The release of two compositionally different solutes from a composite gel composed of two different populations of microgel particles embedded in a single bulk gel matrix is described, showing the potential of the "plum-pudding gel" as a multifunctional platform for controlled surface release. One hydrophobic solute (pyrene) and one hydrophobic and charged solute (rhodamine 123) were chosen as the solutes to be released. Hydrophobic microgels composed of 50% N-isopropylacrylamide (NIPAM) and 50% N-tert-butylacrylamide (BAM) were loaded with pyrene, and anionic microgels composed of 30% acrylic acid (AAc), 20% NIPAM, and 50% BAM were loaded with rhodamine 123. The two solute-loaded microgel populations were incorporated into a single bulk gel network, from which the two solutes were released simultaneously and independently. Using this structural motif, solutes that are mutually incompatible can be incorporated into a single matrix with which they may also be incompatible. The electrostatically incorporated solute was released much more slowly than the hydrophobically attracted solute, indicating that the microgel composition can be tailored to the specific solute, and thus control its release rate. The choice of bulk matrix was also found to influence the release rate much more than expected, offering a further control element to the system.

We analyze heat and work fluctuations in the gravitational wave detector AURIGA, modeled as a macroscopic electromechanical oscillator in contact with a thermostat and cooled by an active feedback system. The oscillator is driven to a steady state by the feedback cooling, equivalent to a viscous force. The experimentally measured fluctuations are in agreement with our theoretical analysis based on a stochastically driven Langevin system. The asymmetry of the fluctuations of the absorbed heat characterizes the oscillator's nonequilibrium steady state and reveals the extent to which a feedback cooled system departs from equilibrium in a statistical mechanics perspective.

We introduce an order parameter for dynamical arrest. Dynamically available volume (unoccupied space that is available to the motion of particles) is expressed as holes for the simple lattice models we study. Near the arrest transition the system is dilute in holes, so we expand dynamical quantities in a series of hole density. Unlike the situation when presented in particle density, all cases of simple models that we examine have a quadratic dependence of the diffusion constant on hole density. This observation implies that in certain regimes ideal dynamical arrest transitions may possess a hitherto unnoticed degree of universality.

We study the onset of the bootstrap percolation transition as a model of generalized dynamical arrest. Our results apply to two dimensions, but there is no significant barrier to extending them to higher dimensionality. We develop a new importance-sampling procedure in simulation, based on rare events around "holes", that enables us to access bootstrap lengths beyond those previously studied. By framing a new theory in terms of paths or processes that lead to emptying of the lattice we are able to develop systematic corrections to the existing theory and compare them to simulations. Thereby, for the first time in the literature, it is possible to obtain credible comparisons between theory and simulation in the accessible density range.

Jamming, or dynamical arrest, is a transition at which many particles stop moving in a collective manner. In nature it is brought about by, for example, increasing the packing density, changing the interactions between particles, or otherwise restricting the local motion of the elements of the system. The onset of collectivity occurs because, when one particle is blocked, it may lead to the blocking of a neighbor. That particle may then block one of its neighbors, these effects propagating across some typical domain of size named the dynamical correlation length. When this length diverges, the system becomes immobile. Even where it is finite but large the dynamics is dramatically slowed. Such phenomena lead to glasses, gels, and other very long-lived nonequilibrium solids. The bootstrap percolation models are the simplest examples describing these spatio-temporal correlations. We have been able to solve one such model in two dimensions exactly, exhibiting the precise evolution of the jamming correlations on approach to arrest. We believe that the nature of these correlations and the method we devise to solve the problem are quite general. Both should be of considerable help in further developing this field.T here exists within nature a whole class of systems that exhibit a geometrical percolation transition at which they become spanned by a single infinite cluster extending across the whole system (1-3). Such transitions may be observed, for example, by randomly occupying lattice sites at some prescribed density. Spatio-temporal particle correlations implied by simple dynamical models may also be studied by using percolation ideas. Indeed, since its introduction (4, 5), the potential of the bootstrap percolation problem (6, 7) to analyze the dynamics of a system of highly coupled and locally interacting units has been recognized. The range of applications has continued to grow (8)(9)(10)(11)(12).This problem is of particular interest because of a growing focus on, and appreciation of, the unifying role of dynamical arrest (13-17) or jamming (18) in the formation of complex condensed states of matter. Despite many advances, there is as yet no complete and fundamental conceptual framework to describe the phenomena. In comparable situations it has been an important lesson of critical phenomena (19,20) that an exact solution, even of a 2D model system, can be of great assistance in broader efforts to understand the issues. Thus, an exact closed solution of one bootstrap problem (with all of the implications of strong packing-induced coupling and divergent correlated domains) would represent, even without direct access to transport coefficients, a solution of a nontrivial (and non-mean field) jamming or arrest scenario. We will present such a solution in this article.That such a treatment is possible must be considered surprising, for there have been no prior indications of such simplification, to our knowledge.The connection of the bootstrap percolation problem to jamming phenomena is clear. Thus, particles, process...

We write equations of motion for density variables that are equivalent to Newtons equations. We then propose a set of trial equations parameterised by two unknown functions to describe the exact equations. These are chosen to best fit the exact Newtonian equations. Following established ideas, we choose to separate these trial functions into a set representing integrable motions of density waves, and a set containing all effects of non-integrability. The density waves are found to have the dispersion of sound waves, and this ensures that the interactions between the independent waves are minimised. Furthermore, it transpires that the static structure factor is fixed by this minimum condition to be the solution of the Yvon-Born-Green (YBG) equation. The residual interactions between density waves are explicitly isolated in their Newtonian representation and expanded by choosing the dominant objects in the phase space of the system, that can be represented by a dissipative term with memory and a random noise. This provides a mapping between deterministic and stochastic dynamics. Imposing the Fluctuation-Dissipation Theorem (FDT) allows us to calculate the memory kernel. We write exactly the expression for it, following two different routes, i.e. using explicitly Newtons equations, or instead, their implicit form, that must be projected onto density pairs, as in the development of the well-established Mode Coupling Theory (MCT). We compare these two ways of proceeding, showing the necessity to enforce a new equation of constraint for the two schemes to be consistent. Thus, while in the first 'Newtonian' representation a simple gaussian approximation for the random process leads easily to the Mean Spherical Approximation (MSA) for the statics and to MCT for the dynamics of the system, in the second case higher levels of approximation are required to have a fully consistent theory.

When the energy content of a resonant mode of a crystalline solid in thermodynamic equilibrium is directly measured, assuming that quantum effects can be neglected it coincides with temperature except for a proportionality factor. This is due to the principle of energy equipartition and the equilibrium hypothesis. However, most natural systems found in nature are not in thermodynamic equilibrium and thus the principle cannot be granted. We measured the extent to which the low-frequency modes of vibration of a solid can defy energy equipartition, in presence of a steady state heat flux, even close to equilibrium. We found, experimentally and numerically, that the energy separately associated with low frequency normal modes strongly depends on the heat flux, and decouples sensibly from temperature. A 4% in the relative temperature difference across the object around room temperature suffices to excite two modes of a macroscopic oscillator, as if they were at equilibrium, respectively, at temperatures about 20% and a factor 3.5 higher. We interpret the result in terms of new fluxmediated correlations between modes in the nonequilibrium state, which are absent at equilibrium.

We study several examples of kinetically constrained lattice models using dynamically accessible volume as an order parameter. Thereby we identify two distinct regimes exhibiting dynamical slowing, with a sharp threshold between them. These regimes are identified both by a new response function in dynamically available volume, as well as directly in the dynamics. Results for the selfdiffusion constant in terms of the connected hole density are presented, and some evidence is given for scaling in the limit of dynamical arrest. * Electronic address: aonghus@fiachra.ucd.ie