Quantum effect induced reverse kinetic molecular sieving in microporous materials

We report kinetic molecular sieving of hydrogen and deuterium in zeolite rho at low temperatures, using atomistic molecular dynamics simulations incorporating quantum effects via the Feynman-Hibbs approach. We find that diffusivities of confined molecules decrease when quantum effects are considered, in contrast with bulk fluids which show an increase. Indeed, at low temperatures, a reverse kinetic sieving effect is demonstrated in which the heavier isotope, deuterium, diffuses faster than hydrogen. At 65 K, the flux selectivity is as high as 46, indicating a good potential for isotope separation.

Time-evolution of highly localized positive-energy states of the free Dirac electron

Highly localized positive-energy states of the free Dirac electron are constructed and shown to evolve in a simple way under the action of Dirac's equation. When the initial uncertainty in position is small on the scale of the Compton wavelength, there is an associated uncertainty in the mean energy that is large compared with the rest mass of the electron. However, this does not lead to any breakdown of the one-particle description, associated with the possibility of pair-production, but rather leads to a rapid expansion of the probability density outwards from the point of localization, at speeds close to the speed of light.

High-fidelity measurement and quantum feedback control in circuit QED

Circuit QED is a promising solid-state quantum computing architecture. It also has excellent potential as a platform for quantum control-especially quantum feedback control-experiments. However, the current scheme for measurement in circuit QED is low efficiency and has low signal-to-noise ratio for single-shot measurements. The low quality of this measurement makes the implementation of feedback difficult, and here we propose two schemes for measurement in circuit QED architectures that can significantly improve signal-to-noise ratio and potentially achieve quantum-limited measurement. Such measurements would enable the implementation of quantum feedback protocols and we illustrate this with a simple entanglement-stabilization scheme.

Insights into hydrogen atom adsorption on and the electrochemical properties of nitrogen-substituted carbon materials

The nitrogen substitution in carbon materials is investigated theoretically using the density functional theory method. Our calculations show that nitrogen substitution decreases the hydrogen adsorption energy if hydrogen atoms are adsorbed on both nitrogen atoms and the neighboring carbon atoms. On the contrary, the hydrogen adsorption energy can be increased if hydrogen atoms are adsorbed only on the neighboring carbon atoms. The reason can be explained by the electronic structures analysis of N-substituted graphene sheets. Nitrogen substitution reduces the pi electron conjugation and increases the HOMO energy of a graphene sheet, and the nitrogen atom is not stable due to its 3-valent character. This raises an interesting research topic on the optimization of the N-substitution degree, and is important to many applications such as hydrogen storage and the tokamaks device. The electronic structure studies also explain well why nitrogen substitution increases the capacitance but decreases the electron conductivity of carbon electrodes as was experimentally observed in our experiments on the supercapacitor.

Multidimensional modelling to investigate interspecies hydrogen transfer in anaerobic biofilms

Anaerobic digestion is a multistep process, mediated by a functionally and phylogenetically diverse microbial population. One of the crucial steps is oxidation of organic acids, with electron transfer via hydrogen or formate from acetogenic bacteria to methanogens. This syntrophic microbiological process is strongly restricted by a thermodynamic limitation on the allowable hydrogen or formate concentration. In order to study this process in more detail, we developed an individual-based biofilm model which enables to describe the processes at a microbial resolution. The biochemical model is the ADM1, implemented in a multidimensional domain. With this model, we evaluated three important issues for the syntrophic relationship: (i) is there a fundamental difference in using hydrogen or formate as electron carrier? (ii) Does a thermodynamic-based inhibition function produced substantially different results from an empirical function? and; (iii) Does the physical colocation of acetogens and methanogens follow directly from a general model. Hydrogen or formate as electron carrier had no substantial impact on model results. Standard inhibition functions or thermodynamic inhibition function gave similar results at larger substrate field grid sizes (> 10 mu m), but at smaller grid sizes, the thermodynamic-based function reduced the number of cells with long interspecies distances (> 2.5 mu m). Therefore, a very fine grid resolution is needed to reflect differences between the thermodynamic function, and a more generic inhibition form. The co-location of syntrophic bacteria was well predicted without a need to assume a microbiological based mechanism (e.g., through chemotaxis) of biofilm formation.

Spin-detection in a quantum electromechanical shuttle system

We study the electrical transport of a harmonically bound, single-molecule C-60 shuttle operating in the Coulomb blockade regime, i.e. single electron shuttling. In particular, we examine the dependance of the tunnel current on an ultra-small stationary force exerted on the shuttle. As an example, we consider the force exerted on an endohedral N@C-60 by the magnetic field gradient generated by a nearby nanomagnet. We derive a Hamiltonian for the full shuttle system which includes the metallic contacts, the spatially dependent tunnel couplings to the shuttle, the electronic and motional degrees of freedom of the shuttle itself and a coupling of the shuttle's motion to a phonon bath. We analyse the resulting quantum master equation and find that, due to the exponential dependence of the tunnel probability on the shuttle-contact separation, the current is highly sensitive to very small forces. In particular, we predict that the spin state of the endohedral electrons of N@C-60 in a large magnetic gradient field can be distinguished from the resulting current signals within a few tens of nanoseconds. This effect could prove useful for the detection of the endohedral spin-state of individual paramagnetic molecules such as N@C-60 and P@C-60, or the detection of very small static forces acting on a C-60 shuttle.

New insights into the interaction of hydrogen atoms with boron-substituted carbon

Boron substitution in carbon materials has been comprehensively investigated using the density functional theory method. It was found that there is a correlation between the stability of the graphene sheet, the distribution of T electrons, the electrostatic potential, and the capability for hydrogen-atom adsorption. Boron substitution destabilizes the graphene structure, increases the density of the electron wave around the substitutional boron atoms, and lowers the electrostatic potential, thus improving the hydrogen adsorption energy on carbon. However, this improvement is only ca. 10-20% instead of a factor of 4 or 5. Our calculations also show that two substitutional boron atoms provide consistent and reliable results, but one substitutional boron results in contradictory conclusions. This is a warning to other computational chemists who work on boron substitution that the conclusion from one substitutional boron might not be reliable.

Analytical electron microscopy of proton exchange membrane fuel cells

Microtome sections of proton exchange membrane cells produce a wide range of information ranging from macroscopic distribution of components through specimens in which the detailed distribution of catalyst particles can be observed. Using modern data management practices it is possible to combine information at different scales and correlate processing and performance data. Analytical electron microscopy reveals the compositional variations across used cells at the electrolyte/electrode interface. In particular analytical techniques indicate that sulphur concentrations are likely to diminish at the interface Nafion/anode interface. © 2006 Elsevier B.V. All rights reserved.

Ultramicroporous membranes for hydrogen separation

Fuel cell systems offer excellent efficiencies when compared to internal combustion engines, which result in reduced fuel consumption and greenhouse gas emissions. One of the areas requiring research for the success of fuel cell technology is the H2 fuel purification to reduce CO, which is a poison to fuel cells. Molecular sieve silica (MSS) membranes have a potential application in this area. In this work showed activated transport, a characteristic of ultramicroporous (dp

Quantum noise in optical fibers. I. Stochastic equations

We analyze the quantum dynamics of radiation propagating in a single-mode optical fiber with dispersion, nonlinearity, and Raman coupling to thermal phonons. We start from a fundamental Hamiltonian that includes the principal known nonlinear effects and quantum-noise sources, including linear gain and loss. Both Markovian and frequency-dependent, non-Markovian reservoirs are treated. This treatment allows quantum Langevin equations, which have a classical form except for additional quantum-noise terms, to be calculated. In practical calculations, it is more useful to transform to Wigner or 1P quasi-probability operator representations. These transformations result in stochastic equations that can be analyzed by use of perturbation theory or exact numerical techniques. The results have applications to fiber-optics communications, networking, and sensor technology.

Time-reversal test for stochastic quantum dynamics

The calculation of quantum dynamics is currently a central issue in theoretical physics, with diverse applications ranging from ultracold atomic Bose-Einstein condensates to condensed matter, biology, and even astrophysics. Here we demonstrate a conceptually simple method of determining the regime of validity of stochastic simulations of unitary quantum dynamics by employing a time-reversal test. We apply this test to a simulation of the evolution of a quantum anharmonic oscillator with up to 6.022×1023 (Avogadro's number) of particles. This system is realizable as a Bose-Einstein condensate in an optical lattice, for which the time-reversal procedure could be implemented experimentally.

Gauge P-representations for quantum-dynamical problems: Removal of boundary terms

P-representation techniques, which have been very successful in quantum optics and in other fields, are also useful for general bosonic quantum-dynamical many-body calculations such as Bose-Einstein condensation. We introduce a representation called the gauge P representation, which greatly widens the range of tractable problems. Our treatment results in an infinite set of possible time evolution equations, depending on arbitrary gauge functions that can be optimized for a given quantum system. In some cases, previous methods can give erroneous results, due to the usual assumption of vanishing boundary conditions being invalid for those particular systems. Solutions are given to this boundary-term problem for all the cases where it is known to occur: two-photon absorption and the single-mode laser. We also provide some brief guidelines on how to apply the stochastic gauge method to other systems in general, quantify the freedom of choice in the resulting equations, and make a comparison to related recent developments.

Experimental study of the quantum driven pendulum and its classical analog in atom optics

We present experimental results for the dynamics of cold atoms in a far detuned amplitude-modulated optical standing wave. Phase-space resonances constitute distinct peaks in the atomic momentum distribution containing up to 65% of all atoms resulting from a mixed quantum chaotic phase space. We characterize the atomic behavior in classical and quantum regimes and we present the applicable quantum and classical theory, which we have developed and refined. We show experimental proof that the size and the position of the resonances in phase space can be controlled by varying several parameters, such as the modulation frequency, the scaled well depth, the modulation amplitude, and the scaled Planck’s constant of the system. We have found a surprising stability against amplitude noise. We present methods to accurately control the momentum of an ensemble of atoms using these phase-space resonances which could be used for efficient phase-space state preparation.

Quantum dynamics of three coupled atomic Bose-Einstein condensates

The simplest model of three coupled Bose-Einstein condensates is investigated using a group theoretical method. The stationary solutions are determined using the SU(3) group under the mean-field approximation. This semiclassical analysis, using system symmetries, shows a transition in the dynamics of the system from self trapping to delocalization at a critical value for the coupling between the condensates. The global dynamics are investigated by examination of the stable points, and our analysis shows that the structure of the stable points depends on the ratio of the condensate coupling to the particle-particle interaction, and undergoes bifurcations as this ratio is varied. This semiclassical model is compared to a full quantum treatment, which also displays a dynamical transition. The quantum case has collapse and revival sequences superimposed on the semiclassical dynamics, reflecting the underlying discreteness of the spectrum. Nonzero circular current states are also demonstrated as one of the higher-dimensional effects displayed in this system.

Radiative Relaxation Quantum Yields for Synthetic Eumelanin

We report absolute values for the radiative relaxation quantum yield of synthetic eumelanin as a function of excitation energy. These values were determined by correcting for pump beam attenuation and emission reabsorption in both eumelanin samples and fluorescein standards over a large range of concentrations. Our results confirm that eumelanins are capable of dissipating >99.9% of absorbed UV and visible radiation through nonradiative means. Furthermore, we have found that the radiative quantum yield of synthetic eumelanin is excitation energy dependent. This observation is supported by corrected emission spectra, which also show a clear dependence of both peak position and peak width on excitation energy. Our findings indicate that photoluminescence emission in eumelanins is derived from ensembles of small chemically distinct oligomeric units that can be selectively pumped. This hypothesis lends support to the theory that the basic structural unit of eumelanin is oligomeric rather than heteropolymeric.