to be quite efficient. • A new Ag 61 cluster with stacking-fault face-centered cubic motif is found. - Abstract: Geometrical optimization of atomic clusters is performed by a development of adaptive immune optimization algorithm (AIOA) with dynamic lattice searching (DLS) operation (AIOA-DLS method). By a cycle of construction and searching of the dynamic lattice (DL), DLS algorithm rapidly makes the clusters more regular and greatly reduces the potential energy. DLS can thus be used as an operation acting on the new individuals after mutation operation in AIOA to improve the performance of the AIOA. The AIOA-DLS method combines the merit of evolutionary algorithm and idea of dynamic lattice. The performance of the proposed method is investigated in the optimization of Lennard-Jones clusters within 250 atoms and silver clusters described by many-body Gupta potential within 150 atoms. Results reported in the literature are reproduced, and the motif of Ag 61 cluster is found to be stacking-fault face-centered cubic, whose energy is lower than that of previously obtained icosahedron
Yuhara, Daisuke; Brumby, Paul E.; Wu, David T.; Sum, Amadeu K.; Yasuoka, Kenji
2018-05-01
To develop prediction methods of three-phase equilibrium (coexistence) conditions of methane hydrate by molecular simulations, we examined the use of NVT (isometric-isothermal) molecular dynamics (MD) simulations. NVT MD simulations of coexisting solid hydrate, liquid water, and vapor methane phases were performed at four different temperatures, namely, 285, 290, 295, and 300 K. NVT simulations do not require complex pressure control schemes in multi-phase systems, and the growth or dissociation of the hydrate phase can lead to significant pressure changes in the approach toward equilibrium conditions. We found that the calculated equilibrium pressures tended to be higher than those reported by previous NPT (isobaric-isothermal) simulation studies using the same water model. The deviations of equilibrium conditions from previous simulation studies are mainly attributable to the employed calculation methods of pressure and Lennard-Jones interactions. We monitored the pressure in the methane phase, far from the interfaces with other phases, and confirmed that it was higher than the total pressure of the system calculated by previous studies. This fact clearly highlights the difficulties associated with the pressure calculation and control for multi-phase systems. The treatment of Lennard-Jones interactions without tail corrections in MD simulations also contributes to the overestimation of equilibrium pressure. Although improvements are still required to obtain accurate equilibrium conditions, NVT MD simulations exhibit potential for the prediction of equilibrium conditions of multi-phase systems.
Comparison of potentials for polymeric liquids
International Nuclear Information System (INIS)
Jung, Hae Young
2002-01-01
Many theories for polymeric liquids are based on the concepts of cell, hole, free volume of lattice etc. In this theories, van der Waals potential, Lennard-Jones 6-12 potential and their modified potentials are commonly used. In this work, Mie(p,6)potential was applied to the Continuous Lattice Fluid Theory (which extends the discrete lattices of Lattice Fluid Theory to classically continuous lattices) and Dee-Walsch's Cell Theory (which modifies Flory's Equation of State Theory). Both of them are known to be successful theories for polymeric liquids. Thus, PVT values changing with p (the exponent in the repulsion potential) were calculated and compared with experimental values. And, calculated values of Lattice Fluid theory, Flory's Equation of State Theory and Cho-Sanchez Theory using perturbation method were also compared. Through the calculated results, van der Waals potential, Lennard-Jones 6-12 potential and Mie(p,6) potential for polymeric liquids were compared with each other
The thermodynamic properties of normal liquid helium 3
Modarres, M.; Moshfegh, H. R.
2009-09-01
The thermodynamic properties of normal liquid helium 3 are calculated by using the lowest order constrained variational (LOCV) method. The Landau Fermi liquid model and Fermi-Dirac distribution function are considered as our statistical model for the uncorrelated quantum fluid picture and the Lennard-Jones and Aziz potentials are used in our truncated cluster expansion (LOCV) to calculate the correlated energy. The single particle energy is treated variationally through an effective mass. The free energy, pressure, entropy, chemical potential and liquid phase diagram as well as the helium 3 specific heat are evaluated, discussed and compared with the corresponding available experimental data. It is found that the critical temperature for the existence of the pure gas phase is about 4.90 K (4.45 K), which is higher than the experimental prediction of 3.3 K, and the helium 3 flashing temperature is around 0.61 K (0.50 K) for the Lennard-Jones (Aziz) potential.
The importance of accurate interaction potentials in the melting of argon nanoclusters
Pahl, E.; Calvo, F.; Schwerdtfeger, P.
The melting temperatures of argon clusters ArN (N = 13, 55, 147, 309, 561, and 923) and of bulk argon have been obtained from exchange Monte Carlo simulations and are compared using different two-body interaction potentials, namely the standard Lennard-Jones (LJ), Aziz and extended Lennard-Jones (ELJ) potentials. The latter potential has many advantages: while maintaining the computational efficiency of the commonly used LJ potential, it is as accurate as the Aziz potential but the computer time scales more favorably with increasing cluster size. By applying the ELJ form and extrapolating the cluster data to the infinite system, we are able to extract the melting point of argon already in good agreement with experimental measurements. By considering the additional Axilrod-Teller three-body contribution as well, we calculate a melting temperature of T meltELJ = 84.7 K compared to the experimental value of T meltexp = 83.85 K, whereas the LJ potential underestimates the melting point by more than 7 K. Thus melting temperatures within 1 K accuracy are now feasible.
Termodinâmica estatística de líquidos com o método de Monte Carlo. II. O líquido clorofórmio
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Barlette Vania Elisabeth
1999-01-01
Full Text Available Thermodynamic properties and radial distribution functions for liquid chloroform were calculated using the Monte Carlo method implemented with Metropolis algorithm in the NpT ensemble at 298 K and 1 atm. A five site model was developed to represent the chloroform molecules. A force field composed by Lennard-Jones and Coulomb potential functions was used to calculate the intermolecular energy. The partial charges needed to represent the Coulombic interactions were obtained from quantum chemical ab initio calculations. The Lennard-Jones parameters were adjusted to reproduce experimental values for density and enthalpy of vaporization for pure liquid. All thermodynamic results are in excelent agreement with experimental data. The correlation functions calculated are in good accordance with theoretical results avaliable in the literature. The free energy for solvating one chloroform molecule into its own liquid at 298 K and 1 atm was computed as an additional test of the potential model. The result obtained compares well with the experimental value. The medium effects on cis/trans convertion of a hypotetical solute in water TIP4P and chloroform solvents were also accomplished. The results obtained from this investigation are in agreement with estimates of the continuous theory of solvation.
Evolution of short range order in Ar: Liquid to glass and solid transitions-A computational study
Shor, Stanislav; Yahel, Eyal; Makov, Guy
2018-04-01
The evolution of the short range order (SRO) as a function of temperature in a Lennard-Jones model liquid with Ar parameters was determined and juxtaposed with thermodynamic and kinetic properties obtained as the liquid was cooled (heated) and transformed between crystalline solid or glassy states and an undercooled liquid. The Lennard-Jones system was studied by non-equilibrium molecular dynamics simulations of large supercells (approximately 20000 atoms) rapidly cooled or heated at selected quenching rates and at constant pressure. The liquid to solid transition was identified by discontinuities in the atomic volume and molar enthalpy; the glass transition temperature range was identified from the temperature dependence of the self-diffusion. The SRO was studied within the quasi-crystalline model (QCM) framework and compared with the Steinhardt bond order parameters. Within the QCM it was found that the SRO evolves from a bcc-like order in the liquid through a bct-like short range order (c/a=1.2) in the supercooled liquid which persists into the glass and finally to a fcc-like ordering in the crystalline solid. The variation of the SRO that results from the QCM compares well with that obtained with Steinhardt's bond order parameters. The hypothesis of icosahedral order in liquids and glasses is not supported by our results.
A simple extrapolation of thermodynamic perturbation theory to infinite order
International Nuclear Information System (INIS)
Ghobadi, Ahmadreza F.; Elliott, J. Richard
2015-01-01
Recent analyses of the third and fourth order perturbation contributions to the equations of state for square well spheres and Lennard-Jones chains show trends that persist across orders and molecular models. In particular, the ratio between orders (e.g., A 3 /A 2 , where A i is the ith order perturbation contribution) exhibits a peak when plotted with respect to density. The trend resembles a Gaussian curve with the peak near the critical density. This observation can form the basis for a simple recursion and extrapolation from the highest available order to infinite order. The resulting extrapolation is analytic and therefore cannot fully characterize the critical region, but it remarkably improves accuracy, especially for the binodal curve. Whereas a second order theory is typically accurate for the binodal at temperatures within 90% of the critical temperature, the extrapolated result is accurate to within 99% of the critical temperature. In addition to square well spheres and Lennard-Jones chains, we demonstrate how the method can be applied semi-empirically to the Perturbed Chain - Statistical Associating Fluid Theory (PC-SAFT)
Divergence of activity expansions: Is it actually a problem?
Ushcats, M. V.; Bulavin, L. A.; Sysoev, V. M.; Ushcats, S. Yu.
2017-12-01
For realistic interaction models, which include both molecular attraction and repulsion (e.g., Lennard-Jones, modified Lennard-Jones, Morse, and square-well potentials), the asymptotic behavior of the virial expansions for pressure and density in powers of activity has been studied taking power terms of high orders into account on the basis of the known finite-order irreducible integrals as well as the recent approximations of infinite irreducible series. Even in the divergence region (at subcritical temperatures), this behavior stays thermodynamically adequate (in contrast to the behavior of the virial equation of state with the same set of irreducible integrals) and corresponds to the beginning of the first-order phase transition: the divergence yields the jump (discontinuity) in density at constant pressure and chemical potential. In general, it provides a statistical explanation of the condensation phenomenon, but for liquid or solid states, the physically proper description (which can turn the infinite discontinuity into a finite jump of density) still needs further study of high-order cluster integrals and, especially, their real dependence on the system volume (density).
Solvation in atomic liquids: connection between Gaussian field theory and density functional theory
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V. Sergiievskyi
2017-12-01
Full Text Available For the problem of molecular solvation, formulated as a liquid submitted to the external potential field created by a molecular solute of arbitrary shape dissolved in that solvent, we draw a connection between the Gaussian field theory derived by David Chandler [Phys. Rev. E, 1993, 48, 2898] and classical density functional theory. We show that Chandler's results concerning the solvation of a hard core of arbitrary shape can be recovered by either minimising a linearised HNC functional using an auxiliary Lagrange multiplier field to impose a vanishing density inside the core, or by minimising this functional directly outside the core — indeed a simpler procedure. Those equivalent approaches are compared to two other variants of DFT, either in the HNC, or partially linearised HNC approximation, for the solvation of a Lennard-Jones solute of increasing size in a Lennard-Jones solvent. Compared to Monte-Carlo simulations, all those theories give acceptable results for the inhomogeneous solvent structure, but are completely out-of-range for the solvation free-energies. This can be fixed in DFT by adding a hard-sphere bridge correction to the HNC functional.
Quantum complex rotation and uniform semiclassical calculations of complex energy eigenvalues
International Nuclear Information System (INIS)
Connor, J.N.L.; Smith, A.D.
1983-01-01
Quantum and semiclassical calculations of complex energy eigenvalues have been carried out for an exponential potential of the form V 0 r 2 exp(-r) and Lennard-Jones (12,6) potential. A straightforward method, based on the complex coordinate rotation technique, is described for the quantum calculation of complex eigenenergies. For singular potentials, the method involves an inward and outward integration of the radial Schroedinger equation, followed by matching of the logarithmic derivatives of the wave functions at an intermediate point. For regular potentials, the method is simpler, as only an inward integration is required. Attention is drawn to the World War II researches of Hartree and co-workers who anticipated later quantum mechanical work on the complex rotation method. Complex eigenenergies are also calculated from a uniform semiclassical three turning point quantization formula, which allows for the proximity of the outer pair of complex turning points. Limiting cases of this formula, which are valid for very narrow or very broad widths, are also used in the calculations. We obtain good agreement between the semiclassical and quantum results. For the Lennard-Jones (12,6) potential, we compare resonance energies and widths from the complex energy definition of a resonance with those obtained from the time delay definition
International Nuclear Information System (INIS)
Schwarzer, N
2014-01-01
In order to understand the principle differences between rheological or simple stress tests like the uniaxial tensile test to contact mechanical tests and the differences between quasistatic contact experiments and oscillatory ones, this study resorts to effective first principles. This study will show how relatively simple models simulating bond interactions in solids using effective potentials like Lennard-Jones and Morse can be used to investigate the effect of time dependent stress-induced softening or stiffening of these solids. The usefulness of the current study is in the possibility of deriving relatively simple dependences of the bulk-modulus B on time, shear and pressure P with time t. In cases where it is possible to describe, or at least partially describe a material by Lennard-Jones potential approaches, the above- mentioned dependences are even completely free of microscopic material parameters. Instead of bond energies and length, only specific integral parameters like Young’s modulus and Poisson’s ratio are required. However, in the case of time dependent (viscose) material behavior the parameters are not constants anymore. They themselves depend on time and the actual stress field, especially the shear field. A body completely consisting of so called standard linear solid interacting particles will then phenomenologically show a completely different and usually much more complicated mechanical behavior. The influence of the time dependent pressure-shear-induced Young’s modulus change is discussed with respect to mechanical contact experiments and their analysis in the case of viscose materials. (papers)
Test of a new heat-flow equation for dense-fluid shock waves.
Holian, Brad Lee; Mareschal, Michel; Ravelo, Ramon
2010-09-21
Using a recently proposed equation for the heat-flux vector that goes beyond Fourier's Law of heat conduction, we model shockwave propagation in the dense Lennard-Jones fluid. Disequilibrium among the three components of temperature, namely, the difference between the kinetic temperature in the direction of a planar shock wave and those in the transverse directions, particularly in the region near the shock front, gives rise to a new transport (equilibration) mechanism not seen in usual one-dimensional heat-flow situations. The modification of the heat-flow equation was tested earlier for the case of strong shock waves in the ideal gas, which had been studied in the past and compared to Navier-Stokes-Fourier solutions. Now, the Lennard-Jones fluid, whose equation of state and transport properties have been determined from independent calculations, allows us to study the case where potential, as well as kinetic contributions are important. The new heat-flow treatment improves the agreement with nonequilibrium molecular-dynamics simulations under strong shock wave conditions, compared to Navier-Stokes.
Energy Technology Data Exchange (ETDEWEB)
Kadoura, Ahmad; Sun, Shuyu, E-mail: shuyu.sun@kaust.edu.sa; Salama, Amgad
2014-08-01
Accurate determination of thermodynamic properties of petroleum reservoir fluids is of great interest to many applications, especially in petroleum engineering and chemical engineering. Molecular simulation has many appealing features, especially its requirement of fewer tuned parameters but yet better predicting capability; however it is well known that molecular simulation is very CPU expensive, as compared to equation of state approaches. We have recently introduced an efficient thermodynamically consistent technique to regenerate rapidly Monte Carlo Markov Chains (MCMCs) at different thermodynamic conditions from the existing data points that have been pre-computed with expensive classical simulation. This technique can speed up the simulation more than a million times, making the regenerated molecular simulation almost as fast as equation of state approaches. In this paper, this technique is first briefly reviewed and then numerically investigated in its capability of predicting ensemble averages of primary quantities at different neighboring thermodynamic conditions to the original simulated MCMCs. Moreover, this extrapolation technique is extended to predict second derivative properties (e.g. heat capacity and fluid compressibility). The method works by reweighting and reconstructing generated MCMCs in canonical ensemble for Lennard-Jones particles. In this paper, system's potential energy, pressure, isochoric heat capacity and isothermal compressibility along isochors, isotherms and paths of changing temperature and density from the original simulated points were extrapolated. Finally, an optimized set of Lennard-Jones parameters (ε, σ) for single site models were proposed for methane, nitrogen and carbon monoxide.
Instantaneous, parameter-free methods to define a solute’s hydration shell
International Nuclear Information System (INIS)
Chatterjee, Anupam; Higham, Jonathan; Henchman, Richard H.
2015-01-01
A range of methods are presented to calculate a solute’s hydration shell from computer simulations of dilute solutions of monatomic ions and noble gas atoms. The methods are designed to be parameter-free and instantaneous so as to make them more general, accurate, and consequently applicable to disordered systems. One method is a modified nearest-neighbor method, another considers solute-water Lennard-Jones overlap followed by hydrogen-bond rearrangement, while three methods compare various combinations of water-solute and water-water forces. The methods are tested on a series of monatomic ions and solutes and compared with the values from cutoffs in the radial distribution function, the nearest-neighbor distribution functions, and the strongest-acceptor hydrogen bond definition for anions. The Lennard-Jones overlap method and one of the force-comparison methods are found to give a hydration shell for cations which is in reasonable agreement with that using a cutoff in the radial distribution function. Further modifications would be required, though, to make them capture the neighboring water molecules of noble-gas solutes if these weakly interacting molecules are considered to constitute the hydration shell
Carbon nanotori as traps for atoms and ions
International Nuclear Information System (INIS)
Chan Yue; Cox, Barry J.; Hill, James M.
2012-01-01
Carbon nanotori surely represent an ideal location to trap both charged and uncharged atoms, since they are open, accessible and possess strong attractive energy. In this paper, we investigate the plausibility of carbon nanotori as atomic traps and we use the continuum approximation together with the Lennard-Jones potential to model the encapsulation of an atom or ion by a nanotorus. The critical geometric factors such as the minor and major radii, i.e. r and R of the nanotorus, for which the maximum interaction between the atom and the nanotorus occurs, are determined. For various atoms, assumed situated along the axis of the torus, the minimum potential energy between the atom and the nanotorus is calculated and compared, and shown to be approximately kηεσ 2 , where η is the uniform atomic density, ε and σ are the Lennard-Jones well depth and the van der Waals radius, respectively, and k is a universal non-dimensional constant with the approximate value -12.42. The results given in this paper might be used for future drug delivery and biosensing design.
Simplicity of condensed matter at its core: generic definition of a Roskilde-simple system.
Schrøder, Thomas B; Dyre, Jeppe C
2014-11-28
The isomorph theory is reformulated by defining Roskilde-simple systems by the property that the order of the potential energies of configurations at one density is maintained when these are scaled uniformly to a different density. If the potential energy as a function of all particle coordinates is denoted by U(R), this requirement translates into U(Ra) < U(Rb) ⇒ U(λRa) < U(λRb). Isomorphs remain curves in the thermodynamic phase diagram along which structure, dynamics, and excess entropy are invariant, implying that the phase diagram is effectively one-dimensional with respect to many reduced-unit properties. In contrast to the original formulation of the isomorph theory, however, the density-scaling exponent is not exclusively a function of density and the isochoric heat capacity is not an exact isomorph invariant. A prediction is given for the latter quantity's variation along the isomorphs. Molecular dynamics simulations of the Lennard-Jones and Lennard-Jones Gaussian systems validate the new approach.
Energy Technology Data Exchange (ETDEWEB)
Mokhtari, B.; Enayati, M. [Iranian Offshore Oil Co., Tehran (Iran, Islamic Republic of); Heidaryan, E. [Islamic Azad Univ., Tehran (Iran, Islamic Republic of). Masjidosolayman Branch
2008-07-01
Theoretical methods show that crystalline hydrates can form from single-phase systems consisting of both vapor water with gaseous hydrate former and liquid water with dissolved hydrate former. Two phase systems consist of both liquid water with gaseous hydrate former and with liquid hydrate former on the surface. This paper presented a Langmuir constant related model for the prediction of equilibrium pressures and cage occupancies of pure component hydrates. Intermolecular potentials were fit to quantum mechanical energies to obtain the Langmuir constants, which differed from the procedure utilized with the vdWP model. The paper described the experimental method and model calculations. This included the Fugacity model and Van der Waals and Platteeuw model. The paper also discussed pair potential of non-spherical molecules, including the multicentre (site-site) potential; Gaussian overlap potential; Lennard-Jones potential; and Kihara generalized pair potential. It was concluded that fraction of occupied cavities is a function of pair potentials between hard core and empty hydrate lattice. These pair potentials could be calculated from some model as Kihara cell potential, Gaussian potential, Lennard-Jones potential and multicentre pair potential. 49 refs., 3 figs.
O'Keeffe, C J; Ren, Ruichao; Orkoulas, G
2007-11-21
Spatial updating grand canonical Monte Carlo algorithms are generalizations of random and sequential updating algorithms for lattice systems to continuum fluid models. The elementary steps, insertions or removals, are constructed by generating points in space either at random (random updating) or in a prescribed order (sequential updating). These algorithms have previously been developed only for systems of impenetrable spheres for which no particle overlap occurs. In this work, spatial updating grand canonical algorithms are generalized to continuous, soft-core potentials to account for overlapping configurations. Results on two- and three-dimensional Lennard-Jones fluids indicate that spatial updating grand canonical algorithms, both random and sequential, converge faster than standard grand canonical algorithms. Spatial algorithms based on sequential updating not only exhibit the fastest convergence but also are ideal for parallel implementation due to the absence of strict detailed balance and the nature of the updating that minimizes interprocessor communication. Parallel simulation results for three-dimensional Lennard-Jones fluids show a substantial reduction of simulation time for systems of moderate and large size. The efficiency improvement by parallel processing through domain decomposition is always in addition to the efficiency improvement by sequential updating.
Okumura, Hisashi
2011-01-07
The partial multicanonical algorithm for molecular dynamics and Monte Carlo simulations samples a wide range of an important part of the potential energy. Although it is a strong technique for structure prediction of biomolecules, the choice of the partial potential energy has not been optimized. In order to find the best choice, partial multicanonical molecular dynamics simulations of an alanine dipeptide in explicit water solvent were performed with 15 trial choices for the partial potential energy. The best choice was found to be the sum of the electrostatic, Lennard-Jones, and torsion-angle potential energies between solute atoms. In this case, the partial multicanonical simulation sampled all of the local-minimum free-energy states of the P(II), C(5), α(R), α(P), α(L), and C states and visited these states most frequently. Furthermore, backbone dihedral angles ϕ and ψ rotated very well. It is also found that the most important term among these three terms is the electrostatic potential energy and that the Lennard-Jones term also helps the simulation to overcome the steric restrictions. On the other hand, multicanonical simulation sampled all of the six states, but visited these states fewer times. Conventional canonical simulation sampled only four of the six states: The P(II), C(5), α(R), and α(P) states.
Droplet spreading driven by van der Waals force: a molecular dynamics study
Wu, Congmin
2010-07-07
The dynamics of droplet spreading is investigated by molecular dynamics simulations for two immiscible fluids of equal density and viscosity. All the molecular interactions are modeled by truncated Lennard-Jones potentials and a long-range van der Waals force is introduced to act on the wetting fluid. By gradually increasing the coupling constant in the attractive van der Waals interaction between the wetting fluid and the substrate, we observe a transition in the initial stage of spreading. There exists a critical value of the coupling constant, above which the spreading is pioneered by a precursor film. In particular, the dynamically determined critical value quantitatively agrees with that determined by the energy criterion that the spreading coefficient equals zero. The latter separates partial wetting from complete wetting. In the regime of complete wetting, the radius of the spreading droplet varies with time as R(t) ∼ √t, a behavior also found in molecular dynamics simulations where the wetting dynamics is driven by the short-range Lennard-Jones interaction between liquid and solid. © 2010 IOP Publishing Ltd.
Slepoy, A; Peters, M D; Thompson, A P
2007-11-30
Molecular dynamics and other molecular simulation methods rely on a potential energy function, based only on the relative coordinates of the atomic nuclei. Such a function, called a force field, approximately represents the electronic structure interactions of a condensed matter system. Developing such approximate functions and fitting their parameters remains an arduous, time-consuming process, relying on expert physical intuition. To address this problem, a functional programming methodology was developed that may enable automated discovery of entirely new force-field functional forms, while simultaneously fitting parameter values. The method uses a combination of genetic programming, Metropolis Monte Carlo importance sampling and parallel tempering, to efficiently search a large space of candidate functional forms and parameters. The methodology was tested using a nontrivial problem with a well-defined globally optimal solution: a small set of atomic configurations was generated and the energy of each configuration was calculated using the Lennard-Jones pair potential. Starting with a population of random functions, our fully automated, massively parallel implementation of the method reproducibly discovered the original Lennard-Jones pair potential by searching for several hours on 100 processors, sampling only a minuscule portion of the total search space. This result indicates that, with further improvement, the method may be suitable for unsupervised development of more accurate force fields with completely new functional forms. Copyright (c) 2007 Wiley Periodicals, Inc.
International Nuclear Information System (INIS)
Koudriavtsev, A.B.; Linert, W.
2005-01-01
Parameters of the formalism [1-6] describing spin crossover in the solid state have been defined via molecular potentials in model systems of neutral and ionic complexes. In the first instance Lennard-Jones and electric dipole-dipole potentials have been used whereas in ionic systems Lennard-Jones and electric point-charge potentials have been used. Electric dipole-dipole interaction of neutral complexes brings about a positive excess energy controlled by the difference of electric dipole moments of HS and LS molecules. Differences of the order of Δμ = 1-2D cause an abrupt spin crossover in systems with T 1/2 = 100-150K. Magnetic coupling contributes both to the excess energy and excess entropy, however the overall effect is equivalent to a modest positive excess energy. Ionic systems in the absence of specific interactions are characterized by very small excess energies corresponding to practically linear van't Hoff plots. Detectable positive and negative excess energies in these systems may arise from interactions of ligands belonging to neighbouring complexes. The HOMO-LUMO overlap in HS-LS pairs can bring about a nontrivial variation of the shape of transition curves. Examples of regression analysis of experimental transition curves in terms of molecular potentials are given. (author)
Solid phase stability of a double-minimum interaction potential system
International Nuclear Information System (INIS)
Suematsu, Ayumi; Yoshimori, Akira; Saiki, Masafumi; Matsui, Jun; Odagaki, Takashi
2014-01-01
We study phase stability of a system with double-minimum interaction potential in a wide range of parameters by a thermodynamic perturbation theory. The present double-minimum potential is the Lennard-Jones-Gauss potential, which has a Gaussian pocket as well as a standard Lennard-Jones minimum. As a function of the depth and position of the Gaussian pocket in the potential, we determine the coexistence pressure of crystals (fcc and bcc). We show that the fcc crystallizes even at zero pressure when the position of the Gaussian pocket is coincident with the first or third nearest neighbor site of the fcc crystal. The bcc crystal is more stable than the fcc crystal when the position of the Gaussian pocket is coincident with the second nearest neighbor sites of the bcc crystal. The stable crystal structure is determined by the position of the Gaussian pocket. These results show that we can control the stability of the solid phase by tuning the potential function
Kadoura, Ahmad Salim
2014-08-01
Accurate determination of thermodynamic properties of petroleum reservoir fluids is of great interest to many applications, especially in petroleum engineering and chemical engineering. Molecular simulation has many appealing features, especially its requirement of fewer tuned parameters but yet better predicting capability; however it is well known that molecular simulation is very CPU expensive, as compared to equation of state approaches. We have recently introduced an efficient thermodynamically consistent technique to regenerate rapidly Monte Carlo Markov Chains (MCMCs) at different thermodynamic conditions from the existing data points that have been pre-computed with expensive classical simulation. This technique can speed up the simulation more than a million times, making the regenerated molecular simulation almost as fast as equation of state approaches. In this paper, this technique is first briefly reviewed and then numerically investigated in its capability of predicting ensemble averages of primary quantities at different neighboring thermodynamic conditions to the original simulated MCMCs. Moreover, this extrapolation technique is extended to predict second derivative properties (e.g. heat capacity and fluid compressibility). The method works by reweighting and reconstructing generated MCMCs in canonical ensemble for Lennard-Jones particles. In this paper, system\\'s potential energy, pressure, isochoric heat capacity and isothermal compressibility along isochors, isotherms and paths of changing temperature and density from the original simulated points were extrapolated. Finally, an optimized set of Lennard-Jones parameters (ε, σ) for single site models were proposed for methane, nitrogen and carbon monoxide. © 2014 Elsevier Inc.
Yuhara, Daisuke; Brumby, Paul E; Wu, David T; Sum, Amadeu K; Yasuoka, Kenji
2018-05-14
To develop prediction methods of three-phase equilibrium (coexistence) conditions of methane hydrate by molecular simulations, we examined the use of NVT (isometric-isothermal) molecular dynamics (MD) simulations. NVT MD simulations of coexisting solid hydrate, liquid water, and vapor methane phases were performed at four different temperatures, namely, 285, 290, 295, and 300 K. NVT simulations do not require complex pressure control schemes in multi-phase systems, and the growth or dissociation of the hydrate phase can lead to significant pressure changes in the approach toward equilibrium conditions. We found that the calculated equilibrium pressures tended to be higher than those reported by previous NPT (isobaric-isothermal) simulation studies using the same water model. The deviations of equilibrium conditions from previous simulation studies are mainly attributable to the employed calculation methods of pressure and Lennard-Jones interactions. We monitored the pressure in the methane phase, far from the interfaces with other phases, and confirmed that it was higher than the total pressure of the system calculated by previous studies. This fact clearly highlights the difficulties associated with the pressure calculation and control for multi-phase systems. The treatment of Lennard-Jones interactions without tail corrections in MD simulations also contributes to the overestimation of equilibrium pressure. Although improvements are still required to obtain accurate equilibrium conditions, NVT MD simulations exhibit potential for the prediction of equilibrium conditions of multi-phase systems.
African Journal of Health Professions Education - Vol 9, No 4 (2017)
African Journals Online (AJOL)
Research: Self-leadership traits of academics to conform to a changing highereducation environment · EMAIL FREE FULL TEXT EMAIL FREE FULL TEXT DOWNLOAD FULL TEXT DOWNLOAD FULL TEXT. K. Jooste, J. Frantz, 199-202 ...
effects of antilymphocyte serum on hyperacute renal rejection in goats
African Journals Online (AJOL)
1971-04-17
Apr 17, 1971 ... SoMARJE V. JOOSTE, Life Sciences Division, Atomic Energy Board, Pretoria. SUMMARY ... and is more in accord with the 'blindfolding' theory than any other. ... used could provide evidence on whether ALS can act on the.
The motivational needs of primary health care nurses to acquire ...
African Journals Online (AJOL)
Karien Jooste
for a significant part of service delivery in the health system. Professional nurses' .... motivational needs of PHC nurses to acquire power in the workplace at mine clinic .... recognition through rewards and status (Jooste, 2009, p. 165). 10.1.1.
Longhurst, M. J.; Quirke, N.
2006-11-01
We have previously shown that the upshift in the radial breathing mode (RBM) of closed (or infinite) carbon nanotubes in solution is almost entirely due to coupling of the RBM with an adsorbed layer of fluid on the nanotube surface. The upshift can be modeled analytically by considering the adsorbed fluid as an infinitesimally thin shell, which interacts with the nanotube via a continuum Lennard-Jones potential. Here we extend the model to include internally as well as externally adsorbed waterlike molecules, and find that filling the nanotubes leads to an additional upshift of two to six wave numbers. We show that using molecular dynamics, the RBM can be accurately reproduced by replacing the fluid molecules with a mean field harmonic shell potential, greatly reducing simulation times.
NVU dynamics. I. Geodesic motion on the constant-potential-energy hypersurface
DEFF Research Database (Denmark)
Ingebrigtsen, Trond; Toxværd, Søren; Heilmann, Ole
2011-01-01
that ensures potential-energy and step-length conservation; center-of-mass drift is also eliminated. Analytical arguments confirmed by simulations demonstrate that the modified NVU algorithm is absolutely stable. Finally, we present simulations showing that the NVU algorithm and the standard leap-frog NVE......An algorithm is derived for computer simulation of geodesics on the constant-potential-energy hypersurface of a system of N classical particles. First, a basic time-reversible geodesic algorithm is derived by discretizing the geodesic stationarity condition and implementing the constant......-potential-energy constraint via standard Lagrangian multipliers. The basic NVU algorithm is tested by single-precision computer simulations of the Lennard-Jones liquid. Excellent numerical stability is obtained if the force cutoff is smoothed and the two initial configurations have identical potential energy within machine...
Molecular dynamics investigation of tracer diffusion in a simple liquid
International Nuclear Information System (INIS)
Ould-Kaddour, F.; Barrat, J.L.
1991-05-01
Extensive Molecular-Dynamics (MD) simulations have been carried out for a model trace-solvent system made up of 100 solvent molecules and 8 tracer molecules interacting through truncated Lennard-Jones potentials. The influence of the size ratio between solute and solvent, of their mass ratio and of the solvent viscosity on the diffusivity of a small tracer were investigated. Positive deviations from a Stokes-Einstein behaviour are observed, in qualitative agreement with experimental observations. It was also observed that as tracer and solvent become increasingly dissimilar, their respective dynamics becomes decoupled. We suggest that such decouplings can be interpreted by writing their mobility of the tracer as the sum of two terms, the first one arising from a coupling between tracer dynamics and hydrodynamics modes of the solvent, and the second one describing jump motion in a locally nearly frozen environment. (author). 17 refs, 4 figs, 6 tabs
The effect of normal load on polytetrafluoroethylene tribology.
Barry, Peter R; Chiu, Patrick Y; Perry, Scott S; Sawyer, W Gregory; Phillpot, Simon R; Sinnott, Susan B
2009-04-08
The tribological behavior of oriented poly(tetrafluoroethylene) (PTFE) sliding surfaces is examined as a function of sliding direction and applied normal load in classical molecular dynamics (MD) simulations. The forces are calculated with the second-generation reactive empirical bond-order potential for short-range interactions, and with a Lennard-Jones potential for long-range interactions. The range of applied normal loads considered is 5-30 nN. The displacement of interfacial atoms from their initial positions during sliding is found to vary by a factor of seven, depending on the relative orientation of the sliding chains. However, within each sliding configuration the magnitude of the interfacial atomic displacements exhibits little dependence on load over the range considered. The predicted friction coefficients are also found to vary with chain orientation and are in excellent quantitative agreement with experimental measurements.
International Nuclear Information System (INIS)
Fang, T.-H.; Chang, W.-J.; Lin, S.-L.
2006-01-01
This paper uses molecular dynamics simulation based on the Lennard-Jones potential to study the effects that temperature and velocity have on, the nanojet droplet ejection process, when the droplet is ejected at an angle onto a moving plate's surface. According to the analysis, it was found that the width of the spreading droplet increased as the temperature and the time were increased. Also found was an energy wave phenomenon. The contact angle of the droplet deposited on the plate decreased as the temperature was increased. Furthermore, the layer phenomena became apparent when the atoms were deposited on a moving plate. Thinner film layers were obtained as the velocity of the moving plate was increased. The contact angle on the left side of the droplet was larger than that on the right side when the plate was moving from right to left
Molecular dynamics of contact behavior of self-assembled monolayers on gold using nanoindentation
Energy Technology Data Exchange (ETDEWEB)
Fang, Te-Hua [Institute of Mechanical and Electromechanical Engineering National Formosa University, Yunlin 632, Taiwan (China); Chang, Win-Jin, E-mail: changwj@mail.ksu.edu.tw [Department of Mechanical Engineering Kun Shan University, Tainan 710, Taiwan (China); Fan, Yu-Cheng [Institute of Mechanical and Electromechanical Engineering National Formosa University, Yunlin 632, Taiwan (China); Weng, Cheng-I [Department of Mechanical Engineering National Cheng Kung University, Tainan, 710, Taiwan (China)
2009-08-15
Molecular dynamics simulation is used to study nanoindentation of the self-assembled monolayers (SAMs) on an Au surface. The interaction of SAM atoms is described by a general universal force field (UFF), the tight-binding second-moment approximation (TB-SMA) is used for Au substrate, and the Lennard-Jones potential function is employed to describe interaction among the indenter, the SAMs, and the Au substrate atoms. The model consists of a planar Au substrate with n-hexadecanethiol SAM chemisorbed to the substrate. The simulation results show that the contact pressure increases as the SAMs temperature increases. In addition, the contact pressure also increases as the depth and velocity of indentation increase.
Molecular dynamics of contact behavior of self-assembled monolayers on gold using nanoindentation
International Nuclear Information System (INIS)
Fang, Te-Hua; Chang, Win-Jin; Fan, Yu-Cheng; Weng, Cheng-I
2009-01-01
Molecular dynamics simulation is used to study nanoindentation of the self-assembled monolayers (SAMs) on an Au surface. The interaction of SAM atoms is described by a general universal force field (UFF), the tight-binding second-moment approximation (TB-SMA) is used for Au substrate, and the Lennard-Jones potential function is employed to describe interaction among the indenter, the SAMs, and the Au substrate atoms. The model consists of a planar Au substrate with n-hexadecanethiol SAM chemisorbed to the substrate. The simulation results show that the contact pressure increases as the SAMs temperature increases. In addition, the contact pressure also increases as the depth and velocity of indentation increase.
Cantilever-based sensing: the origin of surface stress and optimization strategies
International Nuclear Information System (INIS)
Godin, Michel; Tabard-Cossa, Vincent; Miyahara, Yoichi; Grutter, Peter; Monga, Tanya; Bruce Lennox, R; Williams, P J; Beaulieu, L Y
2010-01-01
Many interactions drive the adsorption of molecules on surfaces, all of which can result in a measurable change in surface stress. This article compares the contributions of various possible interactions to the overall induced surface stress for cantilever-based sensing applications. The surface stress resulting from adsorption-induced changes in the electronic density of the underlying surface is up to 2-4 orders of magnitude larger than that resulting from intermolecular electrostatic or Lennard-Jones interactions. We reveal that the surface stress associated with the formation of high quality alkanethiol self-assembled monolayers on gold surfaces is independent of the molecular chain length, supporting our theoretical findings. This provides a foundation for the development of new strategies for increasing the sensitivity of cantilever-based sensors for various applications.
A dynamic lattice searching method with rotation operation for optimization of large clusters
International Nuclear Information System (INIS)
Wu Xia; Cai Wensheng; Shao Xueguang
2009-01-01
Global optimization of large clusters has been a difficult task, though much effort has been paid and many efficient methods have been proposed. During our works, a rotation operation (RO) is designed to realize the structural transformation from decahedra to icosahedra for the optimization of large clusters, by rotating the atoms below the center atom with a definite degree around the fivefold axis. Based on the RO, a development of the previous dynamic lattice searching with constructed core (DLSc), named as DLSc-RO, is presented. With an investigation of the method for the optimization of Lennard-Jones (LJ) clusters, i.e., LJ 500 , LJ 561 , LJ 600 , LJ 665-667 , LJ 670 , LJ 685 , and LJ 923 , Morse clusters, silver clusters by Gupta potential, and aluminum clusters by NP-B potential, it was found that both the global minima with icosahedral and decahedral motifs can be obtained, and the method is proved to be efficient and universal.
Numerical investigation of elastic mechanical properties of graphene structures
International Nuclear Information System (INIS)
Georgantzinos, S.K.; Giannopoulos, G.I.; Anifantis, N.K.
2010-01-01
The computation of the elastic mechanical properties of graphene sheets, nanoribbons and graphite flakes using spring based finite element models is the aim of this paper. Interatomic bonded interactions as well as van der Waals forces between carbon atoms are simulated via the use of appropriate spring elements expressing corresponding potential energies provided by molecular theory. Each layer is idealized as a spring-like structure with carbon atoms represented by nodes while interatomic forces are simulated by translational and torsional springs with linear behavior. The non-bonded van der Waals interactions among atoms which are responsible for keeping the graphene layers together are simulated with the Lennard-Jones potential using appropriate spring elements. Numerical results concerning the Young's modulus, shear modulus and Poisson's ratio for graphene structures are derived in terms of their chilarity, width, length and number of layers. The numerical results from finite element simulations show good agreement with existing numerical values in the open literature.
Gas Permeation Characteristics across Nano-Porous Inorganic Membranes
Directory of Open Access Journals (Sweden)
M.R Othman, H. Mukhtar
2012-10-01
Full Text Available An overview of parameters affecting gas permeation in inorganic membranes is presented. These factors include membrane physical characteristics, operational parameters and gas molecular characteristics. The membrane physical characteristics include membrane materials and surface area, porosity, pore size and pore size distribution and membrane morphology. The operational parameters include feed flow rate and concentration, stage cut, temperature and pressure. The gas molecular characteristics include gas molecular weight, diameter, critical temperature, critical pressure, Lennard-Jones parameters and diffusion volumes. The current techniques of material characterization may require complementary method in describing microscopic heterogeneity of the porous ceramic media. The method to be incorporated in the future will be to apply a stochastic model and/or fractal dimension. Keywords: Inorganic membrane, surface adsorption, Knudsen diffusion, Micro-porous membrane, permeation, gas separation.
Pinney, Rhiannon; Liverpool, Tanniemola B; Royall, C Patrick
2016-12-21
We consider a binary Lennard-Jones glassformer whose super-Arrhenius dynamics are correlated with the formation of particles organized into icosahedra under simple steady state shear. We recast this glassformer as an effective system of icosahedra [Pinney et al., J. Chem. Phys. 143, 244507 (2015)]. From the observed population of icosahedra in each steady state, we obtain an effective temperature which is linearly dependent on the shear rate in the range considered. Upon shear banding, the system separates into a region of high shear rate and a region of low shear rate. The effective temperatures obtained in each case show that the low shear regions correspond to a significantly lower temperature than the high shear regions. Taking a weighted average of the effective temperature of these regions (weight determined by region size) yields an estimate of the effective temperature which compares well with an effective temperature based on the global mesocluster population of the whole system.
Diffusion in Coulomb crystals.
Hughto, J; Schneider, A S; Horowitz, C J; Berry, D K
2011-07-01
Diffusion in Coulomb crystals can be important for the structure of neutron star crusts. We determine diffusion constants D from molecular dynamics simulations. We find that D for Coulomb crystals with relatively soft-core 1/r interactions may be larger than D for Lennard-Jones or other solids with harder-core interactions. Diffusion, for simulations of nearly perfect body-centered-cubic lattices, involves the exchange of ions in ringlike configurations. Here ions "hop" in unison without the formation of long lived vacancies. Diffusion, for imperfect crystals, involves the motion of defects. Finally, we find that diffusion, for an amorphous system rapidly quenched from Coulomb parameter Γ=175 to Coulomb parameters up to Γ=1750, is fast enough that the system starts to crystalize during long simulation runs. These results strongly suggest that Coulomb solids in cold white dwarf stars, and the crust of neutron stars, will be crystalline and not amorphous.
Local elastic properties of nano-confined fluids: A density functional study
Energy Technology Data Exchange (ETDEWEB)
Sun, Zongli, E-mail: zongli_sun@163.com [Science and Technology College, North China Electric Power University, Baoding 071051 (China); Kang, Yanshuang [College of Science, Agriculture University of Hebei, Baoding 071001 (China)
2014-05-01
The understanding of mechanical properties of confined fluids is essential for modeling and manipulating of nano-scaled systems. Unlike the uniform phase, the confined fluids usually display different features in structure and related properties. Due to the presence of the confining geometry, the density profile and many physical and chemical properties may be position-dependent. The aim of our research is to derive an expression for the local elastic property by using the classical elastic theory. Both the bulk and shear moduli are expressed as functional of density of particle. The theoretical result derived is applied to the Lennard-Jones fluids confined in nano-cavity. Comparison of our numerical result and the simulation result is made and qualitative agreement is observed. Further, influence of bulk density, temperature and external potential on moduli is calculated and the physical mechanism is analyzed. Relationship between contact modulus and the interfacial tension is also calculated. Their opposite trend with temperature is observed.
Two Universal Equations of State for Solids
Sun, Jiu-Xun; Wu, Qiang; Guo, Yang; Cai, Ling-Cang
2010-01-01
In this paper, two equations of state (EOSs) (Sun Jiu-Xun-Morse with parameters n = 3 and 4, designated by SMS3 and SMS4) with two parameters are proposed to satisfy four merits proposed previously and give improved results for the cohesive energy. By applying ten typical EOSs to fit experimental compression data of 50 materials, it is shown that the SMS4 EOS gives the best results; the Baonza and Morse EOSs give the second best results; the SMS3 and modified generalized Lennard-Jones (mGLJ) EOSs give the third best results. However, the Baonza and mGLJ EOSs cannot give physically reasonable values of cohesive energy and P-V curves in the expansion region; the SMS3 and SMS4 EOS give fairly good results, and have some advantages over the Baonza and mGLJ EOSs in practical applications.
Isoviscosity lines and the liquid-glass transition in simple liquids.
Fomin, Yu D; Brazhkin, V V; Ryzhov, V N
2012-07-01
This article presents the study of the generic behavior of viscosity of liquids based on some simple theoretical models, the soft-spheres and Lennard-Jones systems. The use of these simple models allows us to investigate in detail the viscosity behavior in a wide range of temperatures and pressures including the high-temperature-high-pressure limits. Based on the simulation results, we discuss the shape of isoviscosity lines and analyze the glass transition at high temperatures and high pressures. Despite the fact that the viscosity drastically increases in the limit of high temperatures and high pressures along the melting line, the relaxation time rapidly decreases in this region, and the system becomes further from the glass transition.
Low-temperature behaviour of the Kob-Andersen binary mixture
International Nuclear Information System (INIS)
Ashwin S S; Sastry, Srikanth
2003-01-01
The dynamical behaviours of glass-forming liquids have been analysed extensively via computer simulations of model liquids, among which the Kob-Andersen binary Lennard-Jones mixture has been a widely studied system. Typically, studies of this model have been restricted to temperatures above the mode coupling temperature. Preliminary results concerning the dynamics of the Kob-Andersen binary mixture are presented at temperatures that extend below the mode coupling temperature, along with properties of the local energy minima sampled. These results show that a crossover in the dynamics occurs alongside changes in the properties of the inherent structures sampled. Furthermore, a crossover is observed from non-Arrhenius behaviour of the diffusivity above the mode coupling temperature to Arrhenius behaviour at lower temperatures
Coronene molecules in helium clusters: Quantum and classical studies of energies and configurations
Energy Technology Data Exchange (ETDEWEB)
Rodríguez-Cantano, Rocío; Pérez de Tudela, Ricardo; Bartolomei, Massimiliano; Hernández, Marta I.; Campos-Martínez, José; González-Lezana, Tomás, E-mail: t.gonzalez.lezana@csic.es; Villarreal, Pablo [Instituto de Física Fundamental, IFF-CSIC, Serrano 123, 28006 Madrid (Spain); Hernández-Rojas, Javier; Bretón, José [Departamento de Física and IUdEA, Universidad de La Laguna, 38205 Tenerife (Spain)
2015-12-14
Coronene-doped helium clusters have been studied by means of classical and quantum mechanical (QM) methods using a recently developed He–C{sub 24}H{sub 12} global potential based on the use of optimized atom-bond improved Lennard-Jones functions. Equilibrium energies and geometries at global and local minima for systems with up to 69 He atoms were calculated by means of an evolutive algorithm and a basin-hopping approach and compared with results from path integral Monte Carlo (PIMC) calculations at 2 K. A detailed analysis performed for the smallest sizes shows that the precise localization of the He atoms forming the first solvation layer over the molecular substrate is affected by differences between relative potential minima. The comparison of the PIMC results with the predictions from the classical approaches and with diffusion Monte Carlo results allows to examine the importance of both the QM and thermal effects.
Molecular Dynamics Simulation for the Mechanical Properties of CNT/Polymer Nanocomposites
International Nuclear Information System (INIS)
Yang, Seung Hwa; Cho, Maeg Hyo
2007-01-01
In order to obtain mechanical properties of CNT/Polymer nano-composites, molecular dynamics simulation is performed. Overall system was modeled as a flexible unit cell in which carbon nanotubes are embedded into a polyethylene matrix for N σ T ensemble simulation. COMPASS force field was chosen to describe inter and intra molecular potential and bulk effect was achieved via periodic boundary conditions. In CNT-polymer interface, only Lennard-Jones non-bond potential was considered. Using Parrinello-Rahman fluctuation method, mechanical properties of orthotropic nano-composites under various temperatures were successfully obtained. Also, we investigated thermal behavior of the short CNT reinforced nanocomposites system with predicting glass transition temperature
Coarse graining from variationally enhanced sampling applied to the Ginzburg-Landau model
Invernizzi, Michele; Valsson, Omar; Parrinello, Michele
2017-03-01
A powerful way to deal with a complex system is to build a coarse-grained model capable of catching its main physical features, while being computationally affordable. Inevitably, such coarse-grained models introduce a set of phenomenological parameters, which are often not easily deducible from the underlying atomistic system. We present a unique approach to the calculation of these parameters, based on the recently introduced variationally enhanced sampling method. It allows us to obtain the parameters from atomistic simulations, providing thus a direct connection between the microscopic and the mesoscopic scale. The coarse-grained model we consider is that of Ginzburg-Landau, valid around a second-order critical point. In particular, we use it to describe a Lennard-Jones fluid in the region close to the liquid-vapor critical point. The procedure is general and can be adapted to other coarse-grained models.
A variational approach to nucleation simulation.
Piaggi, Pablo M; Valsson, Omar; Parrinello, Michele
2016-12-22
We study by computer simulation the nucleation of a supersaturated Lennard-Jones vapor into the liquid phase. The large free energy barriers to transition make the time scale of this process impossible to study by ordinary molecular dynamics simulations. Therefore we use a recently developed enhanced sampling method [Valsson and Parrinello, Phys. Rev. Lett.113, 090601 (2014)] based on the variational determination of a bias potential. We differ from previous applications of this method in that the bias is constructed on the basis of the physical model provided by the classical theory of nucleation. We examine the technical problems associated with this approach. Our results are very satisfactory and will pave the way for calculating the nucleation rates in many systems.
Statistical ensembles and molecular dynamics studies of anisotropic solids. II
International Nuclear Information System (INIS)
Ray, J.R.; Rahman, A.
1985-01-01
We have recently discussed how the Parrinello--Rahman theory can be brought into accord with the theory of the elastic and thermodynamic behavior of anisotropic media. This involves the isoenthalpic--isotension ensemble of statistical mechanics. Nose has developed a canonical ensemble form of molecular dynamics. We combine Nose's ideas with the Parrinello--Rahman theory to obtain a canonical form of molecular dynamics appropriate to the study of anisotropic media subjected to arbitrary external stress. We employ this isothermal--isotension ensemble in a study of a fcc→ close-packed structural phase transformation in a Lennard-Jones solid subjected to uniaxial compression. Our interpretation of the Nose theory does not involve a scaling of the time variable. This latter fact leads to simplifications when studying the time dependence of quantities
Exploring the free energy surfaces of clusters using reconnaissance metadynamics
Tribello, Gareth A.; Cuny, Jérôme; Eshet, Hagai; Parrinello, Michele
2011-09-01
A new approach is proposed for exploring the low-energy structures of small to medium-sized aggregates of atoms and molecules. This approach uses the recently proposed reconnaissance metadynamics method [G. A. Tribello, M. Ceriotti, and M. Parrinello. Proc. Natl. Acad. Sci. U.S.A. 107(41), 17509 (2010), 10.1073/pnas.1011511107] in tandem with collective variables that describe the average structure of the coordination sphere around the atoms/molecules. We demonstrate this method on both Lennard-Jones and water clusters and show how it is able to quickly find the global minimum in the potential energy surface, while exploring the finite temperature free energy surface.
Cumulative distribution functions associated with bubble-nucleation processes in cavitation
Watanabe, Hiroshi
2010-11-15
Bubble-nucleation processes of a Lennard-Jones liquid are studied by molecular dynamics simulations. Waiting time, which is the lifetime of a superheated liquid, is determined for several system sizes, and the apparent finite-size effect of the nucleation rate is observed. From the cumulative distribution function of the nucleation events, the bubble-nucleation process is found to be not a simple Poisson process but a Poisson process with an additional relaxation time. The parameters of the exponential distribution associated with the process are determined by taking the relaxation time into account, and the apparent finite-size effect is removed. These results imply that the use of the arithmetic mean of the waiting time until a bubble grows to the critical size leads to an incorrect estimation of the nucleation rate. © 2010 The American Physical Society.
Molecular Dynamics Simulations of a Linear Nanomotor Driven by Thermophoretic Forces
DEFF Research Database (Denmark)
Zambrano, Harvey A; Walther, Jens Honore; Jaffe, Richard L.
Molecular Dynamics of a Linear Nanomotor Driven by Thermophoresis Harvey A. Zambrano1, Jens H. Walther1,2 and Richard L. Jaffe3 1Department of Mechanical Engineering, Fluid Mechanics, Technical University of Denmark, DK-2800 Lyngby, Denmark; 2Computational Science and Engineering Laboratory, ETH...... future molecular machines a complete understanding of the friction forces involved on the transport process at the molecular level have to be addressed.18 In this work we perform Molecular Dynamics (MD) simulations using the MD package FASTTUBE19 to study a molecular linear motor consisting of coaxial...... the valence forces within the CNT using Morse, harmonic angle and torsion potentials.19We include a nonbonded carbon-carbon Lennard-Jones potential to describe the vdW interaction between the carbon atoms within the double wall portion of the system. We equilibrate the system at 300K for 0.1 ns, by coupling...
Molecular simulation of water removal from simple gases with zeolite NaA.
Csányi, Eva; Ható, Zoltán; Kristóf, Tamás
2012-06-01
Water vapor removal from some simple gases using zeolite NaA was studied by molecular simulation. The equilibrium adsorption properties of H(2)O, CO, H(2), CH(4) and their mixtures in dehydrated zeolite NaA were computed by grand canonical Monte Carlo simulations. The simulations employed Lennard-Jones + Coulomb type effective pair potential models, which are suitable for the reproduction of thermodynamic properties of pure substances. Based on the comparison of the simulation results with experimental data for single-component adsorption at different temperatures and pressures, a modified interaction potential model for the zeolite is proposed. In the adsorption simulations with mixtures presented here, zeolite exhibits extremely high selectivity of water to the investigated weakly polar/non-polar gases demonstrating the excellent dehydration ability of zeolite NaA in engineering applications.
Energy Technology Data Exchange (ETDEWEB)
Geysermans, P.; Pontikis, V. [Centre National de la Recherche Scientifique (CNRS), 94 - Vitry-sur-Seine (France). Centre d' Etudes de Chimie Metallurgique
2002-09-01
The atomic structure of the solid-liquid heterophase interface was investigated by using molecular dynamics. Two kinds of systems were studied; the first one was crystalline copper with (100) and (111) surface terminations in contact with liquid aluminium, while in the second one the interface was modelled by two systems in contact made of Lennard-Jones particles with different size ({sigma}) and energy ({epsilon}) parameters. We found that at the interface the liquid was layered whatever the crystallographic orientation of the surface. The layering of the liquid is still preserved when the ratio of particles sites ({chi}={sigma}{sub 1}/{sigma}{sub 2}) changes while an epitaxial relationship is always found between the crystal and the first liquid layer. The average density of the latter is closely related to the {chi} value. (authors)
Application of a non-integer Bessel uniform approximation to inelastic molecular collisions
International Nuclear Information System (INIS)
Connor, J.N.L.; Mayne, H.R.
1979-01-01
A non-integer Bessel uniform approximation has been used to calculate transition probabilities for collinear atom-oscillator collisions. The collision systems used are a harmonic oscillator interacting via a Lennard-Jones potential and a Morse oscillator interacting via an exponential potential. Both classically allowed and classically forbidden transitions have been treated. The order of the Bessel function is chosen by a physical argument that makes use of information contained in the final-action initial-angle plot. Limitations of this procedure are discussed. It is shown that the non-integer Bessel approximation is accurate for elastic 0 → 0 collisions at high collision energies, where the integer Bessel approximation is inaccurate or inapplicable. (author)
Continuum modelling for carbon and boron nitride nanostructures
International Nuclear Information System (INIS)
Thamwattana, Ngamta; Hill, James M
2007-01-01
Continuum based models are presented here for certain boron nitride and carbon nanostructures. In particular, certain fullerene interactions, C 60 -C 60 , B 36 N 36 -B 36 N 36 and C 60 -B 36 N 36 , and fullerene-nanotube oscillator interactions, C 60 -boron nitride nanotube, C 60 -carbon nanotube, B 36 N 36 -boron nitride nanotube and B 36 N 36 -carbon nanotube, are studied using the Lennard-Jones potential and the continuum approach, which assumes a uniform distribution of atoms on the surface of each molecule. Issues regarding the encapsulation of a fullerene into a nanotube are also addressed, including acceptance and suction energies of the fullerenes, preferred position of the fullerenes inside the nanotube and the gigahertz frequency oscillation of the inner molecule inside the outer nanotube. Our primary purpose here is to extend a number of established results for carbon to the boron nitride nanostructures
Long-range interaction of anisotropic systems
Zhang, Junyi
2015-02-01
The first-order electrostatic interaction energy between two far-apart anisotropic atoms depends not only on the distance between them but also on their relative orientation, according to Rayleigh-Schrödinger perturbation theory. Using the first-order interaction energy and the continuum model, we study the long-range interaction between a pair of parallel pristine graphene sheets at zero temperature. The asymptotic form of the obtained potential density, &epsi:(D) &prop: ?D ?3 ?O(D?4), is consistent with the random phase approximation and Lifshitz theory. Accordingly, neglectance of the anisotropy, especially the nonzero first-order interaction energy, is the reason why the widely used Lennard-Jones potential approach and dispersion corrections in density functional theory give a wrong asymptotic form ε(D) &prop: ?D?4. © EPLA, 2015.
Theoretical equation of state for classical fluids. I. Test by perturbation theory
International Nuclear Information System (INIS)
Gil-Villegas, A.; Chavez, M.; Del Rio, F.
1993-01-01
This paper shows how to construct the theoretical equation of state (TEOS) of a classical simple fluid. The theory relies on the mean collisional diameter and range, and maps the thermodynamical properties of the fluid into those of an equivalent square-well (ESW) fluid of appropriate depth ε , diameter σ and range R. It is shown that the ESW has the same pressure as the fluid of interest. Hence the THEOS of any simple fluid takes the form of a SW EOS of the given ε , σ and R. The theory is applied to a Lennard-Jones (LJ) system in a first-order perturbation. The mapping equation have a physical solution for densities where the SW EOS is accurate; the resulting LJ TEOS agrees very well with the results of computer simulations, and compares favorably with the recent TEOS developed by Song and Mason. (Author). 17 refs, 7 figs, 1 tab
Sub- and super-Maxwellian evaporation of simple gases from liquid water
International Nuclear Information System (INIS)
Kann, Z. R.; Skinner, J. L.
2016-01-01
Non-Maxwellian evaporation of light atoms and molecules (particles) such as He and H 2 from liquids has been observed experimentally. In this work, we use simulations to study systematically the evaporation of Lennard-Jones particles from liquid water. We find instances of sub- and super-Maxwellian evaporation, depending on the mass of the particle and the particle-water interaction strength. The observed trends are in qualitative agreement with experiment. We interpret these trends in terms of the potential of mean force and the effectiveness and frequency of collisions during the evaporation process. The angular distribution of evaporating particles is also analyzed, and it is shown that trends in the energy from velocity components tangential and normal to the liquid surface must be understood separately in order to interpret properly the angular distributions.
Sub- and super-Maxwellian evaporation of simple gases from liquid water
Energy Technology Data Exchange (ETDEWEB)
Kann, Z. R.; Skinner, J. L., E-mail: skinner@chem.wisc.edu [Theoretical Chemistry Institute and Department of Chemistry, University of Wisconsin, Madison, Wisconsin 53706 (United States)
2016-04-21
Non-Maxwellian evaporation of light atoms and molecules (particles) such as He and H{sub 2} from liquids has been observed experimentally. In this work, we use simulations to study systematically the evaporation of Lennard-Jones particles from liquid water. We find instances of sub- and super-Maxwellian evaporation, depending on the mass of the particle and the particle-water interaction strength. The observed trends are in qualitative agreement with experiment. We interpret these trends in terms of the potential of mean force and the effectiveness and frequency of collisions during the evaporation process. The angular distribution of evaporating particles is also analyzed, and it is shown that trends in the energy from velocity components tangential and normal to the liquid surface must be understood separately in order to interpret properly the angular distributions.
Classically exact surface diffusion constants at arbitrary temperature
International Nuclear Information System (INIS)
Voter, A.F.; Cohen, J.M.
1989-01-01
An expression is presented for computing the classical diffusion constant of a point defect (e.g., an adatom) in an infinite lattice of binding sites at arbitrary temperature. The transition state theory diffusion constant is simply multiplied by a dynamical correction factor that is computed from short-time classical trajectories initiated at the site boundaries. The time scale limitations of direct molecular dynamics are thus avoided in the low- and middle-temperature regimes. The expression results from taking the time derivative of the particle mean-square displacement in the lattice-discretized coordinate system. Applications are presented for surface diffusion on fcc(100) and fcc(111) Lennard-Jones crystal faces
Bardhan, Jaydeep P; Knepley, Matthew G
2014-10-07
We show that charge-sign-dependent asymmetric hydration can be modeled accurately using linear Poisson theory after replacing the standard electric-displacement boundary condition with a simple nonlinear boundary condition. Using a single multiplicative scaling factor to determine atomic radii from molecular dynamics Lennard-Jones parameters, the new model accurately reproduces MD free-energy calculations of hydration asymmetries for: (i) monatomic ions, (ii) titratable amino acids in both their protonated and unprotonated states, and (iii) the Mobley "bracelet" and "rod" test problems [D. L. Mobley, A. E. Barber II, C. J. Fennell, and K. A. Dill, "Charge asymmetries in hydration of polar solutes," J. Phys. Chem. B 112, 2405-2414 (2008)]. Remarkably, the model also justifies the use of linear response expressions for charging free energies. Our boundary-element method implementation demonstrates the ease with which other continuum-electrostatic solvers can be extended to include asymmetry.
International Nuclear Information System (INIS)
Bardhan, Jaydeep P.; Knepley, Matthew G.
2014-01-01
We show that charge-sign-dependent asymmetric hydration can be modeled accurately using linear Poisson theory after replacing the standard electric-displacement boundary condition with a simple nonlinear boundary condition. Using a single multiplicative scaling factor to determine atomic radii from molecular dynamics Lennard-Jones parameters, the new model accurately reproduces MD free-energy calculations of hydration asymmetries for: (i) monatomic ions, (ii) titratable amino acids in both their protonated and unprotonated states, and (iii) the Mobley “bracelet” and “rod” test problems [D. L. Mobley, A. E. Barber II, C. J. Fennell, and K. A. Dill, “Charge asymmetries in hydration of polar solutes,” J. Phys. Chem. B 112, 2405–2414 (2008)]. Remarkably, the model also justifies the use of linear response expressions for charging free energies. Our boundary-element method implementation demonstrates the ease with which other continuum-electrostatic solvers can be extended to include asymmetry
A general mixture theory. I. Mixtures of spherical molecules
Hamad, Esam Z.
1996-08-01
We present a new general theory for obtaining mixture properties from the pure species equations of state. The theory addresses the composition and the unlike interactions dependence of mixture equation of state. The density expansion of the mixture equation gives the exact composition dependence of all virial coefficients. The theory introduces multiple-index parameters that can be calculated from binary unlike interaction parameters. In this first part of the work, details are presented for the first and second levels of approximations for spherical molecules. The second order model is simple and very accurate. It predicts the compressibility factor of additive hard spheres within simulation uncertainty (equimolar with size ratio of three). For nonadditive hard spheres, comparison with compressibility factor simulation data over a wide range of density, composition, and nonadditivity parameter, gave an average error of 2%. For mixtures of Lennard-Jones molecules, the model predictions are better than the Weeks-Chandler-Anderson perturbation theory.
Membrane methods for separation of radioactive noble gases
International Nuclear Information System (INIS)
Bekman, I.N.; Bozhenko, E.I.; Ievlev, A.L.; Kazankin, Yu.N.; Nikonov, V.N.; Teplyakov, V.V.; Shvyryaev, A.A.
1984-01-01
Using the different ial permeability method at different temperatures (20-120 deg C) transport characteristics of inert gases, N 2 , O 2 , CH 4 , CQ 2 and H 2 as the main components of waste gases in homogeneous films of arylate-siloxane block-copolymer (silar) of different composition, as well as of its components - polydimethylsiloxane (PDMS) and polyarylate, have been measured. Dependences of diffusion and permeability coefficients on inert gas atom dimensions, and solubility coefficient - on strength constant of the Lennard-Jones potential, are analyzed. It is shown that selectivity of silar gas permbility is determined by the properties of siloxane component, and the values of permeability coefficients decrease with the increase of polyarylate block part due to dominating decrease in diffusion coefficients as compared with solubility coefficients
International Nuclear Information System (INIS)
Corti, Giancarlo; Zhan, Yingqian; Wang, Lidong; Hare, Brian; Cantrell, Timothy; II, Miles Beaux; Prakash, Tej; Ytreberg, F Marty; McIlroy, David N; Miller, Michael A
2013-01-01
Silica nanosprings (NSs) consisting of multiple nanowires intertwined were demonstrated to reversibly store 0.85 wt% hydrogen at 20 bar and room temperature. X-ray photoelectron spectroscopy indicates a mixed 3 + –4 + ionization state of the silicon atoms and partially explains the enhanced surface adsorption of H 2 relative to other forms of silica. Theoretical modeling and simulation using a Lennard-Jones potential demonstrated that interstitial sites between the silica nanowires forming the NS are energetically more favorable adsorption sites relative to single nanowires. The addition of Pd nanoparticles to the surface of the silica NSs was demonstrated to increase the hydrogen storage capacity to ≈3.5 wt% at 66 bar and room temperature. Palladium-nanoparticle-induced hydrogen spillover is attributed to the enhanced storage capacity relative to bare silica NSs. (paper)
Si-coated single-walled carbon nanotubes under axial loads: An atomistic simulation study
International Nuclear Information System (INIS)
Song Haiyang; Zha Xinwei
2007-01-01
The mechanical properties of the Si-coated imperfect (5, 5) single-walled carbon nanotube (SWCNT), the imperfect (5, 5) SWCNT and several perfect armchair SWCNTs under axial loads were investigated using molecular dynamics simulation. The interactions between atoms were modeled using the empirical Tersoff potential and the Tersoff-Brenner potential coupled with the Lennard-Jones potential. We get Young's modulus of the defective (5, 5) nanotube with and without the Si coating under axial tension 1107.92 and 1076.02 GPa, respectively. The results also show that the structure failure of the Si-coated imperfect (5, 5) SWCNT under axial compression occurs at a slightly higher strain than for the perfect (5, 5) SWCNT. Therefore, we can confirm the protective effect of Si as a coating material for defective SWCNTs. We also obtain the critical buckling strains of perfect SWCNTs
Stability of molecular dynamics simulations of classical systems
DEFF Research Database (Denmark)
Toxværd, Søren
2012-01-01
The existence of a shadow Hamiltonian for discrete classical dynamics, obtained by an asymptotic expansion for a discrete symplectic algorithm, is employed to determine the limit of stability for molecular dynamics (MD) simulations with respect to the time-increment h of the discrete dynamics....... The investigation is based on the stability of the shadow energy, obtained by including the first term in the asymptotic expansion, and on the exact solution of discrete dynamics for a single harmonic mode. The exact solution of discrete dynamics for a harmonic potential with frequency ω gives a criterion...... for the limit of stability h ⩽ 2/ω. Simulations of the Lennard-Jones system and the viscous Kob-Andersen system show that one can use the limit of stability of the shadow energy or the stability criterion for a harmonic mode on the spectrum of instantaneous frequencies to determine the limit of stability of MD...
Communication: Thermodynamic analysis of critical conditions of polymer adsorption
International Nuclear Information System (INIS)
Cimino, R.; Neimark, A. V.; Rasmussen, C. J.
2013-01-01
Polymer adsorption to solid surfaces is a ubiquitous phenomenon, which has attracted long-lasting attention. Dependent on the competition between the polymer-solid adsorption and polymer-solvent solvation interactions, a chain may assume either 3d solvated conformation when adsorption is weak or 2d adsorbed conformation when adsorption is strong. The transition between these conformations occurring upon variation of adsorption strength is quite sharp, and in the limit of “infinite” chain length, can be treated as a critical phenomenon. We suggest a novel thermodynamic definition of the critical conditions of polymer adsorption from the equality of incremental chemical potentials of adsorbed and free chains. We show with the example of freely jointed Lennard-Jones chains tethered to an adsorbing surface that this new definition provides a link between thermodynamic and geometrical features of adsorbed chains and is in line with classical scaling relationships for the fraction of adsorbed monomers, chain radii of gyration, and free energy
International Nuclear Information System (INIS)
Li Yongqing; Song Peng; Chen Yuehui; Wang Weili; Ma Fengcai
2005-01-01
In our previous theoretical studies [Meng-Tao Sun, Yong-Qing Lee, and Feng-Cai Ma, Chem. Phys. Lett. 371 (2003) 342], we have reported the quantum interference on collision-induced rotational energy transfer on CO (A 1 Π, v = 3) with inert gases, which originates from the difference between the two Λ-related collision potential energy surfaces. The interference angle, which measures the degree of coherence, is presented in this paper. Based on the time-dependent first order Born approximation, taking into account the anisotropic Lennard-Jones interaction potentials, the relation of the interference angle with the factors, including experimental temperature, partner, and rotational quantum number, are obtained. The changing tendencies with them are discussed. This theoretical model is important to understanding and performing this kind of experiment.
Shape matters: The case for Ellipsoids and Ellipsoidal Water
Energy Technology Data Exchange (ETDEWEB)
Tillack, Andreas F. [ORNL; Robinson, Bruce H. [University of Washington, Seattle
2017-11-01
We describe the shape potentials used for the van der Waals interactions between soft-ellipsoids used to coarse-grain molecular moieties in our Metropolis Monte-Carlo simulation software. The morphologies resulting from different expressions for these van der Waals interaction potentials are discussed for the case of a prolate spheroid system with a strong dipole at the ellipsoid center. We also show that the calculation of ellipsoids is, at worst, only about fivefold more expensive computationally when compared to a simple Lennard- Jones sphere. Finally, as an application of the ellipsoidal shape we parametrize water from the original SPC water model and observe – just through the difference in shape alone – a significant improvement of the O-O radial distribution function when compared to experimental data.
Probing heterogeneous dynamics from spatial density correlation in glass-forming liquids.
Li, Yan-Wei; Zhu, You-Liang; Sun, Zhao-Yan
2016-12-01
We numerically investigate the connection between spatial density correlation and dynamical heterogeneity in glass-forming liquids. We demonstrate that the cluster size defined by the spatial aggregation of densely packed particles (DPPs) can better capture the difference between the dynamics of the Lennard-Jones glass model and the Weeks-Chandler-Andersen truncation model than the commonly used pair correlation functions. More interestingly, we compare the mobility of DPPs and loosely packed particles, and we find that high local density correlates well with slow dynamics in systems with relatively hard repulsive interactions but links to mobile ones in the system with soft repulsive interactions at one relaxation time scale. Our results show clear evidence that the above model dependence behavior stems from the hopping motion of DPPs at the end of the caging stage due to the compressive nature of soft repulsive spheres, which activates the dynamics of DPPs in the α relaxation stage.
Interaction energy for a fullerene encapsulated in a carbon nanotorus
Sarapat, Pakhapoom; Baowan, Duangkamon; Hill, James M.
2018-06-01
The interaction energy of a fullerene symmetrically situated inside a carbon nanotorus is studied. For these non-bonded molecules, the main interaction originates from the van der Waals energy which is modelled by the 6-12 Lennard-Jones potential. Upon utilising the continuum approximation which assumes that there are infinitely many atoms that are uniformly distributed over the surfaces of the molecules, the total interaction energy between the two structures is obtained as a surface integral over the spherical and the toroidal surfaces. This analytical energy is employed to determine the most stable configuration of the torus encapsulating the fullerene. The results show that a torus with major radius around 20-22 Å and minor radius greater than 6.31 Å gives rise to the most stable arrangement. This study will pave the way for future developments in biomolecules design and drug delivery system.
Long-range interaction of anisotropic systems
Zhang, Junyi; Schwingenschlö gl, Udo
2015-01-01
The first-order electrostatic interaction energy between two far-apart anisotropic atoms depends not only on the distance between them but also on their relative orientation, according to Rayleigh-Schrödinger perturbation theory. Using the first-order interaction energy and the continuum model, we study the long-range interaction between a pair of parallel pristine graphene sheets at zero temperature. The asymptotic form of the obtained potential density, &epsi:(D) &prop: ?D ?3 ?O(D?4), is consistent with the random phase approximation and Lifshitz theory. Accordingly, neglectance of the anisotropy, especially the nonzero first-order interaction energy, is the reason why the widely used Lennard-Jones potential approach and dispersion corrections in density functional theory give a wrong asymptotic form ε(D) &prop: ?D?4. © EPLA, 2015.
Hatch, Harold W.; Jiao, Sally; Mahynski, Nathan A.; Blanco, Marco A.; Shen, Vincent K.
2017-12-01
Virial coefficients are predicted over a large range of both temperatures and model parameter values (i.e., alchemical transformation) from an individual Mayer-sampling Monte Carlo simulation by statistical mechanical extrapolation with minimal increase in computational cost. With this extrapolation method, a Mayer-sampling Monte Carlo simulation of the SPC/E (extended simple point charge) water model quantitatively predicted the second virial coefficient as a continuous function spanning over four orders of magnitude in value and over three orders of magnitude in temperature with less than a 2% deviation. In addition, the same simulation predicted the second virial coefficient if the site charges were scaled by a constant factor, from an increase of 40% down to zero charge. This method is also shown to perform well for the third virial coefficient and the exponential parameter for a Lennard-Jones fluid.
International Nuclear Information System (INIS)
Matsuyama, M.; Miyake, H.; Ashida, K.; Watanabe, K.
1982-01-01
Tetrafluoroethylene (TFE) is widely used for conventional tritium handling systems such as vacuum seals, tubing and so on. We measured the permeation of the three hydrogen isotopes, methane and the inert gases through a TFE film at room temperature by means of the time-lag method in order to establish the physicochemical properties which determine the solubility and diffusivity of those gases. It was found that the diffusion constant of the inert gases changed exponentially with the heat of vaporization and the solubility was an exponential function of the Lennard-Jones force constant of the gases. On the other hand, hydrogen isotopes and methane deviated from these relations. It is concluded that chemical interactions between the solute and the solvent play an important role for the dissolution and the diffusion of these gases in TFE. (orig.)
DEFF Research Database (Denmark)
Curutchet, Carles; Cupellini, Lorenzo; Kongsted, Jacob
2018-01-01
embedding approaches, respectively, nonelectrostatic dispersion and repulsion interactions are instead commonly described through classical potentials despite their quantum mechanical origin. Here we present an extension of the Tkatchenko-Scheffler semiempirical van der Waals (vdWTS) scheme aimed......Mixed multiscale quantum/molecular mechanics (QM/MM) models are widely used to explore the structure, reactivity, and electronic properties of complex chemical systems. Whereas such models typically include electrostatics and potentially polarization in so-called electrostatic and polarizable...... at describing dispersion and repulsion interactions between quantum and classical regions within a QM/MM polarizable embedding framework. Starting from the vdWTSexpression, we define a dispersion and a repulsion term, both of them density-dependent and consistently based on a Lennard-Jones-like potential. We...
Bardhan, Jaydeep P.; Knepley, Matthew G.
2014-01-01
We show that charge-sign-dependent asymmetric hydration can be modeled accurately using linear Poisson theory after replacing the standard electric-displacement boundary condition with a simple nonlinear boundary condition. Using a single multiplicative scaling factor to determine atomic radii from molecular dynamics Lennard-Jones parameters, the new model accurately reproduces MD free-energy calculations of hydration asymmetries for: (i) monatomic ions, (ii) titratable amino acids in both their protonated and unprotonated states, and (iii) the Mobley “bracelet” and “rod” test problems [D. L. Mobley, A. E. Barber II, C. J. Fennell, and K. A. Dill, “Charge asymmetries in hydration of polar solutes,” J. Phys. Chem. B 112, 2405–2414 (2008)]. Remarkably, the model also justifies the use of linear response expressions for charging free energies. Our boundary-element method implementation demonstrates the ease with which other continuum-electrostatic solvers can be extended to include asymmetry. PMID:25296776
Energy Technology Data Exchange (ETDEWEB)
Bardhan, Jaydeep P. [Department of Mechanical and Industrial Engineering, Northeastern University, Boston, Massachusetts 02115 (United States); Knepley, Matthew G. [Computation Institute, The University of Chicago, Chicago, Illinois 60637 (United States)
2014-10-07
We show that charge-sign-dependent asymmetric hydration can be modeled accurately using linear Poisson theory after replacing the standard electric-displacement boundary condition with a simple nonlinear boundary condition. Using a single multiplicative scaling factor to determine atomic radii from molecular dynamics Lennard-Jones parameters, the new model accurately reproduces MD free-energy calculations of hydration asymmetries for: (i) monatomic ions, (ii) titratable amino acids in both their protonated and unprotonated states, and (iii) the Mobley “bracelet” and “rod” test problems [D. L. Mobley, A. E. Barber II, C. J. Fennell, and K. A. Dill, “Charge asymmetries in hydration of polar solutes,” J. Phys. Chem. B 112, 2405–2414 (2008)]. Remarkably, the model also justifies the use of linear response expressions for charging free energies. Our boundary-element method implementation demonstrates the ease with which other continuum-electrostatic solvers can be extended to include asymmetry.
Shukla-Eliasson attractive force: Revisited
Akbari-Moghanjoughi, M.; Akbari-Moghanjoughi
2013-04-01
By investigating the dielectric response of the Fermi-Dirac plasma in the linear limit and evaluating the electrostatic potential around the positive stationary test charge, we find that the Shukla-Eliasson attractive force is present for the plasma density range expected in the interiors of large planets for a wide range of plasma atomic number. This research, which is based on the generalized electron Fermi-momentum, further confirms the existence of the newly discovered Lennard-Jones-like attractive potential and its inevitable role in plasma crystallization in the cores of planets. Moreover, it is observed that the characteristics of the attractive potential are strongly sensitive to the variation of plasma density and composition. Current research can also have applications in the study of strong laser-matter interactions and inertially confined plasmas.
New theories for smectic and nematic liquid crystalline polymers
International Nuclear Information System (INIS)
Dowell, F.
1987-01-01
A summary of results from new statistical-physics theories for both backbone and side-chain liquid crystalline polymers (LCPs) and for mixtures with LCPs is presented. Thermodynamic and molecular ordering properties (including odd-even effects) have been calculated as a function of pressure, density, temperature, and molecule chemical structures (including degree of polymerization and the following properties of the chemical structures of the repeat units: lengths and shapes, intra-chain rotation energies, dipole moments, site-site polarizabilities and Lennard-Jones potentials, etc.) in nematic and multiple smectic-A LC phases and in the isotropic liquid phase. These theories can also be applied to combined LCPs. Since these theories have no ad hoc or arbitrarily adjustable parameters, these theories have been used to design new LCPs and new solvents and to predict and explain properties
Predicting Flory-Huggins χ from Simulations
Zhang, Wenlin; Gomez, Enrique D.; Milner, Scott T.
2017-07-01
We introduce a method, based on a novel thermodynamic integration scheme, to extract the Flory-Huggins χ parameter as small as 10-3k T for polymer blends from molecular dynamics (MD) simulations. We obtain χ for the archetypical coarse-grained model of nonpolar polymer blends: flexible bead-spring chains with different Lennard-Jones interactions between A and B monomers. Using these χ values and a lattice version of self-consistent field theory (SCFT), we predict the shape of planar interfaces for phase-separated binary blends. Our SCFT results agree with MD simulations, validating both the predicted χ values and our thermodynamic integration method. Combined with atomistic simulations, our method can be applied to predict χ for new polymers from their chemical structures.
Unusual mechanism of capillary condensation in pores modified with chains forming pillars.
Borówko, M; Patrykiejew, A; Sokołowski, S
2011-08-07
Density functional approach is applied to study the phase behavior of Lennard-Jones(12,6) fluid in pillared slit-like pores. Our focus is in the evaluation of phase transitions in fluid adsorbed in the pore of a fixed width. If the length of pillars is sufficiently large, we observe additional phase transitions of the first and second order due to the symmetry breaking of the distribution of chain segments and fluid species with respect to the slit-like pore center. Re-entrant symmetry changes and additional critical, critical end points and tricritical points then are observed. The scenario of phase changes is sensitive to the energy of fluid-solid interaction, the amount, and the length of the pillars. Quantitative trends and qualitative changes of the phase diagrams topology are examined depending on the values of these parameters.
Berim, Gersh O; Ruckenstein, Eli
2012-08-07
Adsorption isoterms and capillary condensation in an open slit with walls decorated with arrays of pillars are examined using the density functional theory. Compared with the main substrate, the pillars can have the same or different parameters in the Lennard-Jones interaction potential between them and the fluid in the slit. The roughness of the solid surface, defined as the ratio between the area of the actual surface and the area of the surface free of pillars, is controlled by the height of the pillars. It is shown that the capillary condensation pressure first increases with increasing roughness, passes through a maximum, and then decreases. The amount of adsorbed fluid at constant volume of the slit has, in general, a nonmonotonic dependence on roughness. These features of adsorption and capillary condensation are results of increased surface area and changes in the fluid-solid potential energy due to changes in roughness.
International Nuclear Information System (INIS)
Bishop, M.; Kalos, M.H.; Frisch, H.L.
1983-01-01
The influence of the attractive portion of the Lennard-Jones potential on the statics and dynamics of both single chain and multichain systems is investigated by reptation and molecular dynamics simulations. There is no significant effect at a reduced temperature of 10.0. At a temperature of 1.7 the single chain and multichain system at low densities (0.1) indicate that the attractions cause both the chains to be significantly more compact and a slowing of the time autocorrelation functions of the square of the end-to-end distance and radius of gyration. At a moderate density of 0.5, the attractions have almost no effect on the static structure, but they still influence the dynamic properties
Comment on 'Path integral solution for a Mie-type potential'
International Nuclear Information System (INIS)
Steiner, F.
1985-01-01
We comment on several incorrect results given in a recent paper by Erkoc and Sever (ES). In particular, it is pointed out that their path integral formula for the one-dimensional Mie-Lennard-Jones potential is wrong, since a quantum correction proportional to (h/2π) 2 - which is a consequence of the stochastic nature of the Feynman paths - has been overlooked. The correct expression can be obtained from a general path integral formula, which we have derived in a previous paper. For the particular potential discussed in detail by ES, we give a complete path integral treatment, which allows us to derive the energies and normalized wave functions of the discrete spectrum. (orig.)
Density functional study of the pressure tensor for inhomogeneous Lennard—Jones fluids
International Nuclear Information System (INIS)
Sun Zong-Li; Liu Zhi-Cheng; Kang Yan-Shuang; Ma Heng-Xin; Kang Yan-Mei
2012-01-01
Based on classical density functional theory, an expression of the pressure tensor for inhomogeneous fluids is presented. This takes into account greater correlation between particles, especially for systems that are geometrically confined or involve an interface. The density and pressure components of Lennard-Jones fluids confined in hard and softened nano-cavities are calculated. A comparison between the results of this work and IK expression suggests that the agreement depends on temperature. The interfacial tension for hard sphere fluids agrees well with the Monte Carlo result when the bulk density is not too large. The results of the solid-fluid interfacial tension for Lennard—Jones fluids demonstrate that different types of external potentials modulate the interfacial tension in different manners. (condensed matter: structural, mechanical, and thermal properties)
International Nuclear Information System (INIS)
Dowell, F.
1987-01-01
A summary of predictions and explanations from statistical-physics theories for both backbone and side-chain liquid crystalline polymers (LCPs) and for mixtures with backbone LCPs are presented. Trends in the thermodynamic and molecular ordering properties have been calculated as a function of pressure, density, temperature, and molecule chemical structures (including degree of polymerization and the following properties of the chemical structures of the repeat units: lengths and shapes, intra-chain rotation energies, dipole moments, site-site polarizabilities and Lennard-Jones potentials, etc.) in nematic and multiple smectic-A LC phases and in the isotropic liquid phase. The theoretical results are found to be in good agreement with existing experimental data. These theories can also be applied to combined LCPs. Since these theories have no ad hoc or arbitrarily adjustable parameters, these theories can be used to design new LCPs and new solvents as well as to predict and explain properties. 27 refs., 4 tabs
Continuous approximation for interaction energy of adamantane encapsulated inside carbon nanotubes
Baowan, Duangkamon; Hill, James M.; Bacsa, Wolfgang
2018-02-01
The interaction energy for two adjacent adamantane molecules and that of adamantane molecules encapsulated inside carbon nanotubes are investigated considering only dipole-dipole induced interaction. The Lennard-Jones potential and the continuous approximation are utilised to derive analytical expressions for these interaction energies. The equilibrium distance 3.281 Å between two adamantane molecules is determined. The smallest carbon nanotube radius b0 that can encapsulate the adamantane molecule and the radius of the tube bmax that gives the maximum suction energy, linearly depend on the adamantane radius, are calculated. For larger diameter tubes, the off axis position has been calculated, and equilibrium distance between molecule and tube wall is found to be close to the interlayer spacing in graphene.
Mechanical properties of pillared-graphene nanostructures using molecular dynamics simulations
International Nuclear Information System (INIS)
Wang, Chih-Hao; Fang, Te-Hua; Sun, Wei-Li
2014-01-01
The deformation behaviour and mechanical properties of three-dimensional (3D) pillared graphene are investigated using molecular dynamics simulations. The Tersoff–Brenner many-body potential model is employed to evaluate the interactions between 3D pillared-graphene carbon atoms and nanotube carbons. The Lennard-Jones potential model is used to compute the interactions between a conical indenter and 3D pillared-graphene carbon atoms. The effects of the size and geometric structure of 3D pillared-graphene are evaluated in terms of the indentation force and contact stiffness. The simulation results for an armchair nanotube of 3D pillared graphene show that the contact stiffness increases with increasing chiral vector of the 3D-pillared graphene. However, the adhesive force sharply decreases with increasing chiral vector of the 3D-pillared graphene. A zigzag nanotube of 3D-pillared graphene exhibits better mechanical properties compared with those of the armchair nanotube. (paper)
Simulating prescribed particle densities in the grand canonical ensemble using iterative algorithms.
Malasics, Attila; Gillespie, Dirk; Boda, Dezso
2008-03-28
We present two efficient iterative Monte Carlo algorithms in the grand canonical ensemble with which the chemical potentials corresponding to prescribed (targeted) partial densities can be determined. The first algorithm works by always using the targeted densities in the kT log(rho(i)) (ideal gas) terms and updating the excess chemical potentials from the previous iteration. The second algorithm extrapolates the chemical potentials in the next iteration from the results of the previous iteration using a first order series expansion of the densities. The coefficients of the series, the derivatives of the densities with respect to the chemical potentials, are obtained from the simulations by fluctuation formulas. The convergence of this procedure is shown for the examples of a homogeneous Lennard-Jones mixture and a NaCl-CaCl(2) electrolyte mixture in the primitive model. The methods are quite robust under the conditions investigated. The first algorithm is less sensitive to initial conditions.
Classical molecular dynamics simulation on the dynamical properties of H2 on silicene layer
Directory of Open Access Journals (Sweden)
Casuyac Miqueas
2016-01-01
Full Text Available This study investigates the diffusion of hydrogen molecule physisorbed on the surface of silicene nanoribbon (SiNRusing the classical molecular dynamic (MD simulation in LAMMPS (Large-scale Atomic/Molecular Massively Parallel Simulator. The interactions between silicon atoms are modeled using the modified Tersoff potential, the Adaptive Intermolecular Reactive Empirical Bond Order (AIREBO potential for hydrogen – hydrogen interaction and the Lennard – Jones potential for the physisorbed H2 on SiNR. By varying the temperatures (60 K Δ 130 K, we observed that the Δxdisplacement of H2 on the surface SiNR shows a Brownian motion on a Lennard-Jones potential and a Gaussian probability distribution can be plotted describing the diffusion of H2. The calculated mean square displacement (MSD was approximately increasing in time and the activation energy barrier for diffusion has been found to be 43.23meV.
Dislocations and melting in two and three dimensions
DEFF Research Database (Denmark)
Tallon, Jeffery L.
1980-01-01
included, the model system may jump discontinuously from a volume below the dislocation transition to a volume above the disclination transition so that both transitions are virtual and are hidden in the first-order discontinuity. A reinterpretation of the recent molecular-dynamics simulation of two-dimensional......Comments are presented on the recent theories of two-dimensional melting which envisage melting as proceeding via two second-order transitions comprising dislocation dipole dissociation followed by disclination dipole dissociation. It is suggested that if the configurational entropy is properly...... melting of Frenkel and McTague, reveals that such is the case for a Lennard-Jones system. There may be no fundamental difference between two-and three-dimensional melting. ©1980 The American Physical Society...
Theoretical-experimental study of the solvation enthalpy of acetone in dilute aqueous solution
International Nuclear Information System (INIS)
Arroyo, S. Tolosa; Martin, J.A. Sanson; Garcia, A. Hidalgo
2005-01-01
The present paper describes molecular dynamics simulations of aqueous solutions at infinite dilution with acetone as solute. Lennard-Jones with electrostatic term (12-6-1 potentials) were employed to describe the solute-solvent interactions. The Morokuma decomposition scheme of ab initio interaction energies at the SCF level and the ESIE charges on the solute atoms were used to reproduce the exchange and Coulomb electrostatic contributions of the solute-water interaction potential. Some extensions, such as including the dispersion component evaluated at MP2 level, were added to the traditional calculation procedures in order to improve the results of the solvation enthalpy. The results obtained with the EX-DIS-ES model were compared with the experimental calorimetry values, the observed agreement being acceptable
Memory function approach to the line shape problem in collision-induced light scattering
International Nuclear Information System (INIS)
Balucani, U.; Tognetti, V.; Vallauri, R.
1980-01-01
This article mainly deals with the problem of the shape of the spectrum due to interacting pairs of atoms at low and moderate densities. A memory function approach is used which permits to obtain in a consistent way the shape of the scattered spectrum. In order to obtain 'exact' time correlation functions and spectral shapes, molecular-dynamics 'experiments' in Lennard-Jones argon at two different densities were also performed. The dipole-induced dipole (DID) polarizabilities have been used to ascertain the validity of the theoretical approach in a well-defined physical model. The theoretical shapes and correlation functions can be then directly compared with computer simulations. Finally, a comparison with the data of real experiments clarifies the relevance of other-than-DID polarizability mechanisms as far as the spectrum is concerned. (KBE)
Energy Technology Data Exchange (ETDEWEB)
Baer, M.R.; Hobbs, M.L.; McGee, B.C.
1998-11-03
Exponential-13,6 (EXP-13,6) potential pammeters for 750 gases composed of 48 elements were determined and assembled in a database, referred to as the JCZS database, for use with the Jacobs Cowperthwaite Zwisler equation of state (JCZ3-EOS)~l) The EXP- 13,6 force constants were obtained by using literature values of Lennard-Jones (LJ) potential functions, by using corresponding states (CS) theory, by matching pure liquid shock Hugoniot data, and by using molecular volume to determine the approach radii with the well depth estimated from high-pressure isen- tropes. The JCZS database was used to accurately predict detonation velocity, pressure, and temperature for 50 dif- 3 Accurate predictions were also ferent explosives with initial densities ranging from 0.25 glcm3 to 1.97 g/cm . obtained for pure liquid shock Hugoniots, static properties of nitrogen, and gas detonations at high initial pressures.
Computer simulations of nanoindentation in Mg-Cu and Cu-Zr metallic glasses
DEFF Research Database (Denmark)
Paduraru, Anca; Andersen, Ulrik Grønbjerg; Thyssen, Anders
2010-01-01
The formation of shear bands during plastic deformation of Cu0.50Zr0.50 and Mg0.85Cu0.15 metallic glasses is studied using atomic-scale computer simulations. The atomic interactions are described using realistic many-body potentials within the effective medium theory, and are compared with similar...... simulations using a Lennard-Jones description of the material. The metallic glasses are deformed both in simple shear and in a simulated nanoindentation experiment. Plastic shear localizes into shear bands with a width of approximately 5 nm in CuZr and 8 nm in MgCu. In simple shear, the shear band formation...... is very clear, whereas only incipient shear bands are seen in nanoindentation. The shear band formation during nanoindentation is sensitive to the indentation velocity, indenter radius and the cooling rate during the formation of the metallic glass. For comparison, a similar nanoindentation simulation...
Empirical potential for molecular simulation of graphene nanoplatelets
Bourque, Alexander J.; Rutledge, Gregory C.
2018-04-01
A new empirical potential for layered graphitic materials is reported. Interatomic interactions within a single graphene sheet are modeled using a Stillinger-Weber potential. Interatomic interactions between atoms in different sheets of graphene in the nanoplatelet are modeled using a Lennard-Jones interaction potential. The potential is validated by comparing molecular dynamics simulations of tensile deformation with the reported elastic constants for graphite. The graphite is found to fracture into graphene nanoplatelets when subjected to ˜15% tensile strain normal to the basal surface of the graphene stack, with an ultimate stress of 2.0 GPa and toughness of 0.33 GPa. This force field is useful to model molecular interactions in an important class of composite systems comprising 2D materials like graphene and multi-layer graphene nanoplatelets.
Monte Carlo simulation of continuous-space crystal growth
International Nuclear Information System (INIS)
Dodson, B.W.; Taylor, P.A.
1986-01-01
We describe a method, based on Monte Carlo techniques, of simulating the atomic growth of crystals without the discrete lattice space assumed by conventional Monte Carlo growth simulations. Since no lattice space is assumed, problems involving epitaxial growth, heteroepitaxy, phonon-driven mechanisms, surface reconstruction, and many other phenomena incompatible with the lattice-space approximation can be studied. Also, use of the Monte Carlo method circumvents to some extent the extreme limitations on simulated timescale inherent in crystal-growth techniques which might be proposed using molecular dynamics. The implementation of the new method is illustrated by studying the growth of strained-layer superlattice (SLS) interfaces in two-dimensional Lennard-Jones atomic systems. Despite the extreme simplicity of such systems, the qualitative features of SLS growth seen here are similar to those observed experimentally in real semiconductor systems
The effect of system boundaries on the mean free path for confined gases
Directory of Open Access Journals (Sweden)
Sooraj K. Prabha
2013-10-01
Full Text Available The mean free path of rarefied gases is accurately determined using Molecular Dynamics simulations. The simulations are carried out on isothermal argon gas (Lennard-Jones fluid over a range of rarefaction levels under various confinements (unbounded gas, parallel reflective wall and explicit solid platinum wall bounded gas in a nanoscale domain. The system is also analyzed independently in constitutive sub-systems to calculate the corresponding local mean free paths. Our studies which predominate in the transition regime substantiate the boundary limiting effect on mean free paths owing to the sharp diminution in molecular free paths near the planar boundaries. These studies provide insight to the transport phenomena of rarefied gases through nanochannels which have established their potential in microscale and nanoscale heat transfer applications.
Communication: Thermodynamic analysis of critical conditions of polymer adsorption
Energy Technology Data Exchange (ETDEWEB)
Cimino, R.; Neimark, A. V., E-mail: aneimark@rutgers.edu [Department of Chemical and Biochemical Engineering, Rutgers, The State University of New Jersey, 98 Brett Road, Piscataway, New Jersey 08854 (United States); Rasmussen, C. J. [DuPont Central Research and Development, Corporate Center for Analytical Sciences, Macromolecular Characterization, Route 141 and Henry Clay, Wilmington, Delaware 19803 (United States)
2013-11-28
Polymer adsorption to solid surfaces is a ubiquitous phenomenon, which has attracted long-lasting attention. Dependent on the competition between the polymer-solid adsorption and polymer-solvent solvation interactions, a chain may assume either 3d solvated conformation when adsorption is weak or 2d adsorbed conformation when adsorption is strong. The transition between these conformations occurring upon variation of adsorption strength is quite sharp, and in the limit of “infinite” chain length, can be treated as a critical phenomenon. We suggest a novel thermodynamic definition of the critical conditions of polymer adsorption from the equality of incremental chemical potentials of adsorbed and free chains. We show with the example of freely jointed Lennard-Jones chains tethered to an adsorbing surface that this new definition provides a link between thermodynamic and geometrical features of adsorbed chains and is in line with classical scaling relationships for the fraction of adsorbed monomers, chain radii of gyration, and free energy.
Classical square-plus-triangle well fluid
International Nuclear Information System (INIS)
Boghdadi, M.
1984-01-01
A simplified model for the intermolecular-potential function which consists of a hard core and a square-plus-triangle well is proposed. The square width is taken to be lambda 1 -1 and the triangle width is lambda 2 -lambda 1 , where the diameter of the molecules is assumed to be epsilon. Under the restriction that the area under the potential well should be equal to 0.5epsilon, which has its own reason, it is shown that the appropriate choice of lambda 1 and lambda 2 that best mimics the Lennard-Jones (LJ) cut-off results is 1.15 and 1.85 respectively. With this choice for lambda 1 and lambda 2 , the proposed model is effective and satisfactory
Atomistic simulation of processes in Ni-base alloys with account for local relaxations
International Nuclear Information System (INIS)
Bursik, Jiri
2007-01-01
Ordering in Ni-base superalloys is the crucial process controlling the development of the characteristic two-phase microstructure and subsequently the mechanical properties. Systems containing up to six alloying elements typical of advanced Ni-based superalloys are modelled in this work using a Monte Carlo approach with phenomenological Lennard-Jones pair potentials and interactions up to the third coordination sphere. Three-dimensional crystal block is used with over 10 5 atoms. Molecular dynamics approach is used to relax local atomic positions in course of ordering processes under applied stress. The importance of taking into account both relaxation of modelled block dimensions and relaxation of local atomic positions is discussed
Equilibrium location for spherical DNA and toroidal cyclodextrin
Sarapat, Pakhapoom; Baowan, Duangkamon; Hill, James M.
2018-05-01
Cyclodextrin comprises a ring structure composed of glucose molecules with an ability to form complexes of certain substances within its central cavity. The compound can be utilised for various applications including food, textiles, cosmetics, pharmaceutics, and gene delivery. In gene transfer, the possibility of forming complexes depends upon the interaction energy between cyclodextrin and DNA molecules which here are modelled as a torus and a sphere, respectively. Our proposed model is derived using the continuum approximation together with the Lennard-Jones potential, and the total interaction energy is obtained by integrating over both the spherical and toroidal surfaces. The results suggest that the DNA prefers to be symmetrically situated about 1.2 Å above the centre of the cyclodextrin to minimise its energy. Furthermore, an optimal configuration can be determined for any given size of torus and sphere.
The structure of the solid-liquid interface: atomic size effect
International Nuclear Information System (INIS)
Geysermans, P.; Pontikis, V.
2002-01-01
The atomic structure of the solid-liquid heterophase interface was investigated by using molecular dynamics. Two kinds of systems were studied; the first one was crystalline copper with (100) and (111) surface terminations in contact with liquid aluminium, while in the second one the interface was modelled by two systems in contact made of Lennard-Jones particles with different size (σ) and energy (ε) parameters. We found that at the interface the liquid was layered whatever the crystallographic orientation of the surface. The layering of the liquid is still preserved when the ratio of particles sites (χ=σ 1 /σ 2 ) changes while an epitaxial relationship is always found between the crystal and the first liquid layer. The average density of the latter is closely related to the χ value. (authors)
Application of the cluster variation method to ordering in an interstitital solid solution
DEFF Research Database (Denmark)
Pekelharing, Marjon I.; Böttger, Amarante; Somers, Marcel A. J.
1999-01-01
The tetrahedron approximation of the cluster variation method (CVM) was applied to describe the ordering on the fcc interstitial sublattice of gamma-Fe[N] and gamma'-Fe4N1-x. A Lennard-Jones potential was used to describe the dominantly strain-induced interactions, caused by misfitting of the N...... atoms in the interstitial octahedral sites. The gamma-Fe[N]/gamma'-Fe4N1-x miscibility gap, short range ordering (SRO), and long-range ordering (LRO) of nitrogen in gamma-Fe[N] and gamma'-Fe4N1-x, respectively, and lattice parameters of gamma and gamm' were calculated. For the first time, N distribution...... parameters,as calculated by CVM, were compared directly to Mössbauer data for specific surroundings of Fe atoms....
Weak temperature dependence of ageing of structural properties in atomistic model glassformers
Jenkinson, Thomas; Crowther, Peter; Turci, Francesco; Royall, C. Patrick
2017-08-01
Ageing phenomena are investigated from a structural perspective in two binary Lennard-Jones glassformers, the Kob-Andersen and Wahnström mixtures. In both, the geometric motif assumed by the glassformer upon supercooling, the locally favoured structure (LFS), has been established. The Kob-Andersen mixture forms bicapped square antiprisms; the Wahnström model forms icosahedra. Upon ageing, we find that the structural relaxation time has a time-dependence consistent with a power law. However, the LFS population and potential energy increase and decrease, respectively, in a logarithmic fashion. Remarkably, over the time scales investigated, which correspond to a factor of 104 change in relaxation times, the rate at which these quantities age appears almost independent of temperature. Only at temperatures far below the Vogel-Fulcher-Tamman temperature do the ageing dynamics slow.
International Nuclear Information System (INIS)
Damyanova, M; Balabanova, E; Hohm, U
2014-01-01
A temperature-dependent effective intermolecular interaction potential is applied to describe the interaction between two nitrogen fluoride (NF 3 ) molecules in gas phase. To this end, a spherically-symmetric (n-6) Lennard-Jones temperature-dependent potential (LJTDP) is used. The (n-6) LJTDP takes into account the influence of vibrational excitation of the molecules on the potential parameters, namely, the equilibrium distance r m and the potential well depth ε. The potential parameters at T = 0 K were obtained from the very small amount of existing thermophysical equilibrium and transport properties of low-density NF 3 gas. Fitting formulae are tabulated for a fast and reliable prediction of the thermophysical properties and potential parameters in the temperature range between 200 K and 1200 K. A comparison is also presented between our estimates for some thermophysical properties of the NF 3 gas with the available experimental and calculated data.
Local elastic properties of nano-confined fluids: A density functional study
International Nuclear Information System (INIS)
Sun, Zongli; Kang, Yanshuang
2014-01-01
The understanding of mechanical properties of confined fluids is essential for modeling and manipulating of nano-scaled systems. Unlike the uniform phase, the confined fluids usually display different features in structure and related properties. Due to the presence of the confining geometry, the density profile and many physical and chemical properties may be position-dependent. The aim of our research is to derive an expression for the local elastic property by using the classical elastic theory. Both the bulk and shear moduli are expressed as functional of density of particle. The theoretical result derived is applied to the Lennard-Jones fluids confined in nano-cavity. Comparison of our numerical result and the simulation result is made and qualitative agreement is observed. Further, influence of bulk density, temperature and external potential on moduli is calculated and the physical mechanism is analyzed. Relationship between contact modulus and the interfacial tension is also calculated. Their opposite trend with temperature is observed.
Response functions for crystals and surfaces, with applications to surface scattering
International Nuclear Information System (INIS)
Barker, J.A.; Steele, W.A.
1978-01-01
A general solution of the equations of forced motion of a harmonic crystal or other vibrating system with arbitrary time-dependent forces acting on the atoms is given. The solution is given in terms of dynamical 'response functions', for which expressions in terms of the normal mode frequencies and eigenvectors (polarization vectors) are given. Numerical calculations of the response functions are described for (111) and (100) surfaces of face-centered cubic crystals interacting with Lennard-Jones 6-12 potentials, and the qualitative features of the surface and bulk response functions are discussed. The use of these functions in problems of atomic scattering from surface is outlined, and convenient parametrized forms for this application are given. (Auth.)
Structural models for amorphous transition metal binary alloys
International Nuclear Information System (INIS)
Ching, W.Y.; Lin, C.C.
1976-01-01
A dense random packing of 445 hard spheres with two different diameters in a concentration ratio of 3 : 1 was hand-built to simulate the structure of amorphous transition metal-metalloid alloys. By introducing appropriate pair potentials of the Lennard-Jones type, the structure is dynamically relaxed by minimizing the total energy. The radial distribution functions (RDF) for amorphous Fe 0 . 75 P 0 . 25 , Ni 0 . 75 P 0 . 25 , Co 0 . 75 P 0 . 25 are obtained and compared with the experimental data. The calculated RDF's are resolved into their partial components. The results indicate that such dynamically constructed models are capable of accounting for some subtle features in the RDF of amorphous transition metal-metalloid alloys
Computational study of heat transport in compositionally disordered binary crystals
International Nuclear Information System (INIS)
Lyver, John W.; Blaisten-Barojas, Estela
2006-01-01
The thermal conductivity of compositionally disordered binary crystals with atoms interacting through Lennard-Jones potentials has been studied as a function of temperature. The two species in the crystal differ in mass, hard-core atomic diameter, well depth and relative concentration. The isobaric Monte Carlo was used to equilibrate the samples at near-zero pressure. The isoenergy molecular dynamics combined with the Green-Kubo approach was taken to calculate the heat current time-dependent autocorrelation function and determine the lattice thermal conductivity of the sample. The inverse temperature dependence of the lattice thermal conductivity was shown to fail at low temperatures when the atomic diameters of the two species differ. Instead, the thermal conductivity was nearly a constant across temperatures for species with different atomic diameters. Overall, it is shown that there is a dramatic decrease of the lattice thermal conductivity with increasing atomic radii ratio between species and a moderate decrease due to mass disorder
Cluster dynamics: A classical trajectory study of A + A/sub n/arrow-right-leftA*/sub n/+1
International Nuclear Information System (INIS)
Brady, J.W.; Doll, J.D.; Thompson, D.L.
1979-01-01
The dynamics of the collision of an atom A with a small cluster of atoms, A/sub n/, leading to the formation of a quasibound A*/sub n/+1 complex, which subsequently decays, has been studied using classical trajectories. Pairwise Lennard-Jones potentials (with parameters appropriate for argon) were used to describe the identical point masses (Ar). The results illustrate the feasibility of direct calculations of microscopic rates for nucleation processes. The dissociation of collisionally formed A*/sub n/+1 (n=3,4, and 5) occurs by first-order exponential decay. Furthermore the energy dependence of the dissociation rate constants appears to be well described by the RRK functional form
Yin, Jian; Fenley, Andrew T.; Henriksen, Niel M.; Gilson, Michael K.
2015-01-01
Improving the capability of atomistic computer models to predict the thermodynamics of noncovalent binding is critical for successful structure-based drug design, and the accuracy of such calculations remains limited by non-optimal force field parameters. Ideally, one would incorporate protein-ligand affinity data into force field parametrization, but this would be inefficient and costly. We now demonstrate that sensitivity analysis can be used to efficiently tune Lennard-Jones parameters of aqueous host-guest systems for increasingly accurate calculations of binding enthalpy. These results highlight the promise of a comprehensive use of calorimetric host-guest binding data, along with existing validation data sets, to improve force field parameters for the simulation of noncovalent binding, with the ultimate goal of making protein-ligand modeling more accurate and hence speeding drug discovery. PMID:26181208
Application of Statistical Thermodynamics in Refrigeration
International Nuclear Information System (INIS)
Avsec, J.; Marcic, M.
1999-01-01
The paper presents the mathematical model for computing the thermodynamical properties in the liquid, gas and two-phase domain by means of statistical thermodynamics. The paper features all important components (translation, rotation, internal rotation, vibration, intermolecular potential energy and influence of electron and nuclei excitation). To calculate the thermodynamic properties of real gases, we have developed the cluster theory, which yields better results than the virial equation. In case of real liquids, the Johnson-Zollweg-Gubbins model based on the modified Benedict-Webb-Rubin (BWR) equation was applied. The Lennard-Jones intermolecular potential was used. The analytical results are compared with the thermodynamical data and models obtained from classical thermodynamics, and they show relatively good agreement. (author)
Solute-solvent cavity and bridge functions. I. Varying size of the solute
International Nuclear Information System (INIS)
Vyalov, I.; Chuev, G.; Georgi, N.
2014-01-01
In this work we present the results of the extensive molecular simulations of solute-solvent cavity and bridge functions. The mixtures of Lennard-Jones solvent with Lennard-Jones solute at infinite dilution are considered for different solute-solvent size ratios—up to 4:1. The Percus-Yevick and hypernetted chain closures deviate substantially from simulation results in the investigated temperature and density ranges. We also find that the behavior of the indirect and cavity correlation functions is non-monotonous within the hard-core region, but the latter can be successfully approximated by mean-field theory if the solute-solvent interaction energy is divided into repulsive and attractive contribution, according to Weeks-Chandler-Andersen theory. Furthermore, in spite of the non-monotonous behavior of logarithm of the cavity function and the indirect correlation function, their difference, i.e., the bridge function remains constant within the hard-core region. Such behavior of the bridge and indirect correlation functions at small distances and for small values of indirect correlation function is well known from the Duh-Haymet plots, where the non-unique relationship results in loops of the bridge function vs. indirect correlation function graphs. We show that the same pathological behavior appears also when distance is small and indirect correlation function is large. We further show that the unique functional behavior of the bridge function can be established when bridge is represented as a function of the renormalized, repulsive indirect correlation function
Importance of dispersion and electron correlation in ab initio protein folding.
He, Xiao; Fusti-Molnar, Laszlo; Cui, Guanglei; Merz, Kenneth M
2009-04-16
Dispersion is well-known to be important in biological systems, but the effect of electron correlation in such systems remains unclear. In order to assess the relationship between the structure of a protein and its electron correlation energy, we employed both full system Hartree-Fock (HF) and second-order Møller-Plesset perturbation (MP2) calculations in conjunction with the Polarizable Continuum Model (PCM) on the native structures of two proteins and their corresponding computer-generated decoy sets. Because of the expense of the MP2 calculation, we have utilized the fragment molecular orbital method (FMO) in this study. We show that the sum of the Hartree-Fock (HF) energy and force field (LJ6)-derived dispersion energy (HF + LJ6) is well correlated with the energies obtained using second-order Møller-Plesset perturbation (MP2) theory. In one of the two examples studied, the correlation energy as well as the empirical dispersive energy term was able to discriminate between native and decoy structures. On the other hand, for the second protein we studied, neither the correlation energy nor dispersion energy showed discrimination capabilities; however, the ab initio MP2 energy and the HF+LJ6 both ranked the native structure correctly. Furthermore, when we randomly scrambled the Lennard-Jones parameters, the correlation between the MP2 energy and the sum of the HF energy and dispersive energy (HF+LJ6) significantly drops, which indicates that the choice of Lennard-Jones parameters is important.
Interaction potentials and their effect on crystal nucleation and symmetry
International Nuclear Information System (INIS)
Hsu, C.S.; Rahman, A.
1979-01-01
Molecular dynamics technique has been used to study the effect of the interaction potential on crystal nucleation and the symmetry of the nucleated phase. Four systems, namely rubidium, Lennard-Jones, rubidium-truncated, and Lennard-Jones-truncated, have been studied each at reduced density 0.95. Two types of calculations were performed. Firstly, starting from a liquid state, each system was quenched rapidly to a reduced temperature of approx.0.1. The nucleation process for these systems was monitored by studying the time dependence of temperature and the pair correlation function, and the resulting crystalline structure analyzed using among other properties the Voronoi polyhedra. Only in the case of rubidium was a b.c.c. structure nucleated. In the other three cases we obtained a f.c.c. ordering. Secondly, we have studied the effect of changing the interaction potential in a system which has already achieved an ordered state under the action of some other potential. After establishing a b.c.c. structure in a rubidium system, the change in the symmetry of the system was studied when the pair potential was modified to one of the other three forms. The results from both types of calculations are consistent: the rubidium potential leads to a b.c.c. structure while the other three potentials give an f.c.c. structure. Metastable disordered structures were not obtained in any of the calculations. However, the time elapse between the moment when the system is quick-quenched and the moment when nucleation occurs appears to depend upon the potential of interaction
MCCE analysis of the pKas of introduced buried acids and bases in staphylococcal nuclease.
Gunner, M R; Zhu, Xuyu; Klein, Max C
2011-12-01
The pK(a)s of 96 acids and bases introduced into buried sites in the staphylococcal nuclease protein (SNase) were calculated using the multiconformation continuum electrostatics (MCCE) program and the results compared with experimental values. The pK(a)s are obtained by Monte Carlo sampling of coupled side chain protonation and position as a function of pH. The dependence of the results on the protein dielectric constant (ε(prot)) in the continuum electrostatics analysis and on the Lennard-Jones non-electrostatics parameters was evaluated. The pK(a)s of the introduced residues have a clear dependence on ε(prot,) whereas native ionizable residues do not. The native residues have electrostatic interactions with other residues in the protein favoring ionization, which are larger than the desolvation penalty favoring the neutral state. Increasing ε(prot) scales both terms, which for these residues leads to small changes in pK(a). The introduced residues have a larger desolvation penalty and negligible interactions with residues in the protein. For these residues, changing ε(prot) has a large influence on the calculated pK(a). An ε(prot) of 8-10 and a Lennard-Jones scaling of 0.25 is best here. The X-ray crystal structures of the mutated proteins are found to provide somewhat better results than calculations carried out on mutations made in silico. Initial relaxation of the in silico mutations by Gromacs and extensive side chain rotamer sampling within MCCE can significantly improve the match with experiment. Copyright © 2011 Wiley-Liss, Inc.
Guillaume-Gentil, Orane; Zahn, Raphael; Lindhoud, Saskia; Graf, Norma; Voros, Janos; Zambelli, Tomaso
2011-01-01
Using atomic force microscopy, we investigated how the morphology of layer-by-layer deposited polyelectrolyte multilayers is influenced by the physical properties of the supporting substrate. The surface coverage of the assembly and its topography were found to be dependent on the dielectric
International Nuclear Information System (INIS)
Douberly, Gary E.; Liang, Tao; Raston, Paul L.; Marshall, Mark D.
2015-01-01
The T-shaped OH–C 2 H 2 complex is formed in helium droplets via the sequential pick-up and solvation of the monomer fragments. Rovibrational spectra of the a-type OH stretch and b-type antisymmetric CH stretch vibrations contain resolved parity splitting that reveals the extent to which electronic angular momentum of the OH moiety is quenched upon complex formation. The energy difference between the spin-orbit coupled 2 B 1 (A″) and 2 B 2 (A′) electronic states is determined spectroscopically to be 216 cm −1 in helium droplets, which is 13 cm −1 larger than in the gas phase [Marshall et al., J. Chem. Phys. 121, 5845 (2004)]. The effect of the helium is rationalized as a difference in the solvation free energies of the two electronic states. This interpretation is motivated by the separation between the Q(3/2) and R(3/2) transitions in the infrared spectrum of the helium-solvated 2 Π 3/2 OH radical. Despite the expectation of a reduced rotational constant, the observed Q(3/2) to R(3/2) splitting is larger than in the gas phase by ≈0.3 cm −1 . This observation can be accounted for quantitatively by assuming the energetic separation between 2 Π 3/2 and 2 Π 1/2 manifolds is increased by ≈40 cm −1 upon helium solvation
Czech Academy of Sciences Publication Activity Database
Uras-Aytemiz, N.; Cwiklik, Lukasz; Devlin, J. P.
2012-01-01
Roč. 137, č. 20 (2012), s. 204501 ISSN 0021-9606 Institutional support: RVO:61388955 Keywords : Fourier transform infrared emission spectra * clathrate hydrate * simulations Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.164, year: 2012
Formation of Nanodroplets in N_{2}/H_{2}O/SO_{2} under Irradiation of Fast Proton Beams
DEFF Research Database (Denmark)
Nakai, Youchi; Shigeoka, Tomita; Funada, Shuhei
of the droplet growth in thebinary nucleation process of water and H2SO4.We have performed irradiation of proton beam on the gas mixture of N2/H2O/SO2 andAir/H2O/SO2. The reduction of SO2 concentration by beam irradiation was monitored usingan SO2 meter and the size distributions of generated droplets were...
Leong, Kai-Yang; Wang, Feng
2018-04-01
The surface tension of nanoscale droplets of water was studied with molecular dynamics simulations using the BLYPSP-4F water potential. The internal pressure of the droplet was measured using an empirical correlation between the pressure and density, established through a series of bulk simulations performed at pressures from 1 to 1000 bars. Such a procedure allows for reliable determination of internal pressure without the need to calculate the local virial. The surface tension, estimated with the Young-Laplace relation, shows good agreement with the Tolman equation with a Tolman length of -0.48 Å. The interface of a liquid water droplet is shown to be around 1.1-1.3 nm thick depending on radii. The fairly thick interface region puts a lower limit on the size of droplets that still have a bulk-like interior.
International Nuclear Information System (INIS)
Dinpajooh, Mohammadhasan; Bai, Peng; Allan, Douglas A.; Siepmann, J. Ilja
2015-01-01
Since the seminal paper by Panagiotopoulos [Mol. Phys. 61, 813 (1997)], the Gibbs ensemble Monte Carlo (GEMC) method has been the most popular particle-based simulation approach for the computation of vapor–liquid phase equilibria. However, the validity of GEMC simulations in the near-critical region has been questioned because rigorous finite-size scaling approaches cannot be applied to simulations with fluctuating volume. Valleau [Mol. Simul. 29, 627 (2003)] has argued that GEMC simulations would lead to a spurious overestimation of the critical temperature. More recently, Patel et al. [J. Chem. Phys. 134, 024101 (2011)] opined that the use of analytical tail corrections would be problematic in the near-critical region. To address these issues, we perform extensive GEMC simulations for Lennard-Jones particles in the near-critical region varying the system size, the overall system density, and the cutoff distance. For a system with N = 5500 particles, potential truncation at 8σ and analytical tail corrections, an extrapolation of GEMC simulation data at temperatures in the range from 1.27 to 1.305 yields T c = 1.3128 ± 0.0016, ρ c = 0.316 ± 0.004, and p c = 0.1274 ± 0.0013 in excellent agreement with the thermodynamic limit determined by Potoff and Panagiotopoulos [J. Chem. Phys. 109, 10914 (1998)] using grand canonical Monte Carlo simulations and finite-size scaling. Critical properties estimated using GEMC simulations with different overall system densities (0.296 ≤ ρ t ≤ 0.336) agree to within the statistical uncertainties. For simulations with tail corrections, data obtained using r cut = 3.5σ yield T c and p c that are higher by 0.2% and 1.4% than simulations with r cut = 5 and 8σ but still with overlapping 95% confidence intervals. In contrast, GEMC simulations with a truncated and shifted potential show that r cut = 8σ is insufficient to obtain accurate results. Additional GEMC simulations for hard-core square-well particles with various
Hołyst, Robert; Litniewski, Marek; Jakubczyk, Daniel
2017-09-13
Transport of heat to the surface of a liquid is a limiting step in the evaporation of liquids into an inert gas. Molecular dynamics (MD) simulations of a two component Lennard-Jones (LJ) fluid revealed two modes of energy transport from a vapour to an interface of an evaporating droplet of liquid. Heat is transported according to the equation of temperature diffusion, far from the droplet of radius R. The heat flux, in this region, is proportional to temperature gradient and heat conductivity in the vapour. However at some distance from the interface, Aλ, (where λ is the mean free path in the gas), the temperature has a discontinuity and heat is transported ballistically i.e. by direct individual collisions of gas molecules with the interface. This ballistic transport reduces the heat flux (and consequently the mass flux) by the factor R/(R + Aλ) in comparison to the flux obtained from temperature diffusion. Thus it slows down the evaporation of droplets of sizes R ∼ Aλ and smaller (practically for sizes from 10 3 nm down to 1 nm). We analyzed parameter A as a function of interactions between molecules and their masses. The rescaled parameter, A(k B T b /ε 11 ) 1/2 , is a linear function of the ratio of the molecular mass of the liquid molecules to the molecular mass of the gas molecules, m 1 /m 2 (for a series of chemically similar compounds). Here ε 11 is the interaction parameter between molecules in the liquid (proportional to the enthalpy of evaporation) and T b is the temperature of the gas in the bulk. We tested the predictions of MD simulations in experiments performed on droplets of ethylene glycol, diethylene glycol, triethylene glycol and tetraethylene glycol. They were suspended in an electrodynamic trap and evaporated into dry nitrogen gas. A changes from ∼1 (for ethylene glycol) to approximately 10 (for tetraethylene glycol) and has the same dependence on molecular parameters as obtained for the LJ fluid in MD simulations. The value of x = A
The role of pressure in rubber elasticity.
Bower, A F; Weiner, J H
2004-06-22
We describe a series of molecular dynamics computations that reveal an intimate connection at the atomic scale between difference stress (which resists stretches) and pressure (which resists volume changes) in an idealized elastomer, in contrast to the classical theory of rubber elasticity. Our simulations idealize the elastomer as a "pearl necklace," in which the covalent bonds are stiff linear springs, while nonbonded atoms interact through a Lennard-Jones potential with energy epsilon(LJ) and radius sigma(LJ). We calculate the difference stress t(11)-(t(22)+t(33))/2 and mean stress (t(11)+t(22)+t(33))/3 induced by a constant volume extension in the x(1) direction, as a function of temperature T and reduced density rho(*)=Nsigma(IJ) (3)/nu. Here, N is the number of atoms in the simulation cell and nu is the cell volume. Results show that for rho(*)rubber elasticity, which neglects nonbonded interactions. However, data presented by van Krevelen [Properties of Polymers, 3rd ed. (Elsevier, Amsterdam, 1990), p. 79] indicate that rubber at standard conditions corresponds to rho(*)=1.2. For rho(*)>1, the system is entropic for kT/epsilon(LJ)>2, but at lower temperatures the difference stress contains an additional energy component, which increases as rho(*) increases and temperature decreases. Finally, the model exhibits a glass transition for rho(*)=1.2 and kT/epsilon(LJ) approximately 2. The atomic-scale processes responsible for generating stress are explored in detail. Simulations demonstrate that the repulsive portion of the Lennard-Jones potential provides a contribution sigma(nbr)>0 to the difference stress, the attractive portion provides sigma(nba) approximately 0, while the covalent bonds provide sigma(b)nbr)0, and Pi(b)nbr)=-APi(nbr)P(2)(theta(b)), sigma(b)=BPi(b)P(2)(theta(b)), where P(2)(theta(b)) is a measure of the anisotropy of the orientation of the covalent bonds, and A and B are coefficients that depend weakly on rho(*) and temperature. For high