134 research outputs found
Structural Order in Glassy Water
We investigate structural order in glassy water by performing classical
molecular dynamics simulations using the extended simple point charge (SPC/E)
model of water. We perform isochoric cooling simulations across the glass
transition temperature at different cooling rates and densities. We quantify
structural order by orientational and translational order metrics. Upon cooling
the liquid into the glassy state, both the orientational order parameter
and translational order parameter increase. At T=0 K, the glasses fall
on a line in the - plane or {\it order map}.
The position of this line depends only on density and coincides with the
location in the order map of the inherent structures (IS) sampled upon cooling.
We evaluate the energy of the IS, , and find that both order
parameters for the IS are proportional to . We also study the
structural order during the transformation of low-density amorphous ice (LDA)
to high-density amorphous ice (HDA) upon isothermal compression and are able to
identify distinct regions in the order map corresponding to these glasses.
Comparison of the order parameters for LDA and HDA with those obtained upon
isochoric cooling indicates major structural differences between glasses
obtained by cooling and glasses obtained by compression. These structural
differences are only weakly reflected in the pair correlation function. We also
characterize the evolution of structural order upon isobaric annealing, leading
at high pressure to very-high density amorphous ice (VHDA).Comment: submitte
Cooling rate, heating rate and aging effects in glassy water
We report a molecular dynamics simulation study of the properties of the
potential energy landscape sampled by a system of water molecules during the
process of generating a glass by cooling, and during the process of
regenerating the equilibrium liquid by heating the glass. We study the
dependence of these processes on the cooling/heating rates as well as on the
role of aging (the time elapsed in the glass state). We compare the properties
of the potential energy landscape sampled during these processes with the
corresponding properties sampled in the liquid equilibrium state to elucidate
under which conditions glass configurations can be associated with equilibrium
liquid configurations.Comment: to be published in Phys. Rev. E (rapid comunication
RobustBench: a standardized adversarial robustness benchmark
As a research community, we are still lacking a systematic understanding of
the progress on adversarial robustness which often makes it hard to identify
the most promising ideas in training robust models. A key challenge in
benchmarking robustness is that its evaluation is often error-prone leading to
robustness overestimation. Our goal is to establish a standardized benchmark of
adversarial robustness, which as accurately as possible reflects the robustness
of the considered models within a reasonable computational budget. To this end,
we start by considering the image classification task and introduce
restrictions (possibly loosened in the future) on the allowed models. We
evaluate adversarial robustness with AutoAttack, an ensemble of white- and
black-box attacks, which was recently shown in a large-scale study to improve
almost all robustness evaluations compared to the original publications. To
prevent overadaptation of new defenses to AutoAttack, we welcome external
evaluations based on adaptive attacks, especially where AutoAttack flags a
potential overestimation of robustness. Our leaderboard, hosted at
https://robustbench.github.io/, contains evaluations of 120+ models and aims at
reflecting the current state of the art in image classification on a set of
well-defined tasks in - and -threat models and on common
corruptions, with possible extensions in the future. Additionally, we
open-source the library https://github.com/RobustBench/robustbench that
provides unified access to 80+ robust models to facilitate their downstream
applications. Finally, based on the collected models, we analyze the impact of
robustness on the performance on distribution shifts, calibration,
out-of-distribution detection, fairness, privacy leakage, smoothness, and
transferability.Comment: The camera-ready version accepted at the NeurIPS'21 Datasets and
Benchmarks Track: 120+ evaluations, 80+ models, 7 leaderboards (Linf, L2,
common corruptions; CIFAR-10, CIFAR-100, ImageNet), significantly expanded
analysis part (calibration, fairness, privacy leakage, smoothness,
transferability
Potential Energy Landscape Equation of State
Depth, number, and shape of the basins of the potential energy landscape are
the key ingredients of the inherent structure thermodynamic formalism
introduced by Stillinger and Weber [F. H. Stillinger and T. A. Weber, Phys.
Rev. A 25, 978 (1982)]. Within this formalism, an equation of state based only
on the volume dependence of these landscape properties is derived. Vibrational
and configurational contributions to pressure are sorted out in a transparent
way. Predictions are successfully compared with data from extensive molecular
dynamics simulations of a simple model for the fragile liquid orthoterphenyl.Comment: RevTeX4, 4 pages, 5 figure
Physics of the liquid-liquid critical point
Within the inherent structure (IS) thermodynamic formalism introduced by
Stillinger and Weber [F. H. Stillinger and T. A. Weber, Phys. Rev. A {\bf 25},
978 (1982)] we address the basic question of the physics of the liquid-liquid
transition and of density maxima observed in some complex liquids such as water
by identifying, for the first time, the statistical properties of the potential
energy landscape (PEL) responsible for these anomalies.
We also provide evidence of the connection between density anomalies and the
liquid-liquid critical point. Within the simple (and physically transparent)
model discussed, density anomalies do imply the existence of a liquid-liquid
transition.Comment: Physical Review Letters, in publicatio
Static and Dynamic Anomalies in a Repulsive Spherical Ramp Liquid: Theory and Simulation
We compare theoretical and simulation results for static and dynamic
properties for a model of particles interacting via a spherically symmetric
repulsive ramp potential. The model displays anomalies similar to those found
in liquid water, namely, expansion upon cooling and an increase of diffusivity
upon compression. In particular, we calculate the phase diagram from the
simulation and successfully compare it with the phase diagram obtained using
the Rogers-Young (RY) closure for the Ornstein-Zernike equation. Both the
theoretical and the numerical calculations confirm the presence of a line of
isobaric density maxima, and lines of compressibility minima and maxima.
Indirect evidence of a liquid-liquid critical point is found. Dynamic
properties also show anomalies. Along constant temperature paths, as the
density increases, the dynamics alternates several times between slowing down
and speeding up, and we associate this behavior with the progressive
structuring and de-structuring of the liquid. Finally we confirm that mode
coupling theory successfully predicts the non-monotonic behavior of dynamics
and the presence of multiple glass phases, providing strong evidence that
structure (the only input of mode coupling theory) controls dynamics.Comment: Static and Dynamic Anomalies in a Repulsive Spherical Ramp Liquid:
Theory and Simulatio
Energy landscapes, ideal glasses, and their equation of state
Using the inherent structure formalism originally proposed by Stillinger and
Weber [Phys. Rev. A 25, 978 (1982)], we generalize the thermodynamics of an
energy landscape that has an ideal glass transition and derive the consequences
for its equation of state. In doing so, we identify a separation of
configurational and vibrational contributions to the pressure that corresponds
with simulation studies performed in the inherent structure formalism. We
develop an elementary model of landscapes appropriate to simple liquids which
is based on the scaling properties of the soft-sphere potential complemented
with a mean-field attraction. The resulting equation of state provides an
accurate representation of simulation data for the Lennard-Jones fluid,
suggesting the usefulness of a landscape-based formulation of supercooled
liquid thermodynamics. Finally, we consider the implications of both the
general theory and the model with respect to the so-called Sastry density and
the ideal glass transition. Our analysis shows that a quantitative connection
can be made between properties of the landscape and a simulation-determined
Sastry density, and it emphasizes the distinction between an ideal glass
transition and a Kauzmann equal-entropy condition.Comment: 11 pages, 3 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
The dynamic crossover in water does not require bulk water
Many of the anomalous properties of water may be explained by invoking a second critical point that terminates the coexistence line between the low- and high-density amorphous states in the liquid. Direct experimental evidence of this point, and the associated polyamorphic liquid–liquid transition, is elusive as it is necessary for liquid water to be cooled below its homogeneous-nucleation temperature. To avoid crystallization, water in the eutectic LiCl solution has been studied but then it is generally considered that “bulk” water cannot be present. However, recent computational and experimental studies observe cooperative hydration in which case it is possible that sufficient hydrogen-bonded water is present for the essential characteristics of water to be preserved. For femtosecond optical Kerr-effect and nuclear magnetic resonance measurements, we observe in each case a fractional Stokes–Einstein relation with evidence of the dynamic crossover appearing near 220 K and 250 K respectively. Spectra obtained in the glass state also confirm the complex nature of the hydrogen-bonding modes reported for neat room-temperature water and support predictions of anomalous diffusion due to “worm-hole” structure
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