Probing charge screening dynamics and electrochemical processes at the solid–liquid interface with electrochemical force microscopy

The presence of mobile ions complicates the implementation of voltage-modulated scanning probe microscopy techniques such as Kelvin probe force microscopy (KPFM). Overcoming this technical hurdle, however, provides a unique opportunity to probe ion dynamics and electrochemical processes in liquid environments and the possibility to unravel the underlying mechanisms behind important processes at the solid–liquid interface, including adsorption, electron transfer and electrocatalysis. Here we describe the development and implementation of electrochemical force microscopy (EcFM) to probe local bias- and time-resolved ion dynamics and electrochemical processes at the solid–liquid interface. Using EcFM, we demonstrate contact potential difference measurements, consistent with the principles of open-loop KPFM operation. We also demonstrate that EcFM can be used to investigate charge screening mechanisms and electrochemical reactions in the probe–sample junction. We further establish EcFM as a force-based imaging mode, allowing visualization of the spatial variability of sample-dependent local electrochemical properties.

Use of the γ-H2AX Assay to Investigate DNA Repair Dynamics Following Multiple Radiation Exposures

Radiation therapy is one of the most common and effective strategies used to treat cancer. The irradiation is usually performed with a fractionated scheme, where the dose required to kill tumour cells is given in several sessions, spaced by specific time intervals, to allow healthy tissue recovery. In this work, we examined the DNA repair dynamics of cells exposed to radiation delivered in fractions, by assessing the response of histone-2AX (H2AX) phosphorylation (γ-H2AX), a marker of DNA double strand breaks. γ-H2AX foci induction and disappearance were monitored following split dose irradiation experiments in which time interval between exposure and dose were varied. Experimental data have been coupled to an analytical theoretical model, in order to quantify key parameters involved in the foci induction process. Induction of γ-H2AX foci was found to be affected by the initial radiation exposure with a smaller number of foci induced by subsequent exposures. This was compared to chromatin relaxation and cell survival. The time needed for full recovery of γ-H2AX foci induction was quantified (12 hours) and the 1:1 relationship between radiation induced DNA double strand breaks and foci numbers was critically assessed in the multiple irradiation scenarios.

Dynamics of excess electronic charge in aliphatic ionic liquids containing the bis(trifluoromethylsulfonyl)amide anion

In a recent article (J. Am. Chem. Soc. 2011, 133, 20186) we investigated the initial spatial distribution of dry excess electrons in a series of room-temperature ionic liquids (RTILs). Perhaps unexpectedly, we found that in some alkylammonium-based systems the excess negative charge resided on anions and not on the positive cations. Following on these results, in the current paper we describe the time evolution of an excess electronic charge introduced in alkylammonium- and pyrrolidinium-based ionic liquids coupled with the bis(trifluoromethylsulfonyl)amide ([TfN]) anion. We find that on a 50 fs time scale an initially delocalized excess electron localizes on a single [TfN] anion which begins a fragmentation process. Low-energy transitions have a very different physical origin on the several femtoseconds time scale when compared to what occurs on the picosecond time scale. At time zero, these are intraband transitions of the excess electron. However after 40 fs when the excess electronic charge localizes on a single anion, these transitions disappear, and the spectrum is dominated by electron-transfer transitions between the fragments of the doubly charged breaking anion. © 2013 American Chemical Society.

Effect of magnetic bias on Gaussian pulse scattering by stacked nonlinear semiconductor layers

The nonlinear scattering of pulses by periodic stacks of semiconductor layers with magnetic bias has been studied in the self-consistent problem formulation, taking into account mobility of carriers. The three-wave mixing technique has been applied to the analysis of the waveform evolution in the stacks illuminated by two Gaussian pulses with different central frequencies and lengths. The effects of external magnetic bias, and stack physical and geometrical parameters on the properties of the scattered waveforms are discussed. © 2013 IEEE.

Three-mode entanglement by interlinked nonlinear interactions in optical chi((2)) media

We address the generation of fully inseparable three-mode entangled states of radiation by interlinked nonlinear interactions in chi((2)) media. We show how three-mode entanglement can be used to realize symmetric and asymmetric telecloning machines, which achieve optimal fidelity for coherent states. An experimental implementation involving a single nonlinear crystal in which the two interactions take place simultaneously is suggested. Preliminary experimental results showing the feasibility and the effectiveness of the interaction scheme with a seeded crystal are also presented. (C) 2004 Optical Society of America.

Micromaser spectrum and phase diffusion dynamics

We discuss a scheme to relate the phase diffusion dynamics of the micromaser field to the measured atomic population statistics. This can allow us to measure the linewidth of the micromaser spectrum and to solve a relevant decoherence problem in cavity quantum electrodynamics. The main steps are (i) a suitable preparation of the cavity field state to generate coherences, (ii) the transfer of information on the dynamics of field coherences to probe atoms by the action of an external resonant coherent field and (iii) the derivation of the phase diffusion rate, hence the micromaser linewidth, from the measured population statistics of the probe atoms. The method can be applied even in the presence of trapping states, where peculiar linewidth oscillations are expected for increasing pump rate, due to the quantum nature of the micromaser field.

How to measure the phase diffusion dynamics in the micromaser

We propose a realistic scheme for measuring the micromaser linewidth by monitoring the phase diffusion dynamics of the cavity field. Our strategy consists of exciting an initial coherent state with the same photon number distribution as the micromaser steady-state field, singling out a purely diffusive process in the system dynamics. After the injection of a counterfield, measurements of the population statistics of a probe atom allow us to derive the micromaser linewidth in all ranges of the relevant parameters, establishing experimentally the distinctive features of the micromaser spectrum due to the discreteness of the electromagnetic field.

Malthusian Dynamics in a Diverging Europe: Northern Italy, 1650–1881

Recent empirical research questions the validity of using Malthusian theory in preindustrial England. Using real wage and vital rate data for the years 1650–1881, I provide empirical estimates for a different region: Northern Italy. The empirical methodology is theoretically underpinned by a simple Malthusian model, in which population, real wages, and vital rates are determined endogenously. My findings strongly support the existence of a Malthusian economy wherein population growth decreased living standards, which in turn influenced vital rates. However, these results also demonstrate how the system is best characterized as one of weak homeostasis. Furthermore, there is no evidence of Boserupian effects given that increases in population failed to spur any sustained technological progress.

Vibration based seismic damage identification procedure for a steel concentrically braced frame structure

An approach for seismic damage identification of a single-storey steel concentrically braced frame (CBF) structure is presented through filtering and double integration of a recorded acceleration signal. A band-pass filter removes noise from the acceleration signal followed by baseline correction being used to reduce the drift in velocity and displacement during numerical integration. The pre-processing achieves reliable numerical integration that predicts the displacement response accurately when compared to the measured lateral in-plane displacement of the CBF structure. The lateral displacement of the CBF structure is used to infer buckling and yielding of bracing members through seismic tests. The level of interstorey drift of the CBF during a seismic excitation allows the yield and buckling of the bracing members to be identified and indirectly detects damage based on exceedance of calculated displacement limits. The calculated buckling and yielding displacement threshold limits used to identify damage are demonstrated to accurately identify initial buckling and yielding in the bracing members.

Mantle flow, volatiles, slab-surface temperatures and melting dynamics in the north Tonga arc-Lau back-arc basin

The Fonualei Spreading Center affords an excellent opportunity to evaluate geochemical changes with increasing depth to the slab in the Lau back-arc basin. We present H2O and CO2 concentrations and Sr, Nd, Pb, Hf and U-Th-Ra isotope data for selected glasses as well as new Hf isotope data from boninites and seamounts to the north of the Tonga arc. The Pb and Hf isotope data are used to show that mantle flow is oriented to the southwest and that the tear in the northern end of the slab may not extend east as far as the boninite locality. Along the Fonualei Spreading Center, key geochemical parameters change smoothly with increasing distance from the arc front and increasing slab surface temperatures. The latter may range from 720 to 866 degrees C, based on decreasing H2O/Ce ratios. Consistent with experimental data, the geochemical trends are interpreted to reflect changes in the amount and composition of wet pelite melts or super-critical fluids and aqueous fluids derived from the slab. With one exception, all of the lavas preserve both U-238 excesses and Ra-226 excesses. We suggest that lavas from the Fonualei Spreading Center and Valu Fa Ridge are dominated by fluid-fluxed melting whereas those from the East and Central Lau Spreading Centers, where slab surface temperatures exceed similar to 850-900 degrees C, are largely derived through decompression. A similar observation is found for the Manus and East Scotia back-arc basins and may reflect the expiry of a key phase such as lawsonite in the subducted basaltic crust.

Reconfigurable Long-Range Phonon Dynamics in Optomechanical Arrays

We investigate periodic optomechanical arrays as reconfigurable platforms for engineering the coupling between multiple mechanical and electromagnetic modes and for exploring many-body phonon dynamics. Exploiting structural resonances in the coupling between light fields and collective motional modes of the array, we show that tunable effective long-range interactions between mechanical modes can be achieved. This paves the way towards the implementation of controlled phononic walks and heat transfer on densely connected graphs as well as the coherent transfer of excitations between distant elements of optomechanical arrays.

Prediction of Transonic LCOs using an Aeroelastic Harmonic Balance Method

This work proposes a novel approach to compute transonic Lim
it Cycle Oscillations using high fidelity analysis. CFD based Harmonic Balance methods have proven to be efficient tools to predict periodic phenomena. This paper’s contribution is to present a new methodology to determine the unknown frequency of oscillations, enabling HB methods to accurately capture Limit Cycle Oscillations (LCOs); this is achieved by defining a frequency updating procedure based on a coupled CFD/CSD Harmonic Balance formulation to find the LCO condition. A pitch/plunge aerofoil and delta wing aerodynamic and respective linear structural models are used to validate the new method against conventional time-domain simulations. Results show consistent agreement between the proposed and time-marching methods for both LCO amplitude and frequency, while producing at least one order of magnitude reduction in computational time.

Generalized Langevin equation: An efficient approach to nonequilibrium molecular dynamics of open systems

The generalized Langevin equation (GLE) has been recently suggested to simulate the time evolution of classical solid and molecular systems when considering general nonequilibrium processes. In this approach, a part of the whole system (an open system), which interacts and exchanges energy with its dissipative environment, is studied. Because the GLE is derived by projecting out exactly the harmonic environment, the coupling to it is realistic, while the equations of motion are non-Markovian. Although the GLE formalism has already found promising applications, e. g., in nanotribology and as a powerful thermostat for equilibration in classical molecular dynamics simulations, efficient algorithms to solve the GLE for realistic memory kernels are highly nontrivial, especially if the memory kernels decay nonexponentially. This is due to the fact that one has to generate a colored noise and take account of the memory effects in a consistent manner. In this paper, we present a simple, yet efficient, algorithm for solving the GLE for practical memory kernels and we demonstrate its capability for the exactly solvable case of a harmonic oscillator coupled to a Debye bath.