Solvation dynamics in liquid water: III: energy fluxes and structural changes

In previous installments it has been shown how a detailed analysis of energy fluxes induced by electronic excitation of a solute can provide a quantitative understanding of the dominant molecular energy flow channels characterizing solvation—and in particular, hydration— relaxation dynamics. Here this work and power approach is complemented with a detailed characterization of the changes induced by such energy fluxes. We first examine the water solvent’s spatial and orientational distributions and the assorted energy fluxes in the various hydration shells of the solute to provide a molecular picture of the relaxation. The latter analysis is also used to address the issue of a possible “inverse snowball” effect, an ansatz concerning the time scales of the different hydration shells to reach equilibrium. We then establish a link between the instantaneous torque, exerted on the water solvent neighbors’ principal rotational axes immediately after excitation and the final energy transferred into those librational motions, which are the dominant short-time energy receptor.Postprint (author's final draft

Theory of correlations between ultra-cold bosons released from an optical lattice

In this paper we develop a theoretical description of the correlations between ultra-cold bosons after free expansion from confinement in an optical lattice. We consider the system evolution during expansion and give criteria for a far field regime. We develop expressions for first and second order two-point correlations based on a variety of commonly used approximations to the many-body state of the system including Bogoliubov, meanfield decoupling, and particle-hole perturbative solution about the perfect Mott-insulator state. Using these approaches we examine the effects of quantum depletion and pairing on the system correlations. Comparison with the directly calculated correlation functions is used to justify a Gaussian form of our theory from which we develop a general three-dimensional formalism for inhomogeneous lattice systems suitable for numerical calculations of realistic experimental regimes.Comment: 18 pages, 11 figures. To appear in Phys. Rev. A. (few minor changes made and typos fixed

Examples of Berezin-Toeplitz Quantization: Finite sets and Unit Interval

We present a quantization scheme of an arbitrary measure space based on overcomplete families of states and generalizing the Klauder and the Berezin-Toeplitz approaches. This scheme could reveal itself as an efficient tool for quantizing physical systems for which more traditional methods like geometric quantization are uneasy to implement. The procedure is illustrated by (mostly two-dimensional) elementary examples in which the measure space is a $N$-element set and the unit interval. Spaces of states for the $N$-element set and the unit interval are the 2-dimensional euclidean $\R^2$ and hermitian \C^2 planes

Closed Spaces in Cosmology

This paper deals with two aspects of relativistic cosmologies with closed (compact and boundless) spatial sections. These spacetimes are based on the theory of General Relativity, and admit a foliation into space sections S(t), which are spacelike hypersurfaces satisfying the postulate of the closure of space: each S(t) is a 3-dimensional, closed Riemannian manifold. The discussed topics are: (1) A comparison, previously obtained, between Thurston's geometries and Bianchi-Kantowski-Sachs metrics for such 3-manifolds is here clarified and developed. (2) Some implications of global inhomogeneity for locally homogeneous 3-spaces of constant curvature are analyzed from an observational viewpoint.Comment: 20 pages, 6 figures, revised version of published paper. In version 2: several misprints corrected, 'redshifting' in figures improved. Version 3: a few style corrections; couple of paragraphs in subsection 2.4 rewritten. Version 4: figures 5 and 6 corrrecte

Magnetization vector in the reversible region of a highly anisotropic cuprate superconductor: anisotropy factor and the role of 2D vortex fluctuations

By using a high quality Tl2Ba2Ca2Cu3O10 (Tl-2223) single crystal as an example, the magnetization vector was probed in the reversible region of highly anisotropic cuprate superconductors. For that, we have measured its components along and transverse to the applied magnetic field for different crystal orientations. The analysis shows that the angular dependence of the perpendicular component of the magnetization vector follows the one predicted by a London-like approach which includes a contribution associated with the thermal fluctuations of the 2D vortex positions. For the Tl-2223 crystal studied here, a lower bound for the anisotropy factor was estimated to be about 190.Comment: 6 pages, 3 figure

Towards an HH-theorem for granular gases

The $H$-theorem, originally derived at the level of Boltzmann non-linear kinetic equation for a dilute gas undergoing elastic collisions, strongly constrains the velocity distribution of the gas to evolve irreversibly towards equilibrium. As such, the theorem could not be generalized to account for dissipative systems: the conservative nature of collisions is an essential ingredient in the standard derivation. For a dissipative gas of grains, we construct here a simple functional $\mathcal H$ related to the original $H$, that can be qualified as a Lyapunov functional. It is positive, and results backed by three independent simulation approaches (a deterministic spectral method, the stochastic Direct Simulation Monte Carlo technique, and Molecular Dynamics) indicate that it is also non-increasing. Both driven and unforced cases are investigated

d-Wave Superfluidity in Optical Lattices of Ultracold Polar Molecules

Recent work on ultracold polar molecules, governed by a generalization of the t-J Hamiltonian, suggests that molecules may be better suited than atoms for studying d-wave superfluidity due to stronger interactions and larger tunability of the system. We compute the phase diagram for polar molecules in a checkerboard lattice consisting of weakly coupled square plaquettes. In the simplest experimentally realizable case where there is only tunneling and an XX-type spin-spin interaction, we identify the parameter regime where d-wave superfluidity occurs. We also find that the inclusion of a density-density interaction destroys the superfluid phase and that the inclusion of a spin-density or an Ising-type spin-spin interaction can enhance the superfluid phase. We also propose schemes for experimentally realizing the perturbative calculations exhibiting enhanced d-wave superfluidity.Comment: 22 pages, 12 figures; v2: revised discussion

Translational versus rotational energy flow in water solvation dynamics

Early molecular dynamics simulations discovered an important asymmetry in the speed of water solvation dynamics for charge extinction and charge creation for an immersed solute, a feature representing a first demonstration of the breakdown of linear response theory. The molecular level mechanism of this asymmetry is examined here via a novel energy flux theoretical approach coupled to geometric probes. The results identify the effect as arising from the translational motions of the solute-hydrating water molecules rather than their rotational/librational motions, even though the latter are more rapid and dominate the energy flow.Postprint (author's final draft