Amorphous Media Research Articles

Liquid-glass transition as the freezing of characteristic acoustic frequencies

Half-quantum interpretation is proposed for the liquid-glass transition as the freezing of characteristic acoustic frequencies (degrees of freedom) that are related to the molecular mobility of delocalized excited kinetic units, namely, linear quantum oscillators. There exists a correlation between the energy quantum of an elementary excitation (atom delocalization energy) and the glass transition temperature, which is proportional to the characteristic Einstein temperature. By analogy with the Einstein theory of the heat capacity of solids, the temperature range of the concentration of excited atoms in an amorphous medium is divided into the following two regions: a high-temperature region with a linear temperature dependence of this concentration and a low-temperature region, where the concentration of excited atoms decreases exponentially to the limiting minimum value (about 3%). At this value, the viscosity increases to a critical value (about 1012 Pa s), which corresponds to the glass transition temperature, i.e., the temperature of freezing the mobility of excited kinetic units. The temperature dependence of the free activation energy of viscous flow in the glass transition range is specified by the temperature dependence of the relative number of excited atoms.

Photoproduction of electron-positron pairs in bent single crystals

The process of photoproduction of electron-positron pairs in bent single crystals is considered in this paper. In particular, it is shown that the probability of the process for gamma-quanta with energies from 100 GeV on is significantly higher than the one in an amorphous medium. A possible scenario for the experimental validation of the process is discussed and the positive features of the photoproduction in bent crystals compared to straight ones are underlined from the point of view of possible applications.

Contribution of incoherent effects to the orientation dependence of bremsstrahlung from rapid electrons in crystal

The bremsstrahlung cross section for relativistic electrons in a crystal is split into the sum of coherent and incoherent parts (the last is due to a thermal motion of atoms in the crystal). Although the spectrum of incoherent radiation in crystal is similar to one in amorphous medium, the incoherent radiation intensity could demonstrate substantial dependence on the crystal orientation due to the electrons' flux redistribution in the crystal. In the present paper we apply our method of the incoherent bremsstrahlung simulation developed earlier to interpretation of some recent experimental results obtained at the Mainz Microtron MAMI.

ADVANCES IN COHERENT BREMSSTRAHLUNG AND LPM-EFFECT STUDIES

2008 accomplished the 100thanniversary from the birth of L.D. Landau (Nobel Prize 1962). In the paper a short description of Kharkov period of Landau's work from 1932 to 1937 is given. One of areas of his work is connected with investigation of bremsstrahlung by ultra relativistic electrons in matter. In this paper a short review of the results obtained studying both Landau-Pomeranchuk-Migdal effect and coherent radiation by high-energy electrons and positrons in crystals, is given. The main attention is paid to the general properties and difference of radiation processes in amorphous media and in a crystal and to advances in the coherent bremsstrahlung studies.

Composable continuous-space programs for robotic swarms

Programmability is an increasingly important barrier to the deployment of multi-robot systems, as no prior approach allows routine composition and reuse of general aggregate behaviors. The Proto spatial computing language, however, already provides this sort of aggregate behavior programming for non-mobile systems using an abstraction of the network as a continuous-space-filling device. We extend this abstraction to mobile systems and show that Proto can be applied to multi-robot systems with an actuator that turns a vector field into device motion. Proto programs operate on fields of values over an abstract device called the amorphous medium and can be joined together using functional composition. These programs are then automatically transformed for execution by individual devices, producing an approximation of the specified continuous-space behavior. We are thus able to build up a library of simple swarm behaviors, and to compose them together into highly succinct programs that predictably produce the desired complex swarm behaviors, as demonstrated in simulation and on a group of 40 iRobot SwarmBots.

Picosecond and femtosecond X-ray absorption spectroscopy of molecular systems

The need to visualize molecular structure in the course of a chemical reaction, a phase transformation or a biological function has been a dream of scientists for decades. The development of time-resolved X-ray and electron-based methods is making this true. X-ray absorption spectroscopy is ideal for the study of structural dynamics in liquids, because it can be implemented in amorphous media. Furthermore, it is chemically selective. Using X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) in laser pump/X-ray probe experiments allows the retrieval of the local geometric structure of the system under study, but also the underlying photoinduced electronic structure changes that drive the structural dynamics. Recent developments in picosecond and femtosecond X-ray absorption spectroscopy applied to molecular systems in solution are reviewed: examples on ultrafast photoinduced processes such as intramolecular electron transfer, low-to-high spin change, and bond formation are presented.

Au nanoparticles doped ZrTiO4 films and hydrogen gas induced Au-plasmon shifting

Au nanoparticle (NP) doped ZrTiO4 films were prepared on glass substrates using the sol–gel process and characterized. An increase of annealing temperature of the doped film from 400 to 800 °C caused growth of the Au NPs from about 7 nm to 17 nm in size, respectively. The matrix ZrTiO4 remained amorphous up to 600 °C and transformed into highly crystalline (orthorhombic) form at 800 °C. The 400 °C annealed Au doped amorphous film showed remarkable blue-shifting (10–11 nm) of the Au surface plasmon resonance (Au-SPR) band in H2 gas (1 and 0.1% in Ar) at 200 °C with appreciable enhancement of optical density (OD). The shifting as well as enhancement of OD of Au-SPR can be reversibly switched between H2 gas (1–0.1%) and air, and found to be repeatable for several cycles. On the contrary, the Au NP doped crystalline ZrTiO4 film showed less shifting (4–5 nm) of Au-SPR with insignificant difference in OD value after exposure in H2 gas at 200–350 °C. The reversible dynamic responses of the transmittance data of Au-SPR in cases of 400 °C annealed films towards H2 gas and air showed quick response and recovery times at the operating temperature 200 °C. Large Au-SPR shifting in H2 with significant OD enhancement can be related to the increase of electron transfer on Au NPs facilitating through the embedding amorphous ZrTiO4 medium.

Electron-phonon interaction in non-polar quantum dots induced by the amorphous polar environment

We propose a Fröhlich-type electron-phonon interaction mechanism for carriers confined in a non-polar quantum dot surrounded by an amorphous polar environment. Carrier transitions under this mechanism are due to their interaction with the oscillating electric field induced by the local vibrations in the surrounding amorphous medium. We estimate the corresponding energy relaxation rate for electrons in Si nanocrystals embedded in a SiO2 matrix as an example. When the nanocrystal diameter is larger than 4 nm then the gaps between the electron energy levels of size quantization are narrow enough to allow for transitions accompanied by emission of a single local phonon having the energy about 140 meV. In such Si/SiO2 nanocrystals the relaxation time is in nanosecond range.

Particle collision frequency and particle density at equilibrium. I

The subject of the present paper is the formation of multiatomic particles such as clusters and nanoparticles. The probability for collision of two particles in an amorphous medium at equilibrium is derived and the particle frequency of collision per unit volume per unit time has been evaluated. Within the frame of given assumptions and approximations, the equilibrium density of two- and three-atomic particles in the medium has been assessed. This approach may be significant in the investigation of the process of new phase nuclei formation. The existence of a limit value of the particle size for coalescence is supposed by this approach.

Investigation of the Physicochemical Changes Preceding Zeolite Nucleation in a Sodium-Rich Aluminosilicate Gel

All industrially available zeolites are obtained from hydrogel systems. Unfortunately the level of understanding of the events preceding zeolite crystallization is far from satisfactory. In this respect, revealing the nature of the processes taking place in the precursor gel is of paramount importance to understanding zeolite nucleation. The investigation of the gel structure, however, is a difficult task due to the complexity of the object in terms of both composition and topology. Therefore, a combination of hyperpolarized (HP) (129)Xe NMR-N(2) adsorption-high-resolution transmission electron microscopy-energy-dispersive spectrometry methods complemented by X-ray diffraction, infrared spectroscopy, scanning electron microscopy, and chemical analyses has been employed to study the changes in composition and structure of sodium hydroxide rich aluminosilicate gel yielding zeolite A. The role of each component in the system and the entire sequence of events during the induction, nucleation, and crystallization stages have been revealed. The high concentration of sodium hydroxide in the studied system has been found to control the size and structure of the gel particles in the beginning stage. During the initial polymerization of aluminosilicate species a significant part of the sodium hydroxide is expelled from the gel into the solution, which restricts extensive polymerization and leads to formation of small aluminosilicate particles with open pore structure. The induction period that follows is marked by incorporation of Na back in the bulk gel. The combined action of the Na ion as a structure-directing agent and the hydroxyl group as a mobilizer results in partial depolymerization of the gel and formation of voids with mesopore sizes. The nucleation maximum coincides temporally with development of pores with sizes in the range of 2-5 nm. The amorphous gel undergoes into crystalline zeolite only after these pores have disappeared and the chemistry of the gel has evolved to reach the stoichiometric zeolite composition. It was established unambiguously by high-resolution transmission electron microscopy and HP (129)Xe NMR that the nucleation of zeolite occurs in the solid part of the system and the succeeding crystallization commences only after the nuclei are released into the liquid, which is consistent with the autocatalytic mechanism. Also this investigation has demonstrated the unrivaled sensitivity of HP (129)Xe NMR that is capable of identifying presence of small amounts of crystalline zeolite material in amorphous medium with detection limit extending below 1 wt %.

Electroproduction of electron–positron pair in oriented crystal at high energy

The process of electroproduction of the electron–positron pair by high energy electron in an oriented single crystal is investigated. Two contributions are considered: the direct (one-step) process via the virtual intermediate photon and the cascade (two-step) process when the electron emits the real photon moving in the field of axis and afterwards the photon converts into the pair. The spectrum of created positron (electron) is found. It is shown that the probability of the process is strongly enhanced comparing with the corresponding amorphous medium.

Meltdown of palladium nanoparticles due to prolonged hydrogen ion bombardment

Nanometric crystalline particles of palladium are known to form on polycrystalline palladium under the bombardment of low-energy hydrogen ions. Mostly, the Pd particles disperse on an amorphous medium or in a matrix protruding from the target surface. Here evidence is presented that Pd nanoparticles originally present on the matrix surface are liquefied by bombarding hydrogen ions. The macroscopic target temperature for this to occur is around one-third of the melting point of Pd. This phenomenon is too unfamiliar to be described in terms of existing scientific models and an as-yet unknown process might underlie its occurrence.

Ultrafast heating and resolution of recorded crystalline marks in phase-change media

This work presents an analytical study of the thermally activated amorphous-to-crystalline phase-change process when the heating source has a delta function temporal profile. This simulates the case of ultrafast heating where crystallization in the amorphous phase-change medium occurs during cooling. The study produced closed-form expressions that predict the necessary peak temperature, and hence energy density, in the phase-change medium for successful crystallization during ultrafast annealing as functions of the kinetic and thermal parameters of the medium. Closed-form expressions were also derived that provide estimates of the final crystalline mark widths and tail lengths when phase change has ceased. The analysis indicated the need to reduce the activation energy of crystallization and the thermal diffusivity of the medium to reduce the initial peak temperature, produced by the heating source, to avoid melting, to increase the crystallization rate, to achieve sufficient levels of crystalline fractions during cooling, and to reduce the size of recorded crystalline marks. Perturbation analysis was carried out to study the effects of latent heat of crystallization during the fast kinetics phase. The result was reductions in the cooling rate of the phase-change material, thus requiring lower peak temperatures to achieve higher volumes of crystalline fraction. Nevertheless, the effects of heat release during crystallization were found to be modest for the class of current phase-change material used in data storage.

Preparation and optical study of Au nanograins in amorphous La-oxide medium

Gold-incorporated lanthanum oxide films have been prepared by the vacuum evaporation method on glass and silicon substrates. Samples were investigated by X-ray fluorescence, X-ray diffraction, UV–vis–NIR absorption spectroscopy, and DC-electrical measurements. Sample with molar incorporation level of about 4% consists of Au-nanograins (4.5 nm) embedded in amorphous La-oxide and exhibits insulating properties. Sample with molar incorporation level of 7% consists of Au-nanograins (15 nm) embedded in amorphous La-oxide and exhibits conducting behaviour, which refers to an insulator–metal (I–M) transform. The I–M transform was explained due to the band overlapping effect.

Application of the anisotropic bond model to second-harmonic generation from amorphous media

As a step toward analyzing second-harmonic generation (SHG) from crystalline Si nanospheres in glass, we develop an anisotropic bond model (ABM) that expresses SHG in terms of physically meaningful parameters and provide a detailed understanding of the basic physics of SHG on the atomic scale. Nonlinear-optical (NLO) responses are calculated classically via the four fundamental steps of optics: evaluate the local field at a given bond site, solve the force equation for the acceleration of the charge, calculate the resulting radiation, then superpose the radiation from all charges. Because the emerging NLO signals are orders of magnitude weaker and occur at wavelengths different from that of the pump beam, these steps are independent. Paradoxically, the treatment of NLO is therefore simpler than that of linear optics (LO), where these calculations must be done self-consistently. The ABM goes beyond previous bond models by including the complete set of underlying contributions: retardation (RD), spatial-dispersion (SD), and magnetic (MG) effects, in addition to the anharmonic restoring force acting on the bond charge. Transverse as well as longitudinal motion is also considered. We apply the ABM to obtain analytic expressions for SHG from amorphous materials under Gaussian-beam excitation. These materials represent an interesting test case not only because they are ubiquitous but also because the anharmonic-force contribution that dominates the SHG response of crystalline materials and ordered interfaces vanishes by symmetry. The remaining contributions, and hence the SHG signals, are entirely functions of the LO response and beam geometry, so the only new information available is the anisotropy of the LO response at the bond level. The RD, SD, and MG contributions are all of the same order of magnitude, so none can be ignored. Diffraction is important in determining not only the pattern of the emerging beam but also the phases and amplitudes of the different terms. The plane-wave expansion that gives rise to electric quadrupole magnetic dipole effects in LO appears here as retardation. Using the paraxial-ray approximation, we reduce the results to the isotropic case in two limits, that where the linear restoring force dominates (glasses) and that where it is absent (metals). Both forward- and backscattering geometries are discussed. Estimated signal strengths and conversion efficiencies for fused silica appear to be in general agreement with data where available. Predictions that allow additional critical tests of these results are made.

Defect-Induced Photoluminescence of Powdered Silica Glass

Visible photoluminescence was generated in standard soda-lime-silica glass powder, mechanically milled in a high-energy attrition mill. The broad emission band maximum shows a linear dependence on the exciting wavelength, suggesting the possibility to tune the PL emission. The photoluminescence was attributed to defect generation related to unsatisfied chemical bonds due to the high surface area. Raman scattering and ultraviolet-visible optical reflectance measurements corroborate this assertion. Transmission electron microscopy measurements indicate that the powder is composed by nanocrystallites with about 10-20 nanometers immersed in an amorphous media.

Enhanced multiple scattering in crystals with effective LR length in the micron range

Multiple Coulomb scattering in amorphous media can be characterised by radiation length LR. We find in computer simulations that particles can scatter in bent crystal lattices with effective LR length down to a few microns or up to 700 times shorter than in the corresponding amorphous media. The effect exists only within the angular range of the bent crystal arc. Outside this range LR is back to normal value. This makes the crystal a material with unique enhanced multiple scattering property easily switched on/off. We derive a theoretical estimate independent of energy for the effective LR that is in agreement with our simulations for C, Si, Ge and W crystal lattices. We show that in the ongoing collimation experiment at the Tevatron a crystal-based “super-scattering material” could outperform a channeling crystal in collimation efficiency reducing the local background rate by a factor of 40. The introduced “enhanced multiple scattering” materials could serve for new approaches to beam collimation in accelerators, especially at the high-energy frontier machines like the LHC and ILC.

Plastic response of a two-dimensional amorphous solid to quasistatic shear: Transverse particle diffusion and phenomenology of dissipative events

We perform extensive simulations of a two-dimensional Lennard-Jones glass subjected to quasistatic shear deformation at T=0. We analyze the distribution of nonaffine displacements in terms of contributions of plastic, irreversible events, and elastic, reversible motions. From this, we extract information about correlations between plastic events and about the elastic nonaffine noise. Moreover, we find that nonaffine motion is essentially diffusive, with a clearly size-dependent diffusion constant. These results, supplemented by close inspection of the evolving patterns of the nonaffine tangent displacement field, lead us to propose a phenomenology of plasticity in such amorphous media. It can be schematized in terms of elastic loading and irreversible flips of small, randomly located shear transformation zones, elastically coupled via their quadrupolar fields.

Dispersion of acoustic-like and optic-like vibrational excitations in Ni2B metallic glass

The dynamic structure factor S(Q, E) of Ni2B metallic glass was studied by inelastic neutron scattering in the ranges of momentum transfers 0.7 < ħQ/A−1 < 7, and energy, 2 < E/meV < 70, transfers. The measurements were performed with the IN4 spectrometer (Institut Laue-Langevin (ILL), Grenoble, France) on three samples of the same chemical composition but with different contents of Ni and B isotopes, as a result of which partial contributions were determined. The cuts through S(Q, E) for different values of E and Q demonstrated a characteristic behavior indicating that vibrational excitations, similar to acoustic and optical phonon excitations in crystals, propagate in an amorphous medium in a certain energy and momentum range.

Computer simulation of coherent interaction of charged particles and photons with crystalline solids at high energies

Monte Carlo simulation code has been developed and tested for studying the passage of charged particle beams and radiation through the crystalline matter at energies from tens of MeV up to hundreds of GeV. The developed Monte Carlo code simulates electron, positron and photon shower in single crystals and amorphous media. The Monte Carlo code tracks all the generations of charged particles and photons through the aligned crystal by taking into account the parameters of incoming beam, multiple scattering, energy loss, emission angles, transverse dimension of beams, and linear polarization of produced photons. The simulation results are compared with the CERN-NA-59 experimental data. The realistic descriptions of the electron and photon beams and the physical processes within the silicon and germanium single crystals have been implemented.