The European Physical Journal E,
Год журнала:
2023,
Номер
46(6)
Опубликована: Июнь 1, 2023
We
investigate
a
metallic
glass-forming
(GF)
material
(Al90Sm10)
exhibiting
fragile-strong
(FS)
glass-formation
by
molecular
dynamics
simulation
to
better
understand
this
highly
distinctive
pattern
of
in
which
many
the
usual
phenomenological
relations
describing
relaxation
times
and
diffusion
ordinary
GF
liquids
no
longer
apply,
where
instead
genuine
thermodynamic
features
are
observed
response
functions
little
signature
is
exhibited
at
glass
transition
temperature,
Tg.
Given
unexpected
similarities
between
thermodynamics
with
water,
we
first
focus
on
anomalous
static
scattering
liquid,
following
recent
studies
silicon
other
FS
liquids.
quantify
"hyperuniformity
index"
H
our
provides
quantitative
measure
"jamming".
To
gain
insight
into
T-dependence
magnitude
H,
also
estimate
another
more
familiar
particle
localization,
Debye-Waller
parameter
〈u2〉
mean-square
displacement
timescale
order
fast
time,
calculate
for
heated
crystalline
Cu.
This
comparative
analysis
materials
allows
us
critical
value
10-3
as
being
analogous
Lindemann
criterion
both
melting
crystals
"softening"
glasses.
further
interpret
emergence
liquid-liquid
phase
separation
class
arise
from
cooperative
self-assembly
process
liquid.
The Journal of Physical Chemistry B,
Год журнала:
2022,
Номер
127(1), С. 378 - 386
Опубликована: Дек. 20, 2022
Multiple
numerical
studies
have
unambiguously
shown
the
existence
of
a
liquid-liquid
critical
point
in
supercooled
states
for
different
models
water,
and
various
structural
indicators
been
put
forward
to
describe
transformation
associated
with
this
phase
transition.
Here
we
analyze
simulations
near-critical
water
compare
behavior
several
such
density
fluctuations.
We
show
that
close
most
are
strongly
correlated
density,
some
them
even
display
identical
distributions
These
probe
exact
same
free
energy
landscape,
therefore
providing
thermodynamic
description
which
is
provided
by
order
parameter.
This
implies
point,
there
tight
coupling
between
many,
only
apparently
distinct,
degrees
freedom.
The Journal of Physical Chemistry B,
Год журнала:
2023,
Номер
127(15), С. 3452 - 3462
Опубликована: Апрель 12, 2023
Water
has
anomalous
thermodynamic
and
kinetic
properties
distinct
from
ordinary
liquids.
The
famous
examples
are
the
density
maximum
at
4
°C
viscosity
decrease
upon
pressurization.
presence
of
second
critical
point
been
considered
to
be
responsible
for
these
anomalies
since
its
discovery
in
ST2
water.
Recently,
existence
confirmed
firmly
TIP4P/2005,
which
is
one
most
successful
classical
models
water,
by
Debenedetti
et
al.
[Debenedetti
Science
2020,
369,
289].
Here,
we
study
water
structure
dynamic
quantities
a
wide
temperature
(T)-pressure
(P)
range,
including
vicinity
point,
extensive
molecular
dynamics
simulation
this
model.
We
reveal
that
hierarchical
two-state
model
with
cooperative
formation
tetrahedral
structures
via
hydrogen
bonding
can
describe
T,
P-dependences
structure,
anomalies,
criticality
TIP4P/2005
unified
manner.
shows
very
similar
behaviors
real
all
aspects,
suggesting
possible
Our
physical
description
based
on
two
order
parameters,
fraction
locally
favored
structures,
indicates
latter
relevant
parameter
supported
analysis
fluctuations.
different
nature
arrangements,
conserved
nonconserved,
may
key
unambiguously
identifying
parameter.
Physical Review Letters,
Год журнала:
2024,
Номер
133(7)
Опубликована: Авг. 13, 2024
The
links
of
a
physical
network
cannot
cross,
which
often
forces
the
layout
into
nonoptimal
entangled
states.
Here
we
define
fabric
as
two-dimensional
projection
and
propose
average
crossing
number
measure
entanglement.
We
analytically
derive
dependence
on
density,
link
length,
degree
heterogeneity,
community
structure
show
that
predictions
accurately
estimate
entanglement
both
models
real
networks.
Proceedings of the National Academy of Sciences,
Год журнала:
2024,
Номер
121(36)
Опубликована: Авг. 29, 2024
The
representation
of
complex
systems
as
networks
has
become
a
critical
tool
across
many
fields
science.
In
the
context
physical
networks,
such
biological
neural
vascular
or
network
liquids
where
nodes
and
edges
occupy
volume
in
three-dimensional
space,
question
how
they
densely
packed
is
special
importance.
Here,
we
investigate
model
liquid,
which
known
to
densify
via
two
successive
liquid–liquid
phase
transitions
(LLPTs).
We
elucidate
importance
rings—cyclic
paths
formed
by
bonded
particles
networks—and
their
spatial
disposition
understanding
structural
changes
that
underpin
increase
density
LLPTs.
Our
analyses
demonstrate
densification
these
primarily
driven
formation
linked
rings,
LLPTs
correspond
hierarchy
topological
rings
form
fundamental
building
blocks.
envisage
entanglement
emerge
general
mechanism
for
densification,
with
wide
implications
embedding
especially
confined
spaces.
The Journal of Chemical Physics,
Год журнала:
2024,
Номер
160(9)
Опубликована: Март 4, 2024
Studies
of
water
thermodynamics
have
long
been
tied
to
the
identification
two
distinct
families
local
structures,
whose
competition
could
explain
origin
many
thermodynamic
anomalies
and
hypothesized
liquid–liquid
critical
point
in
water.
Despite
successes
insights
gained,
structural
indicators
proposed
throughout
years
were
not
able
unequivocally
identify
these
over
a
wide
range
conditions.
We
show
that
recently
introduced
indicator,
Ψ,
which
exploits
information
on
hydrogen
bond
network
connectivity,
can
reliably
environments
conditions
(188–300
K
0–13
kbar)
close
point,
spatial
correlations
density
fluctuations
are
identical
those
Ψ
indicator.
Our
results
strongly
support
idea
properties
arise
from
between
identifiable
environments.
Phase
transitions
are
typically
quantified
using
order
parameters,
such
as
crystal
lattice
distances
and
radial
distribution
functions,
which
can
identify
subtle
changes
in
crystalline
materials
or
high-contrast
phases
with
large
structural
differences.
However,
the
identification
of
high
complexity,
multiscale
organization
complex
patterns
during
fluctuations
preceding
phase
transitions,
essential
for
understanding
system
pathways
between
phases,
is
challenging
those
traditional
analyses.
Here,
it
shown
that
two
model
systems-
thermotropic
liquid
crystals
a
lyotropic
water/surfactant
mixtures-graph
theoretical
(GT)
descriptors
successfully
combining
molecular
nanoscale
levels
hard
to
characterize
methodologies.
Furthermore,
GT
also
reveal
different
phases.
Specifically,
centrality
parameters
node-based
fractal
dimension
quantify
behavior
capturing
fluctuation-induced
breakup
aggregates
their
long-range
cooperative
interactions.
parameterization
be
generalized
wide
range
chemical
systems
instrumental
growth
mechanisms
nanostructures.
Proceedings of the National Academy of Sciences,
Год журнала:
2024,
Номер
121(41)
Опубликована: Окт. 2, 2024
The
ability
of
vitrification
when
crossing
the
glass
transition
temperature
(T
g
)
confined
and
bulk
water
is
crucial
for
myriad
phenomena
in
diverse
fields,
ranging
from
cryopreservation
organs
food
to
development
cryoenzymatic
reactions,
frost
damage
buildings,
atmospheric
water.
However,
determining
water’s
T
remains
a
major
challenge.
Here,
we
elucidate
by
analyzing
calorimetric
behavior
nano-confined
across
various
pore
topologies
(diameters:
0.3
2.5
nm).
Our
approach
involves
subjecting
annealing
protocols
identify
time
evolution
nonequilibrium
kinetics.
Furthermore,
complement
this
with
dynamics
water,
as
seen
broadband
dielectric
spectroscopy
linear
measurements,
including
fast
scanning
technique.
This
study
demonstrated
that
undergoes
range
170
200
K,
depending
on
confinement
size
interaction
walls.
Moreover,
also
show
thermal
event
observed
at
~136
K
must
be
interpreted
an
prepeak,
referred
“shadow
transition.”
Calorimetric
measurements
allow
detection
specific
heat
step
above
which
insensitive
and,
thereby,
true
thermodynamic
transition.
Finally,
connecting
our
results
behavior,
offer
comprehensive
understanding
potential
implications
numerous
applications.
Nucleic Acids Research,
Год журнала:
2024,
Номер
unknown
Опубликована: Ноя. 21, 2024
All
life
forms
are
miraculous,
but
some
more
inexplicable
than
others.
Trypanosomes
by
far
one
of
the
most
puzzling
organisms
on
Earth:
their
mitochondrial
genome,
also
called
kinetoplast
DNA
(kDNA)
an
Olympic-ring-like
network
interlinked
circles,
challenging
conventional
paradigms
in
both
biology
and
physics.
In
this
review,
I
will
discuss
kDNA
from
astonished
perspective
a
polymer
physicist
tell
story
how
single
sub-cellular
structure
blood-dwelling
parasite
is
inspiring
generations
chemists
physicists
to
create
new
catenated
materials.
The Journal of Chemical Physics,
Год журнала:
2025,
Номер
162(1)
Опубликована: Янв. 7, 2025
Rigid,
non-polarizable
water
models
are
very
efficient
from
a
computational
point
of
view,
and
some
them
have
great
ability
in
predicting
experimental
properties.
There
is,
however,
little
room
for
improvement
simulating
with
this
strategy,
whose
main
shortcoming
is
that
molecules
do
not
change
their
interaction
parameters
response
to
the
local
molecular
landscape.
In
work,
we
propose
novel
modeling
strategy
involves
using
two
rigid
as
states
can
adopt
depending
on
environment.
During
simulation,
dynamically
transition
one
state
another
order
parameter
quantifies
structural
feature.
particular,
belonging
low-
high-tetrahedral
environments
represented
TIP4P/2005
TIP4P/Ice
models,
respectively.
way,
between
strengthened
when
they
acquire
tetrahedral
coordination,
which
be
viewed
an
effective
way
introducing
polarization
effects.
We
call
resulting
model
TIP4P2005Ice
show
it
outperforms
either
build
it.
This
multi-state
only
slows
down
simulations
by
factor
1.5
compared
standard
holds
promise
improving
aqueous
solutions.