Experimental observation of mesoscopic fluctuations to identify origin of thermodynamic anomalies of ambient liquid water

Kajihara, Y.; Inui, Masanori; Matsuda, Kazuhiro; Ishikawa, Daisuke; Tsutsui, Satoshi; Baron, Alfred Q. R.

doi:10.1103/physrevresearch.5.013120

Cited by 3 publications

(4 citation statements)

References 77 publications

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“…With cooling from 1123 K to approximately 750 K (1b), S 0 gradually decreased, which can be interpreted as the liquid becoming more homogeneous because it moved away from the critical point of liquid-gas transition (LGT), which should be located at a higher temperature. This behavior is more clearly seen for liquid water [25]. In contrast, in the LLT region, S 0 clearly increases to a maximum at approximately 620-630 K. This behavior of maximum scattering intensity of supercooled liquid Te was also confirmed in later similar experiment, and more detailed discussions including the large-Q region have been made [21].…”

Section: Results Of Liquid Tesupporting

confidence: 66%

“…We have devised and proposed a 'dynamical fluctuation' strength measurement method using sound waves as a method to detect such 'fluctuations' beyond static density inhomogeneity. We have actually applied this method to liquid Te [9] and liquid water [25] and confirmed that such dynamic fluctuations exist over a wide range in the real liquid region above T m for both materials. In the case of water, in particular, the measured change in dynamic fluctuation strength is linked to that of the isochoric specific heat over a wide temperature and pressure ranges, strongly suggesting that such dynamical fluctuation is the actual origin of the specific heat anomaly.…”

Section: Discussionmentioning

confidence: 59%

“…In the case of water, in particular, the measured change in dynamic fluctuation strength is linked to that of the isochoric specific heat over a wide temperature and pressure ranges, strongly suggesting that such dynamical fluctuation is the actual origin of the specific heat anomaly. The discussion on the essence of static and dynamical fluctuations is speculative at this stage [9,25] and is an issue for future work. But in any case, by considering the existence of LLT and the effect of static and dynamical fluctuations associated with it, not just Te and water, we hope that our understanding of the thermodynamics of liquids will be deepened.…”

Section: Discussionmentioning

confidence: 99%

“…Meanwhile, liquid water exhibits thermodynamic anomalies (review [22]) similar to those of liquid Te [9,13,[23][24][25] and is often referred to as an 'anomalous liquid'. The density is greatest at 277 K, which is slightly above T m (273 K), the pressure variation of T m is negative, the heat capacity shows a divergent-like increase in the supercooled region, and the ultrasonic sound velocity shows a maximum at approximately 350 K. Furthermore, models that can be classified under the LLT concept (review [26].…”

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Existence of density inhomogeneity of liquid Te associated with liquid–liquid phase transition

Kajihara,

Inui,

Matsuda

et al. 2024

J. Phys.: Condens. Matter

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We performed small-angle X-ray scattering measurements of liquid Te using a synchrotron radiation facility and observed maximum scattering intensity near 620 K in the supercooled region (melting temperature 723 K). This indicates that density inhomogeneity exists in liquid Te, and the fact that this temperature coincides with the temperature at which the specific heat, sound velocity, and thermal expansion coefficient reach their maxima means that this density inhomogeneity is the cause of these thermodynamic anomalies. The thermodynamic anomalies in liquid Te had already been shown in the 1980s to be comprehensively explained by the inhomogeneity associated with the continuous liquid-liquid phase transition (LLT), but direct experimental evidence for the existence of the inhomogeneity had not been obtained. The present results, together with those already obtained for mixture systems (Te-Se, Te-Ge), indicate the existence of inhomogeneity associated with LLT in liquid Te systems, and strongly support the model. Recently, similarmaximum scattering intensity has also been observed in supercooled liquid water, which exhibits thermodynamic anomalies similar to those of Te, indicating the universality of the inhomogeneous model or LLT scenario to explain the thermodynamics of such "anomalous liquids". Further development of the LLT scenario is expected in near future.

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Section: Results Of Liquid Tesupporting

confidence: 66%

Section: Discussionmentioning

confidence: 59%

Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Existence of density inhomogeneity of liquid Te associated with liquid–liquid phase transition

Kajihara,

Inui,

Matsuda

et al. 2024

J. Phys.: Condens. Matter

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Mysteries of Water and Other Anomalous Liquids: “Slow” Sound and Relaxing Compressibility and Heat Capacity (Brief Review)

2023

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Mysteries of Water and Other Anomalous Liquids: “Slow” Sound and Relaxing Compressibility and Heat Capacity (Brief Review)

Brazhkin,

Danilov,

Tsiok

2023

Pisʹma v žurnal êksperimentalʹnoj i teoretičeskoj fiziki

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Reasons for the existence of “fast” sound at terahertz frequencies in various liquids have been analyzed. It has been shown that the fast sound speed is described well by the conventional formula from the theory of elasticity, where ρ is the density of a liquid andandare the bulk and shear moduli at the frequency ω, respectively. The excess of the speed of fast sound over the speed of normal sound in “normal” liquids is 10–20% and is almost completely determined by the contribution of the shear modulusat high frequencies, and vanishes on the Frenkel line. At the same time, the huge excess (50–120%) of the fast speed of sound over the speed of normal sound in some liquids (called “anomalous”), such as water and tellurium melt, is due mainly to the strong frequency dependence of the bulk modulus. Anomalously low relaxing bulk moduli were studied in our previous works for many oxide and chalcogenide glasses near smeared pressure-induced phase transitions. In anomalous liquids, smeared phase transitions also occur in a wide temperature and pressure region, which sharply reduces the bulk moduli and speeds of sound. Thus, the record large difference between speeds of fast and normal sound in anomalous liquids is due not to anomalously fast sound but to the fact that normal sound in such liquids is anomalously “slow” and bulk moduli are anomalously low. Ultrasonic studies of low- and high-density amorphous water ices show that their bulk moduli are indeed a factor of 4–5 higher than the bulk modulus of water. In addition, because of smeared phase transitions, the heat capacities of water and tellurium melt are a factor of 1.5–2 higher than those for normal liquids; i.e., anomalous liquids are characterized not only by an anomalous (nonmonotonic) behavior but also by anomalous magnitudes of physical quantities for most of the available measurement methods. A similar anomalous increase in the compressibility and heat capacity is observed for all fluids in the close vicinity of the liquid–gas critical point. In this case, anomalously fast sound is observed at terahertz frequencies, which is also due to a sharp increase in the bulk modulusat high frequencies. At the same time, high compressibility and heat capacity, as well as a large excess of the speed of fast sound over the speed of normal sound, for anomalous liquids and glasses near smeared phase transitions are not necessarily due to the proximity of critical points and occur in any scenario of the smeared phase transition.

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Experimental observation of mesoscopic fluctuations to identify origin of thermodynamic anomalies of ambient liquid water

Cited by 3 publications

References 77 publications

Existence of density inhomogeneity of liquid Te associated with liquid–liquid phase transition

Existence of density inhomogeneity of liquid Te associated with liquid–liquid phase transition

Mysteries of Water and Other Anomalous Liquids: “Slow” Sound and Relaxing Compressibility and Heat Capacity (Brief Review)

Mysteries of Water and Other Anomalous Liquids: “Slow” Sound and Relaxing Compressibility and Heat Capacity (Brief Review)

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