592 research outputs found
Generic mechanism for generating a liquid-liquid phase transition
Recent experimental results indicate that phosphorus, a single-component
system, can have two liquid phases: a high-density liquid (HDL) and a
low-density liquid (LDL) phase. A first-order transition between two liquids of
different densities is consistent with experimental data for a variety of
materials, including single-component systems such as water, silica and carbon.
Molecular dynamics simulations of very specific models for supercooled water,
liquid carbon and supercooled silica, predict a LDL-HDL critical point, but a
coherent and general interpretation of the LDL-HDL transition is lacking. Here
we show that the presence of a LDL and a HDL can be directly related to an
interaction potential with an attractive part and two characteristic
short-range repulsive distances. This kind of interaction is common to other
single-component materials in the liquid state (in particular liquid metals),
and such potentials are often used to decribe systems that exhibit a density
anomaly. However, our results show that the LDL and HDL phases can occur in
systems with no density anomaly. Our results therefore present an experimental
challenge to uncover a liquid-liquid transition in systems like liquid metals,
regardless of the presence of the density anomaly.Comment: 5 pages, 3 ps Fig
Emergent excitations in a geometrically frustrated magnet
Frustrated systems are ubiquitous and interesting because their behavior is
difficult to predict. Magnetism offers extreme examples in the form of spin
lattices where all interactions between spins cannot be simultaneously
satisfied. Such geometrical frustration leads to macroscopic degeneracies, and
offers the possibility of qualitatively new states of matter whose nature has
yet to be fully understood. Here we have discovered how novel composite spin
degrees of freedom can emerge from frustrated interactions in the cubic spinel
ZnCr2O4. Upon cooling, groups of six spins self-organize into weakly
interacting antiferromagnetic loops whose directors, defined as the unique
direction along which the spins are aligned parallel or antiparallel, govern
all low temperature dynamics. The experimental evidence comes from a
measurement of the magnetic form factor by inelastic neutron scattering. While
the data bears no resemblance to the atomic form factor for chromium, they are
perfectly consistent with the form factor for hexagonal spin loop directors.
The hexagon directors are to a first approximation decoupled from each other
and hence their reorientations embody the long-sought local zero energy modes
for the pyrochlore lattice.Comment: 10 pages, 4 figures upon reques
Liquid Polymorphism and Double Criticality in a Lattice Gas Model
We analyze the possible phase diagrams of a simple model for an associating
liquid proposed previously. Our two-dimensional lattice model combines
oreintati onal ice-like interactions and \"{}Van der Waals\"{} interactions
which may be repulsive, and in this case represent a penalty for distortion of
hydrogen bonds in the presence of extra molecules. These interactions can be
interpreted in terms of two competing distances, but not necessarily soft-core.
We present mean -field calculations and an exhaustive simulation study for
different parameters which represent relative strength of the bonding
interaction to the energy penalty for its distortion. As this ratio decreases,
a smooth disappearance of the doubl e criticality occurs. Possible connections
to liquid-liquid transitions of molecul ar liquids are suggested
Non-monotonic temperature evolution of dynamic correlations in glass-forming liquids
The viscosity of glass-forming liquids increases by many orders of magnitude
if their temperature is lowered by a mere factor of 2-3 [1,2]. Recent studies
suggest that this widespread phenomenon is accompanied by spatially
heterogeneous dynamics [3,4], and a growing dynamic correlation length
quantifying the extent of correlated particle motion [5-7]. Here we use a novel
numerical method to detect and quantify spatial correlations which reveal a
surprising non-monotonic temperature evolution of spatial dynamical
correlations, accompanied by a second length scale that grows monotonically and
has a very different nature. Our results directly unveil a dramatic qualitative
change in atomic motions near the mode-coupling crossover temperature [8] which
involves no fitting or indirect theoretical interpretation. Our results impose
severe new constraints on the theoretical description of the glass transition,
and open several research perspectives, in particular for experiments, to
confirm and quantify our observations in real materials.Comment: 7 page
Irreversible reorganization in a supercooled liquid originates from localised soft modes
The transition of a fluid to a rigid glass upon cooling is a common route of
transformation from liquid to solid that embodies the most poorly understood
features of both phases1,2,3. From the liquid perspective, the puzzle is to
understand stress relaxation in the disordered state. From the perspective of
solids, the challenge is to extend our description of structure and its
mechanical consequences to materials without long range order. Using computer
simulations, we show that the localized low frequency normal modes of a
configuration in a supercooled liquid are causally correlated to the
irreversible structural reorganization of the particles within that
configuration. We also demonstrate that the spatial distribution of these soft
local modes can persist in spite of significant particle reorganization. The
consequence of these two results is that it is now feasible to construct a
theory of relaxation length scales in glass-forming liquids without recourse to
dynamics and to explicitly relate molecular properties to their collective
relaxation.Comment: Published online: 20 July 2008 | doi:10.1038/nphys1025 Available from
http://www.nature.com/nphys/journal/v4/n9/abs/nphys1025.htm
Liquid-liquid critical point in supercooled silicon
A novel liquid-liquid phase transition has been proposed and investigated in
a wide variety of pure substances recently, including water, silica and
silicon. From computer simulations using the Stillinger-Weber classical
empirical potential, Sastry and Angell [1] demonstrated a first order
liquid-liquid transition in supercooled silicon, subsequently supported by
experimental and simulation studies. Here, we report evidence for a
liquid-liquid critical end point at negative pressures, from computer
simulations using the SW potential. Compressibilities exhibit a growing maximum
upon lowering temperature below 1500 K and isotherms exhibit density
discontinuities below 1120 K, at negative pressure. Below 1120 K, isotherms
obtained from constant volume-temperature simulations exhibit non-monotonic,
van der Waals-like behavior signaling a first order transition. We identify Tc
~ 1120 +/- 12 K, Pc -0.60 +/- 0.15 GPa as the critical temperature and pressure
for the liquid-liquid critical point. The structure of the liquid changes
dramatically upon decreasing the temperature and pressure. Diffusivities vary
over 4 orders of magnitude, and exhibit anomalous pressure dependence near the
critical point. A strong relationship between local geometry quantified by the
coordination number, and diffusivity, is seen, suggesting that atomic mobility
in both low and high density liquids can usefully be analyzed in terms of
defects in the tetrahedral network structure. We have constructed the phase
diagram of supercooled silicon. We identify the lines of compressibility,
density extrema (maxima and minima) and the spinodal which reveal the
interconnection between thermodynamic anomalies and the phase behaviour of the
system as suggested in previous works [2-9]Comment: (to be published in revised form); small corrections to previous
version; Nature Physics 201
A thermodynamic unification of jamming
Fragile materials ranging from sand to fire-retardant to toothpaste are able
to exhibit both solid and fluid-like properties across the jamming transition.
Unlike ordinary fusion, systems of grains, foams and colloids jam and cease to
flow under conditions that still remain unknown. Here we quantify jamming via a
thermodynamic approach by accounting for the structural ageing and the
shear-induced compressibility of dry sand. Specifically, the jamming threshold
is defined using a non-thermal temperature that measures the 'fluffiness' of a
granular mixture. The thermodynamic model, casted in terms of pressure,
temperature and free-volume, also successfully predicts the entropic data of
five molecular glasses. Notably, the predicted configurational entropy avoids
the Kauzmann paradox entirely. Without any free parameters, the proposed
equation-of-state also governs the mechanism of shear-banding and the
associated features of shear-softening and thickness-invariance.Comment: 16 pgs double spaced. 4 figure
Configurational Entropy and Diffusivity of Supercooled Water
We calculate the configurational entropy S_conf for the SPC/E model of water
for state points covering a large region of the (T,rho) plane. We find that (i)
the (T,rho) dependence of S_conf correlates with the diffusion constant and
(ii) that the line of maxima in S_conf tracks the line of density maxima. Our
simulation data indicate that the dynamics are strongly influenced by S_conf
even above the mode-coupling temperature T_MCT(rho).Comment: Significant update of reference
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