Low-temperature properties of glassy and crystalline states of n-butanol

Кривчиков, А. И.; Hassaine, Merzak; Sharapova, I. V.; Korolyuk, O. A.; Riobóo, R. J. Jiménez; Ramos, M. A.

doi:10.1016/j.jnoncrysol.2010.05.081

Cited by 22 publications

(16 citation statements)

References 48 publications

(75 reference statements)

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“…Each scenario captures a certain feature of the glacial phase, but fails in explaining all of the experimental results in a consistent manner. Similar situations are often seen in other candidates of LLTs, such as l-butanol [LLT (13) vs. microcrystallization (40)(41)(42)(43)], confined water [LLT (5) vs. other phenomena (44)(45)(46)], and aqueous solutions [LLT (6, 7) vs. microcrystallization (8,28,47,48)]. For TPP, however, some pieces of experimental evidence supportive of the LLT scenario rather than the microcrystallization scenario have recently been reported (11,12).…”

supporting

confidence: 53%

Microscopic identification of the order parameter governing liquid–liquid transition in a molecular liquid

Murata

Tanaka

2015

Proc. Natl. Acad. Sci. U.S.A.

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A liquid-liquid transition (LLT) in a single-component substance is an unconventional phase transition from one liquid to another. LLT has recently attracted considerable attention because of its fundamental importance in our understanding of the liquid state. To access the order parameter governing LLT from a microscopic viewpoint, here we follow the structural evolution during the LLT of an organic molecular liquid, triphenyl phosphite (TPP), by timeresolved small-and wide-angle X-ray scattering measurements. We find that locally favored clusters, whose characteristic size is a few nanometers, are spontaneously formed and their number density monotonically increases during LLT. This strongly suggests that the order parameter of LLT is the number density of locally favored structures and of nonconserved nature. We also show that the locally favored structures are distinct from the crystal structure and these two types of orderings compete with each other. Thus, our study not only experimentally identifies the structural order parameter governing LLT, but also may settle a longstanding debate on the nature of the transition in TPP, i.e., whether the transition is LLT or merely microcrystal formation.liquid-liquid transition | order parameter | X-ray scattering | locally favored structure | transition kinetics L iquid-liquid transition (LLT) is an intriguing phenomenon in which a liquid transforms into another one via a first-order transition. This means that there can be more than two liquid states for a single-component substance. Despite its counterintuitive nature, there have recently been many pieces of experimental and numerical evidence for the existence of LLT, for various liquids such as water (1-5), aqueous solutions (6-8), triphenyl phosphite (9-12), l-butanol (13), phosphorus (14), silicon (15, 16), germanium (17), and Y 2 O 3 -Al 2 O 3 (18,19). This suggests that the LLT may be rather universally observed for various types of liquids. However, none of the LLTs reported so far is free from criticisms (20, 21), mainly because these LLTs take place under experimentally difficult conditions [e.g., at high temperature and pressure (14,15,(17)(18)(19)] or in a supercooled state below the melting point (1-3, 5-7, 9, 10), where the transition is inevitably contaminated by microcrystal formation. The latter is not limited to experiments but arises in numerical simulations, often causing many controversies vs. crystallization (26-28)]. For ST2 water, however, this issue has recently been settled by an extensive simulation study by Palmer et al. (4).One of the hottest and long-standing debates is on the nature of the transition found in a molecular liquid, triphenyl phosphite (TPP), by Kivelson and his coworkers (29). The transition is very easy to access experimentally, because it takes place at ambient pressure and at a temperature range between 230 and 210 K and the transformation speed is slow enough to follow the kinetics. Since the finding of this transition (29, 30), many researchers thus have been inte...

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supporting

confidence: 53%

Microscopic identification of the order parameter governing liquid–liquid transition in a molecular liquid

Murata

Tanaka

2015

Proc. Natl. Acad. Sci. U.S.A.

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“…Notice that the SPM values of E d are in qualitative and quantitative agreement with E b found from experimental results [3,[5][6][7]21,32,33,35]. It is known that the boundary energy E b , like many other features of the glass state (plateau in thermal conductivity curves, smeared maximum C p (T)/T 3 , etc.)…”

Section: Discussionsupporting

confidence: 84%

“…The dependences of the parameters W/k B (subpanel а) and À С (subpanel b) on the molecular mass of the alcohols obtained from the experimental data on heat capacity [7,32] and thermal conductivity (this work) and calculated by Eq. (2) are shown in Fig.…”

Section: Discussionmentioning

confidence: 99%

See 1 more Smart Citation

Thermal conductivity of glassy primary mono-hydroxylalcohols

Кривчиков

Korolyuk

Sharapova

et al. 2011

Journal of Non-Crystalline Solids

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“…Further details on the experimental methods followed can be found in Ref. 50, where earlier experiments conducted on glassy and crystalline phases of n-butanol were described.…”

Section: Experimental Techniques and Materialsmentioning

confidence: 99%

Low-temperature thermal and elastoacoustic properties of butanol glasses: Study of position isomerism effects around the boson peak

et al. 2012

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We have concurrently measured the specific heat, the thermal conductivity, and the longitudinal and transverse sound velocities at low temperature of glasses from different isomers of butanol (n-butanol, sec-butanol and isobutanol), as well as the low-temperature specific heat for the crystals of n-butanol, isobutanol and tert-butanol. Whereas the elastic constants both for crystals and glasses are found to be almost independent of the position of the hydrogen bonds, the thermal properties at low temperatures of these glasses at a few kelvin (around the boson peak in the reduced specific heat or around the plateau in the thermal conductivity) are found to vary strongly. Our experiments clearly contradict other works or models claiming a Debye scaling of the boson peak, and hence of the excess low-temperature specific heat of glasses. Data analysis based upon the soft-potential model and its extensions allows us to estimate the Ioffe-Regel limit in these and other alcohol glasses, finding a correlation with the boson-peak position in agreement with that previously reported by other groups.

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Low-temperature properties of glassy and crystalline states of n-butanol

Cited by 22 publications

References 48 publications

Microscopic identification of the order parameter governing liquid–liquid transition in a molecular liquid

Microscopic identification of the order parameter governing liquid–liquid transition in a molecular liquid

Thermal conductivity of glassy primary mono-hydroxylalcohols

Low-temperature thermal and elastoacoustic properties of butanol glasses: Study of position isomerism effects around the boson peak

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