Annihilation Dynamics Research Articles

Simulation study on defect annihilation dynamics in directed self-assembly lithography

The authors have investigated the defect annihilation dynamics of the grid defects, which are one of the characteristic pattern defects in directed self-assembly lithography, using a simulation method based on self-consistent field theory (SCFT) and dissipative particle dynamics (DPD). First, the mesoscopic morphologies of metastable grid defects using SCFT were calculated. Then, the SCFT simulation result was transformed into the particle representation using the node density biased Monte Carlo method. Next the authors monitored the chronological change of the conformation of the diblock copolymer (BCP) chains during the defect annihilation process using DPD. By DPD simulation, the characteristic changes of the chain conformations of BCP immediately above the bottom neutral layer have been observed. Polymer chains immediately above the bottom were found to be (1) partially vertical to the bottom in the initial defective state conditions, (2) randomly oriented in the intermediate transient state, and (3) parallel to the bottom in the equilibrium lamellar state.

Controlling Positronium Annihilation with Electric Fields.

We show that the annihilation dynamics of excited positronium (Ps) atoms can be controlled using parallel electric and magnetic fields. To achieve this, Ps atoms were optically excited to n=2 sublevels in fields that were adjusted to control the amount of short-lived and long-lived character of the resulting mixed states. Inclusion of the former offers a practical approach to detection via annihilation radiation, whereas the increased lifetimes due to the latter can be exploited to optimize resonance-enhanced two-photon excitation processes (e.g., 1^{3}S→2^{3}P→nS/nD), either by minimizing losses through intermediate state decay, or by making it possible to separate the excitation laser pulses in time. In addition, photoexcitation of mixed states with a 2^{3}S_{1} component represents an efficient route to producing long-lived pure 2^{3}S_{1} atoms via single-photon excitation.

Exciton dynamics of C60-based single-photon emitters explored by Hanbury Brown-Twiss scanning tunnelling microscopy.

Exciton creation and annihilation by charges are crucial processes for technologies relying on charge-exciton-photon conversion. Improvement of organic light sources or dye-sensitized solar cells requires methods to address exciton dynamics at the molecular scale. Near-field techniques have been instrumental for this purpose; however, characterizing exciton recombination with molecular resolution remained a challenge. Here, we study exciton dynamics by using scanning tunnelling microscopy to inject current with sub-molecular precision and Hanbury Brown–Twiss interferometry to measure photon correlations in the far-field electroluminescence. Controlled injection allows us to generate excitons in solid C60 and let them interact with charges during their lifetime. We demonstrate electrically driven single-photon emission from localized structural defects and determine exciton lifetimes in the picosecond range. Monitoring lifetime shortening and luminescence saturation for increasing carrier injection rates provides access to charge-exciton annihilation dynamics. Our approach introduces a unique way to study single quasi-particle dynamics on the ultimate molecular scale.

Spatial resolution versus data acquisition efficiency in mapping an inhomogeneous system with species diffusion.

Traditionally, spatially-resolved photoluminescence (PL) has been performed using a point-by-point scan mode with both excitation and detection occurring at the same spatial location. But with the availability of high quality detector arrays like CCDs, an imaging mode has become popular for performing spatially-resolved PL. By illuminating the entire area of interest and collecting the data simultaneously from all spatial locations, the measurement efficiency can be greatly improved. However, this new approach has proceeded under the implicit assumption of comparable spatial resolution. We show here that when carrier diffusion is present, the spatial resolution can actually differ substantially between the two modes, with the less efficient scan mode being far superior. We apply both techniques in investigation of defects in a GaAs epilayer – where isolated singlet and doublet dislocations can be identified. A superposition principle is developed for solving the diffusion equation to extract the intrinsic carrier diffusion length, which can be applied to a system with arbitrarily distributed defects. The understanding derived from this work is significant for a broad range of problems in physics and beyond (for instance biology) – whenever the dynamics of generation, diffusion, and annihilation of species can be probed with either measurement mode.

Vortex-antivortex dynamics in mesoscopic symmetric and asymmetric superconducting loops with an applied ac current

In the framework of the time-dependent Ginzburg-Landau formalism, we study the dynamics of vortex-antivortex (V-Av) pairs in mesoscopic symmetric and asymmetric superconducting loops under an applied ac current. In contrast to the case of a constant biasing dc current, the process of the V-Av collision and annihilation is strongly affected by the time-periodic ac signal. As the direction of the applied ac current is reversed, the existed V-Av pair moves backward and then collides with a new created Av-V pair in a symmetric loop. In the presence of an appropriate external magnetic field, a novel sinusoidal-like oscillatory mode of the magnetization curve is observed, and the periodic dynamical process of the V-Av annihilation occurs in both branches of the sample. Moreover, for the asymmetric sample with an off-centered hole the creation point of the V-Av pair shifts away from the center of the sample, and the creation and annihilation dynamics of V-Av pairs turns out to be very different from the symmetric case.

Dynamical behaviors of nonlinear dust acoustic waves: From plane waves to dust acoustic wave turbulence

The dust acoustic wave (DAW), associated with longitudinal dust oscillations in dusty plasmas, can be self-excited from the free energy of ion streaming. It is not only a fundamental plasma wave but also a paradigm to understand the generic dynamical behaviors of self-excited nonlinear longitudinal density waves through optically monitoring particle motion and dust density evolutions over a large area. In this paper, the dynamical behaviors of the wave-particle interaction and wave breaking in ordered self-excited DAW with straight wave fronts, and the defect-mediated wave turbulence with fluctuating defects and chaotic low amplitude hole filaments along defect trajectories in the 2+1D space-time space, are briefly reviewed. The first experimental observation of acoustic vortices with helical waveforms in self-excited acoustic-type defect-mediated wave turbulence, and the dynamics of spontaneous pair generation, propagation, and pair annihilation of acoustic vortices, is demonstrated and discussed.

Vortex–antivortex annihilation in mesoscopic superconductors with a central pinning center

In this work we solved the time-dependent Ginzburg–Landau equations, TDGL, to simulate two superconducting systems with different lateral sizes and with an antidot inserted in the center. Then, by cycling the external magnetic field, the creation and annihilation dynamics of a vortex–antivortex pair was studied as well as the range of temperatures for which such processes could occur. We verified that in the annihilation process both vortex and antivortex acquire an elongated format while an accelerated motion takes place.

Annihilation dynamics of stringlike topological defects in a nematic lyotropic liquid crystal

Topological defects can appear whenever there is some type of ordering. Its ubiquity in nature has been the subject of several studies, from early Universe to condensed matter. In this work, we investigated the annihilation dynamics of defects and antidefects in a lyotropic nematic liquid crystal (ternary mixture of potassium laurate, decanol and deionized–destillated water) using the polarized optical light microscopy technique. We analyzed Schlieren textures with topological defects produced due to a symmetry breaking in the transition of the isotropic to nematic calamitic phase after a temperature quench. As result, we obtained for the distance D between two annihilating defects (defect–antidefect pair), as a function of time t remaining for the annihilation, the scaling law D ∝ tα, with α = 0.390 and standard deviation σ = 0.085. Our findings go in the direction to extend experimental results related to dynamics of defects in liquid crystals since only thermotropic and polymerics ones had been investigated. In addition, our results are in good quantitative agreement with previous investigations on the subject.

Velocity Correlations in an Active Nematic

The flow properties of a continuum model for an active nematic are studied and compared with recent experiments on suspensions of microtubule bundles and molecular motors. The velocity correlation length is found to be independent of the strength of the activity while the characteristic velocity scale increases monotonically as the activity is increased, both in agreement with the experimental observations. We interpret our results in terms of the creation and annihilation dynamics of a gas of topological defects.

Defect Annihilation and Proliferation in Active Nematics

Liquid crystals inevitably possess topological defect excitations generated through boundary conditions, through applied fields, or in quenches to the ordered phase. In equilibrium, pairs of defects coarsen and annihilate as the uniform ground state is approached. Here we show that defects in active liquid crystals exhibit profoundly different behavior, depending on the degree of activity and its contractile or extensile character. While contractile systems enhance the annihilation dynamics of passive systems, extensile systems act to drive defects apart so that they swarm around in the manner of topologically well-characterized self-propelled particles. We develop a simple analytical model for the defect dynamics which reproduces the key features of both the numerical solutions and recent experiments on microtubule-kinesin assemblies.

Separating Annihilation and Excitation Energy Transfer Dynamics in Light Harvesting Systems

The dependence of excitation energy transfer kinetics on the electronic state of the acceptor (ground vs excited) has been resolved with a novel multipulse prePump-Pump-Probe spectroscopy. The primary energy transfer and annihilation dynamics in two model light-harvesting systems were explored: an artificially synthesized carotenoid-zinc-phthalocyanine dyad and a naturally occurring light-harvesting peridinin-chlorophyll protein complex from Amphidinium carterae. Both systems use carotenoid as the primary excitation energy donor with porphyrin chromophores as the acceptor molecules. The prePump-Pump-Probe transient signals were analyzed with Monte Carlo modeling to explicitly address the underlying step-by-step kinetics involved in both excitation migration and annihilation processes. Both energy transfer and annihilation dynamics were demonstrated to occur with approximately the same rate in both systems, regardless of the excitation status of the acceptor pigments. The possible reasons for these observations are discussed in the framework of the Förster energy transfer model.

Exciton Annihilation and Dissociation Dynamics in Group II–V Cd3P2 Quantum Dots

Semiconductor quantum dots (QDs) have emerged as a new class of light harvesting materials for solar energy conversion due to their unique size-dependent properties. Most recent studies have focused on II-VI group (such as CdX, X = S, Se, and Te) QDs and lead salt (such as PbS, PbSe, and PbTe) QDs. In this paper, we investigate exciton dissociation and annihilation dynamics of Cd3P2 QDs, a low bulk band gap (0.55 eV) II-V group material, to explore their potential application as a light harvesting component for photoreduction systems. For Cd3P2 QDs with 1S exciton band at 650 nm, a long-lived single exciton state with lifetime of 259 ns and a high emission quantum yield of 65% were observed. In Cd3P2 QD-rhodamine B (RhB, an electron acceptor) complexes, excitons in QDs could be dissociated by ultrafast electron transfer to RhB (6.2 ps), and the charge separated state had a long lifetime (31 ns). Although the photoinduced electron transfer rate in QD-RhB complexes decreased with increasing QD size, electron transfer was observed in QDs with 1S exciton bands at wavelength as long as 1050 nm. Compared with CdSe and PbS, Cd3P2 QDs with both more strongly reducing excited states and broader absorption in the visible and near IR region can be readily achieved, making them potential photosensitizers for photodriven water or CO2 reduction reactions.

Cell Gap Dependence of Nematic Backflow around Annihilating Disclination Pair

This paper reports an experimental study of the dynamics of s = ±1/2 disclinations in the nematic liquid crystalline (LC) phase of 4-cyano-4'- n -pentylbiphenyl (5CB) under strong anchoring condition. The backflow brings asymmetry in annihilation dynamics of disclinations. To reveal the surface effect on backflow, we observed the motion of disclination pair for a various cell gap d . Although the velocity ratio of s = ±1/2 disclinations is comparable with a theoretical prediction, it decreased around the cell gap d = 1 µm when velocity ratio was reduced. This observation shows that the backflow is suppressed in the LC cell with d = 1 µm. The anchoring effect is analyzed through a model calculation within an elastic theory.

Manipulating the Annihilation Dynamics of Positronium via Collective Radiation

A method is investigated to manipulate the annihilation dynamics of a dense gas of positronium atoms employing superradiance and subradiance regimes of the cooperative spontaneous emission of the system. The corresponding annihilation dynamics is explored in two setups with regard to its fundamental novel properties and controlled by the gas density and by the intensity of a driving strong resonant laser field. In particular, the method allows us to increase the annihilation lifetime of an ensemble of positronium atoms by trapping the atoms in the excited state via collective radiative effects in the resonant laser field. In the second setup, the effect is enhanced by employing a cavity field. The maximum lifetime increase is by a factor of about 200 for para-positronium and by a factor of about 100 for ortho-positronium.

Positron annihilation and relaxation dynamics from dielectric spectroscopy: poly(vinylmethylether)

We report on the temperature dependence of the lifetime of the ortho-positronium (o-Ps), τ3, annihilation in amorphous polymer poly(vinylmethylether) (PVME) from positron annihilation lifetime spectroscopy (PALS). We show that the behavior of τ3(T) can be divided into five regions, each of them having a linear temperature dependence, and that the crossover PALS temperatures situated at , , and , and marking the discontinuity in the free volume microstructure are related to various dynamic features from neutron scattering (NS) and broadband dielectric spectroscopy (BDS). First, a slight change in the PALS response in the glassy PVME at is related to the onset of the excess wing in an apparent correspondence with the fast secondary β motion from NS. A further slight bend in the liquid state at is related to a high-frequency tail of the primary α process as well as to the slow secondary β relaxation from BDS. In addition, it lies also in the vicinity of the crossover temperature, , in the spectral dispersion of the primary α process, indicating a connection of the change in the o-Ps lifetime with the variation in the width of the primary α relaxation times distribution. Finally, the τ3 value at is close to the mean relaxation time of the primary α process, τα, in coincidence with the crossover in the secondary effective β process between two regimes in the liquid PVME. All these relationships point to very close connections between the PALS response and the dynamic behavior of PVME, which can be explained in terms of the temperature dependence of the probability function of the liquid-like and the solid-like domains, as obtained from the two-order parameter (TOP) model description of the liquid to glass transition in glass-formers.

Flux-quantum-discretized dynamics of magnetic flux entry, exit, and annihilation in current-driven mesoscopic type-I superconductors

We study nonlinear flux dynamics in a current-carrying type-I superconductor. The stray magnetic field of the current induces the intermediate state, where nucleation of flux domains is discretized to a single fluxoid at a time, while their final shape (tubular or laminar), size, and nucleation rate depend on applied current and edge conditions. The current induces opposite flux domains on opposite sides of the sample, and subsequently drives them to annihilation---which is also discretized, as a sequence of vortex-antivortex pairs. The discretization of both nucleation and annihilation leaves measurable traces in the voltage across the sample and in locally probed magnetization. The reported dynamic phenomena thus provide an unambiguous proof of a flux quantum being the smallest building block of the intermediate state in type-I superconductors.

Anisotropy in the annihilation dynamics of umbilic defects in nematic liquid crystals

Umbilic defects of strength s=±1 were induced in a nematic liquid crystal with negative dielectric anisotropy, confined to Hele-Shaw cells with homeotropic boundary conditions, and their annihilation dynamics followed experimentally. The speeds of individual defects of annihilating defect pairs with strengths of equal magnitude and opposite sign were determined as a function of several externally applied parameters, such as cell gap, electric field amplitude, frequency, and temperature. It was shown that annihilating defects do not approach each other at equal speeds, but that a speed anisotropy is observed, with the positive defect moving faster than the negative one. The defects move more slowly as the strength of the applied electric field or the cell gap is increased. The speed anisotropy is found to be essentially constant for varying external conditions which do not change the material properties of the liquid crystal material, i.e., confinement, electric field amplitude, or frequency. Only for applied conditions that change material properties, such as temperature changing viscosity, does the speed anisotropy vary. The annihilation dynamics was also simulated numerically giving good qualitative agreement with the experiments. Using insight gained from the simulations we interpret the defects' speed in terms of their overlap and the speed asymmetry as arising from backflow effects and anisotropy in the elastic constants.

Defect dynamics in crystalline buckled membranes

We study the dynamics of defect annihilation in flexible crystalline membranes suffering a symmetry-breaking phase transition. The kinetic process leading the system toward equilibrium is described through a Brazovskii-Helfrich-Canham Hamiltonian. In membranes, a negative disclination has a larger energy than a positive disclination. Here we show that this energetic asymmetry does not only affect equilibrium properties, like the Kosterlitz-Thouless transition temperature, but also plays a fundamental role in the dynamic of defects. Both unbinding of dislocations and Carraro-Nelson "antiferromagnetic" interactions between disclinations slow down the dynamics below the Lifshitz-Safran regime observed in flat hexagonal systems.

Positron annihilation and relaxation dynamics from dielectric spectroscopy and nuclear magnetic resonance: Cis–trans-1,4-poly(butadiene)

We report a joint analysis of positron annihilation lifetime spectroscopy (PALS), dielectric spectroscopy (BDS), and nuclear magnetic resonance (NMR) on cis-trans-1,4-poly(butadiene) (c-t-1,4-PBD). Phenomenological analysis of the orthopositronium lifetime τ(3)-T dependence by linear fitting reveals four characteristic PALS temperatures: T(b1)(G)=0.63T(g)(PALS), T(g)(PALS), T(b1)(L)=1.22T(g)(PALS), and T(b2)(L)=1.52T(g)(PALS). Slight bend effects in the glassy and supercooled liquid states are related to the fast or slow secondary β process, from neutron scattering, respectively, the latter being connected with the trans-isomers. In addition, the first bend effect in the supercooled liquid coincides with a deviation of the slow effective secondary β(eff) relaxation related to the cis-isomers from low-T Arrhenius behavior to non-Arrhenius one and correlates with the onset of the primary α process from BDS. The second plateau effect in the liquid state occurs when τ(3) becomes commensurable with the structural relaxation time τ(α)(T(b2)). It is also approximately related to its crossover from non-Arrhenius to Arrhenius regime in the combined BDS and NMR data. Finally, the combined BDS and NMR structural relaxation data, when analyzed in terms of the two-order parameter (TOP) model, suggest the influence of solidlike domains on both the annihilation behavior and the local and segmental chain mobility in the supercooled liquid. All these findings indicate the influence of the dynamic heterogeneity in both the primary and secondary relaxations due to the cis-trans isomerism in c-t-1,4-PBD and their impact into the PALS response.

Coarsening kinetics of a two-dimensional O(2) Ginzburg–Landau model: the effect ofreversible mode coupling

We investigate, via numerical simulations, the phase ordering kinetics of a two-dimensional soft spinO(2) Ginzburg–Landau model when a reversible mode coupling is included via the conservedconjugate momentum of the spin order parameter (Model E). Coarsening of the system,when quenched from a disordered state to zero temperature, is observed to be enhanced bythe existence of the mode coupling terms. The growth of the characteristic length scaleL(t) exhibits an effective superdiffusive growth exponent that can be interpretedas a positive logarithmic-like correction to a diffusive growth, i.e.,L(t) ∼ (tlnt)1/2. In order to understand this behavior, we introduced a simple phenomenological model ofcoarsening based on the annihilation dynamics of a vortex–antivortex pair, incorporatingthe effect of vortex inertia and logarithmically divergent mobility of the vortex. With asuitable choice of the parameters, numerical solutions of the simple model can fit the fullsimulation results very adequately. The effective growth exponent in the early time stage islarger due to the effect of the vortex inertia, which crosses over into the late time stagecharacterized by positive logarithmic correction to a diffusive growth. We alsoinvestigated the nonequilibrium autocorrelation function from which the so-calledλ exponent can be extracted. We get which is distinctly larger than the value of for the purely dissipative Model A dynamics of non-conservedO(2) models.