We calculate the maximal Lyapunov exponent for a bulk system of 256 Lennard-Jones particles in constant energy molecular dynamics simulations deep into the supercritical state. We find that the maximal Lyapunov exponent undergoes a crossover, and that this crossover coincides with the dynamical crossover at the Frenkel line from liquid physics. We explain this crossover in terms of two different contributions to dynamical instability: diffusion in the liquid-like state below the Frenkel line, and collisions in the gas-like state above. These results provide insight into the phase space dynamics far from the melting line and densities where rare-gas approximation are inapplicable.
It is well known that some liquids can demonstrate anomalous behavior. Interestingly, this be- havior can be qualitatively reproduced with simple core-softened isotropic pair-potential systems. Although anomalous properties of liquids usually take place at low and moderate temperatures it was recently recognized that many important phenomena can appear in supercritical fuids. However, no studies of supercritical behavior of core-softened fuids is reported. This paper reports a study of dynamical crossover in supercritical core-softened systems. The crossover line is calculated from three diffe…
Physical properties of an interacting system are governed by collective excitations, but their nature at extreme supercritical conditions is unknown. Here, we present direct evidence for propagating solid-like longitudinal phonon-like excitations with wavelengths extending to interatomic separations deep in the supercritical state at temperatures up to 3,300 times the critical temperature. We observe that the crossover of dispersion curves develops at $k$ points reducing with temperature. We interpret this effect as the crossover from the collective phonon to the collisional mean-free path reg…
Supercritical state has been viewed as an intermediate state between gases and liquids with largely unknown physical properties. Here, we address the important ability of supercritical fluids to sustain collective excitations. We directly study propagating modes on the basis of correlation functions calculated from extensive molecular dynamics simulations, and find that the supercritical system sustains propagating solid-like transverse modes below the Frenkel line but becomes devoid of transverse modes above the line where it supports longitudinal modes only. Important thermodynamic implicati…
Physics of supercritical state is understood to a much lesser degree compared to subcritical liquids. Carbon dioxide in particular has been intensely studied, yet little is known about the supercritical part of its phase diagram. Here, we combine neutron scattering experiments and molecular dynamics simulations and demonstrate the structural crossover at the Frenkel line. The crossover is seen at pressures as high as 14 times the critical pressure and is evidenced by changes of the main features of the structure factor and pair distribution functions.
A hallmark of a thermodynamic phase transition is the qualitative change of system thermodynamic properties such as energy and heat capacity. On the other hand, no phase transition is thought to operate in the supercritical state of matter and, for this reason, it was believed that supercritical thermodynamic properties vary smoothly and without any qualitative changes. Here, we perform extensive molecular dynamics simulations in a wide temperature range and find that a deeply supercritical state is thermodynamically heterogeneous, as witnessed by different temperature dependence of energy, he…
Dusty plasmas represent a powerful playground to study the collective dynamics of strongly coupled systems with important interdisciplinary connections to condensed matter physics. Due to the pure Yukawa repulsive interaction between dust particles, dusty plasmas do not display a traditional liquid-vapor phase transition, perfectly matching the definition of a supercritical fluid. Using molecular dynamics simulations, we verify the supercritical nature of dusty plasmas and reveal the existence of a dynamical liquid-like to gas-like crossover which perfectly matches the salient features of the …
Universal supercritical thermodynamics for black holes
School of Science, Hunan Institute of Technology（湖南工学院理学院）；Institute of Theoretical Physics, Chinese Academy of Sciences（中国科学院理论物理研究所）；Peng Huanwu Collaborative Center for Research and Education, Beihang University（北京航空航天大学彭桓武研究中心）；University of Chinese Academy of Sciences（中国科学院大学）；Wenzhou Institute, University of Chinese Academy of Sciences（中国科学院大学温州研究院）；School of Fundamental Physics and Mathematical Sciences, Hangzhou Institute for Advanced Study, UCAS（中国科学院大学杭州高等研究院基础物理与数学科学中心）
Behavior of supercritical fluids attracts a lot of attention nowadays. It is important both from the point of view of fundamental science and technological applications. However, up to now the progress in the field is rather moderate. In this article we report a computational study of supercritical carbon dioxide which is one of the most important fluids for chemical industry. We study the response functions of $CO_2$ in supercritical regime and calculate the locations of their maxima (Widom lines). We also make preliminary calculations of the line of crossover of microscopic dynamics of parti…
An electronically coarse-grained model for water reveals a persistent vestige of the liquid-gas transition deep into the supercritical region. A crossover in the density dependence of the molecular dipole arises from the onset of non-percolating hydrogen bonds. The crossover points coincide with the Widom line in the scaling region but extend further, tracking the heat capacity maxima, offering evidence for liquid- and gas-like state points in a "one-phase" fluid. The effect is present even in dipole-limit models suggesting that it is common for all molecular liquids exhibiting dipole enhancem…
Supercritical fluids play a significant role in elucidating fundamental aspects of liquid matter under extreme conditions. They have been extensively studied at pressures and temperatures relevant to various industrial applications. However, much less is known about the structural behaviour of supercritical fluids and no structural crossovers have been observed in static compression experiments in any temperature and pressure ranges beyond the critical point. The structure of supercritical state is currently perceived to be uniform everywhere on the pressure-temperature phase diagram, and to c…
Quantum many body systems with long range interactions are known to display many fascinating phenomena experimentally observable in trapped ions, Rydberg atoms and polar molecules. Among these are dynamical phase transitions which occur after an abrupt quench in spin chains with interactions decaying as $r^{-α}$ and whose critical dynamics depend crucially on the power $α$: for systems with $α<1$ the transition is sharp while for $α>1$ it fans out in a chaotic crossover region. In this paper we explore the fate of critical dynamics in Ising chains with long-range interactions when the transver…
Chaos is an important characterization of classical dynamical systems. How is chaos linked to the long-time dynamics of collective modes across phases and phase transitions? We address this by studying chaos across Ising and Kosterlitz-Thouless transitions in classical XXZ model. We show that spatio-temporal chaotic properties have crossovers across the transitions and distinct temperature dependence in the high and low-temperature phases which show normal and anomalous diffusions, respectively. Our results also provide new insights into the dynamics of interacting quantum systems in the semic…
Chaotic quantum systems with Lyapunov exponent $λ_\mathrm{L}$ obey an upper bound $λ_\mathrm{L}\leq 2πk_\mathrm{B}T/\hbar$ at temperature $T$, implying a divergence of the bound in the classical limit $\hbar\to 0$. Following this trend, does a quantum system necessarily become `more chaotic' when quantum fluctuations are reduced? Moreover, how do symmetry breaking and associated non-trivial dynamics influence the interplay of quantum mechanics and chaos? We explore these questions by computing $λ_\mathrm{L}(\hbar,T)$ in the quantum spherical $p$-spin glass model, where $\hbar$ can be continuou…
In this work, we report on inelastic X-ray scattering experiments combined with the molecular dynamics simulations on deeply supercritical Ar. The presented results unveil the mechanism and regimes of sound propagation in the liquid matter and provide compelling evidence for the adiabatic-to-isothermal longitudinal sound propagation transition. We introduce a Hamiltonian predicting low-frequency transverse sound propagation gaps, which is confirmed by experimental findings and molecular dynamics calculations. As a result, a universal link is established between the positive sound dispersion (P…
Our first very wide survey of the supercritical phase diagram and its key properties reveals a universal interrelation between dynamics and thermodynamics and an unambiguous transition between liquidlike and gaslike states. This is seen in the master plot showing a collapse of the data representing the dependence of specific heat on key dynamical parameters in the system for many different paths on the phase diagram. As a result, the observed transition is path-independent. We call it a "c"-transition due to the "c"-shaped curve parameterizing the dependence of the specific heat on key dynamic…
We investigate the operator growth dynamics of the transverse field Ising spin chain in one dimension as varying the strength of the longitudinal field. An operator in the Heisenberg picture spreads in the extended Hilbert space. Recently, it has been proposed that the spreading dynamics has a universal feature signaling chaoticity of underlying quantum dynamics. We demonstrate numerically that the operator growth dynamics in the presence of the longitudinal field follows the universal scaling law for one-dimensional chaotic systems. We also find that the operator growth dynamics satisfies a c…
