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DOI	10.1073/pnas.2018379118
	Enhancement and maximum in the isobaric specific-heat capacity measurements of deeply supercooled water using ultrafast calorimetry
	Pathak H.; Späh A.; Esmaeildoost N.; Sellberg J.A.; Kim K.H.; Perakis F.; Amann-Winkel K.; Ladd-Parada M.; Koliyadu J.; Lane T.J.; Yang C.; Lemke H.T.; Oggenfuss A.R.; Johnson P.J.M.; Deng Y.; Zerdane S.; Mankowsky R.; Beaud P.; Nilsson A.
发表日期	2021
ISSN	00278424
卷号	118 期号:6
英文摘要	Knowledge of the temperature dependence of the isobaric specific heat (Cp) upon deep supercooling can give insights regarding the anomalous properties of water. If a maximum in Cp exists at a specific temperature, as in the isothermal compressibility, it would further validate the liquid-liquid critical point model that can explain the anomalous increase in thermodynamic response functions. The challenge is that the relevant temperature range falls in the region where ice crystallization becomes rapid, which has previously excluded experiments. Here, we have utilized a methodology of ultrafast calorimetry by determining the temperature jump from femtosecond X-ray pulses after heating with an infrared laser pulse and with a sufficiently long time delay between the pulses to allow measurements at constant pressure. Evaporative cooling of ∼15-μm diameter droplets in vacuum enabled us to reach a temperature down to ∼228 K with a small fraction of the droplets remaining unfrozen. We observed a sharp increase in Cp, from 88 J/mol/K at 244 K to about 218 J/mol/K at 229 K where a maximum is seen. The Cp maximum is at a similar temperature as the maxima of the isothermal compressibility and correlation length. From the Cp measurement, we estimated the excess entropy and self-diffusion coefficient of water and these properties decrease rapidly below 235 K. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	Fragile-to-strong transition; Liquid-liquid critical point; Specific-heat capacity; Supercooled water
语种	英语
scopus关键词	deeply supercooled water; unclassified drug; water; Article; calorimetry; cooling; critical temperature; diffusion coefficient; entropy; evaporation; heating; isobaric specific heat capacity measurement; pressure; priority journal; temperature measurement; thermodynamics; ultrafast calorimetry; vacuum; water analysis; X ray
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/180701
作者单位	Department of Physics, AlbaNova University Center, Stockholm University, Stockholm, SE-10691, Sweden; Biomedical and X-Ray Physics, Department of Applied Physics, KTH Royal Institute of Technology, AlbaNova University Center, Stockholm, SE-10691, Sweden; Department of Chemistry, Pohang University of Science and Technology, Pohang, 37673, South Korea; SLAC National Accelerator Laboratory, Linac Coherent Light Source, Menlo Park, CA 94025, United States; SwissFEL, Paul Scherrer Institute, Villigen, CH-5232, Switzerland
推荐引用方式 GB/T 7714	Pathak H.,Späh A.,Esmaeildoost N.,et al. Enhancement and maximum in the isobaric specific-heat capacity measurements of deeply supercooled water using ultrafast calorimetry[J],2021,118(6).
APA	Pathak H..,Späh A..,Esmaeildoost N..,Sellberg J.A..,Kim K.H..,...&Nilsson A..(2021).Enhancement and maximum in the isobaric specific-heat capacity measurements of deeply supercooled water using ultrafast calorimetry.Proceedings of the National Academy of Sciences of the United States of America,118(6).
MLA	Pathak H.,et al."Enhancement and maximum in the isobaric specific-heat capacity measurements of deeply supercooled water using ultrafast calorimetry".Proceedings of the National Academy of Sciences of the United States of America 118.6(2021).