Exothermic Supercooled Liquid—Liquid Transition in Amorphous Sulfur

2014 ◽  
Vol 31 (6) ◽  
pp. 066401
Author(s):  
Dou-Dou Zhang ◽  
Xiu-Ru Liu ◽  
Shi-Ming Hong ◽  
Liang-Bin Li ◽  
Kun-Peng Cui ◽  
...  
Keyword(s):  
Supercooled Liquid ◽  
Liquid Transition ◽  
Amorphous Sulfur

scholarly journals Polyamorphism Mirrors Polymorphism in the Liquid–Liquid Transition of a Molecular Liquid

2020 ◽  
Author(s):  
Finlay Walton ◽  
John Bolling ◽  
Andrew Farrell ◽  
Jamie MacEwen ◽  
Christopher Syme ◽  
...  
Keyword(s):  
Order Parameter ◽  
Supercooled Liquid ◽  
Supercooled Liquids ◽  
Molecular Packing ◽  
Single Component ◽  
Triphenyl Phosphite ◽  
Amorphous Phases ◽  
Geometrically Frustrated ◽  
Intimate Connection ◽  
Liquid Transition

Liquid-liquid transitions between two amorphous phases in a single-component liquid (polyamorphism) have defied explanation and courted controversy. All known examples of liquid–liquid transitions have been observed in the supercooled liquid suggesting an intimate connection with vitrification and locally favored structures inhibiting crystallization. However, there is precious little information about the local molecular packing in supercooled liquids meaning that the order parameter of the transition is still unknown. Here, we investigate the liquid–liquid transition in triphenyl phosphite and show that it is caused by the competition between liquid structures that mirror two crystal polymorphs. The liquid–liquid transition is found to be between a geometrically frustrated liquid to a dynamically frustrated glass. These results indicate a general link between polymorphism and polyamorphism and will lead to a much greater understanding of the physical basis of liquid–liquid transitions and allow the discovery of other examples.

scholarly journals Some Aspects of the Liquid Water Thermodynamic Behavior: From The Stable to the Deep Supercooled Regime

2020 ◽  
Vol 21 (19) ◽  
pp. 7269
Author(s):  
Francesco Mallamace ◽  
Giuseppe Mensitieri ◽  
Domenico Mallamace ◽  
Martina Salzano de Luna ◽  
Sow-Hsin Chen
Keyword(s):  
Liquid Water ◽  
Supercooled Liquid ◽  
Bulk Water ◽  
Bulk Liquid ◽  
Amorphous Phases ◽  
Glass Forming ◽  
Liquid Phases ◽  
Liquid Transition ◽  
Glass Forming Materials ◽  
Thermodynamic Anomalies

Liquid water is considered to be a peculiar example of glass forming materials because of the possibility of giving rise to amorphous phases with different densities and of the thermodynamic anomalies that characterize its supercooled liquid phase. In the present work, literature data on the density of bulk liquid water are analyzed in a wide temperature-pressure range, also including the glass phases. A careful data analysis, which was performed on different density isobars, made in terms of thermodynamic response functions, like the thermal expansion αP and the specific heat differences CP−CV, proves, exclusively from the experimental data, the thermodynamic consistence of the liquid-liquid transition hypothesis. The study confirms that supercooled bulk water is a mixture of two liquid “phases”, namely the high density (HDL) and the low density (LDL) liquids that characterize different regions of the water phase diagram. Furthermore, the CP−CV isobars behaviors clearly support the existence of both a liquid–liquid transition and of a liquid–liquid critical point.

Evidence of a melt like supercooled liquid during a solid to liquid transition of titanium nanowire

2004 ◽  
Vol 399 (1-3) ◽  
pp. 20-25 ◽  
Author(s):  
Li Hui ◽  
B.L. Wang ◽  
J.L. Wang ◽  
G.H. Wang
Keyword(s):  
Supercooled Liquid ◽  
Liquid Transition

scholarly journals Polyamorphism Mirrors Polymorphism in the Liquid–Liquid Transition of a Molecular Liquid

2019 ◽  
Author(s):  
Finlay Walton ◽  
John Bolling ◽  
Andrew Farrell ◽  
Jamie MacEwen ◽  
Christopher Syme ◽  
...  
Keyword(s):  
Order Parameter ◽  
Supercooled Liquid ◽  
Supercooled Liquids ◽  
Molecular Packing ◽  
Single Component ◽  
Triphenyl Phosphite ◽  
Amorphous Phases ◽  
Geometrically Frustrated ◽  
Intimate Connection ◽  
Liquid Transition

Liquid-liquid transitions between two amorphous phases in a single-component liquid (polyamorphism) have defied explanation and courted controversy. All known examples of liquid–liquid transitions have been observed in the supercooled liquid suggesting an intimate connection with vitrification and locally favored structures inhibiting crystallization. However, there is precious little information about the local molecular packing in supercooled liquids meaning that the order parameter of the transition is still unknown. Here, we investigate the liquid–liquid transition in triphenyl phosphite and show that it is caused by the competition between liquid structures that mirror two crystal polymorphs. The liquid–liquid transition is found to be between a geometrically frustrated liquid to a dynamically frustrated glass. These results indicate a general link between polymorphism and polyamorphism and will lead to a much greater understanding of the physical basis of liquid–liquid transitions and allow the discovery of other examples.

scholarly journals Experimental observation of the liquid-liquid transition in bulk supercooled water under pressure

Science ◽  
2020 ◽  
Vol 370 (6519) ◽  
pp. 978-982 ◽  
Author(s):  
Kyung Hwan Kim ◽  
Katrin Amann-Winkel ◽  
Nicolas Giovambattista ◽  
Alexander Späh ◽  
Fivos Perakis ◽  
...  
Keyword(s):  
Time Scales ◽  
Supercooled Water ◽  
Supercooled Liquid ◽  
Laser Pulses ◽  
High Density ◽  
Liquid Transition ◽  
Probe Delay ◽  
Sample Density ◽  
Order Of Magnitude ◽  
Isochoric Heating

We prepared bulk samples of supercooled liquid water under pressure by isochoric heating of high-density amorphous ice to temperatures of 205 ± 10 kelvin, using an infrared femtosecond laser. Because the sample density is preserved during the ultrafast heating, we could estimate an initial internal pressure of 2.5 to 3.5 kilobar in the high-density liquid phase. After heating, the sample expanded rapidly, and we captured the resulting decompression process with femtosecond x-ray laser pulses at different pump-probe delay times. A discontinuous structural change occurred in which low-density liquid domains appeared and grew on time scales between 20 nanoseconds to 3 microseconds, whereas crystallization occurs on time scales of 3 to 50 microseconds. The dynamics of the two processes being separated by more than one order of magnitude provides support for a liquid-liquid transition in bulk supercooled water.

scholarly journals Chain Breakage in the Supercooled Liquid - Liquid Transition and Re-entry of the λ-transition in Sulfur

2018 ◽  
Vol 8 (1) ◽  
Author(s):  
Linji Zhang ◽  
Yang Ren ◽  
Xiuru Liu ◽  
Fei Han ◽  
Kenneth Evans-Lutterodt ◽  
...  
Keyword(s):  
Supercooled Liquid ◽  
Liquid Transition

scholarly journals Signatures of a liquid–liquid transition in an ab initio deep neural network model for water

2020 ◽  
Vol 117 (42) ◽  
pp. 26040-26046
Author(s):  
Thomas E. Gartner ◽  
Linfeng Zhang ◽  
Pablo M. Piaggi ◽  
Roberto Car ◽  
Athanassios Z. Panagiotopoulos ◽  
...  
Keyword(s):  
Neural Network ◽  
Ab Initio ◽  
Density Functional ◽  
Deep Neural Network ◽  
Supercooled Liquid ◽  
State Equation ◽  
Experimental Proof ◽  
Functional Theory ◽  
Liquid Transition ◽  
Advanced Sampling

The possible existence of a metastable liquid–liquid transition (LLT) and a corresponding liquid–liquid critical point (LLCP) in supercooled liquid water remains a topic of much debate. An LLT has been rigorously proved in three empirically parametrized molecular models of water, and evidence consistent with an LLT has been reported for several other such models. In contrast, experimental proof of this phenomenon has been elusive due to rapid ice nucleation under deeply supercooled conditions. In this work, we combined density functional theory (DFT), machine learning, and molecular simulations to shed additional light on the possible existence of an LLT in water. We trained a deep neural network (DNN) model to represent the ab initio potential energy surface of water from DFT calculations using the Strongly Constrained and Appropriately Normed (SCAN) functional. We then used advanced sampling simulations in the multithermal–multibaric ensemble to efficiently explore the thermophysical properties of the DNN model. The simulation results are consistent with the existence of an LLCP, although they do not constitute a rigorous proof thereof. We fit the simulation data to a two-state equation of state to provide an estimate of the LLCP’s location. These combined results—obtained from a purely first-principles approach with no empirical parameters—are strongly suggestive of the existence of an LLT, bolstering the hypothesis that water can separate into two distinct liquid forms.

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