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  • Pathak, HarshadStockholms universitet,Fysikum,Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden; (author)

Enhancement and maximum in the isobaric specific-heat capacity measurements of deeply supercooled water using ultrafast calorimetry

  • Article/chapterEnglish2021

Publisher, publication year, extent ...

  • 2021-02
  • Proceedings of the National Academy of Sciences,2021
  • printrdacarrier

Numbers

  • LIBRIS-ID:oai:DiVA.org:su-190883
  • https://urn.kb.se/resolve?urn=urn:nbn:se:su:diva-190883URI
  • https://doi.org/10.1073/pnas.2018379118DOI
  • https://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-309920URI

Supplementary language notes

  • Language:English
  • Summary in:English

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  • Subject category:ref swepub-contenttype
  • Subject category:art swepub-publicationtype

Notes

  • The importance of molecular understanding of the structure, dynamics. and properties of liquid water is recognized in many scientific disciplines. Here, we study experimentally the structure and thermodynamics of bulk liquid water as it is supercooled by evaporation down to ∼228 K. The unique aspect of this work is the use of ultrafast calorimetry that enables us to determine the specific-heat capacity of water to unprecedentedly low temperatures. The observed maximum of about 218 J/mol/K at 229 K is consistent with the liquid–liquid critical point model and supports a proposed fragile-to-strong transition at ∼220 K to explain the steep decrease in the estimated self-diffusion coefficient below 235 K. 
  • QC 20220317
  • 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.

Subject headings and genre

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  • Späh, AlexanderStockholms universitet,Fysikum,Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden;(Swepub:su)alsp4980 (author)
  • Esmaeildoost, NiloofarKTH,Biomedicinsk fysik och röntgenfysik(Swepub:kth)u12nxvp4 (author)
  • Sellberg, Jonas A.,1985-KTH,Biomedicinsk fysik och röntgenfysik(Swepub:kth)u1ynvdbz (author)
  • Kim, Kyung HwanDepartment of Chemistry, Pohang University of Science and Technology, Pohang 37673, Republic of Korea; (author)
  • Perakis, FivosStockholms universitet,Fysikum,Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden;(Swepub:su)fpera (author)
  • Amann-Winkel, KatrinStockholms universitet,Fysikum,Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden;(Swepub:su)kaama (author)
  • Ladd-Parada, MarjorieStockholms universitet,Fysikum,Department of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden;(Swepub:kth)u14ecfv6 (author)
  • Koliyadu, Jayanath C. P.KTH,Biomedicinsk fysik och röntgenfysik(Swepub:kth)u18un8r9 (author)
  • Lane, Thomas J.SLAC National Accelerator Laboratory, Linac Coherent Light Source, Menlo Park, CA 94025; (author)
  • Yang, CheolheeDepartment of Chemistry, Pohang University of Science and Technology, Pohang 37673, Republic of Korea; (author)
  • Lemke, Henrik TillSwissFEL, Paul Scherrer Institute, CH-5232 Villigen, Switzerland (author)
  • Oggenfuss, Alexander RolandSwissFEL, Paul Scherrer Institute, CH-5232 Villigen, Switzerland (author)
  • Johnson, Philip J. M.SwissFEL, Paul Scherrer Institute, CH-5232 Villigen, Switzerland (author)
  • Deng, YunpeiSwissFEL, Paul Scherrer Institute, CH-5232 Villigen, Switzerland (author)
  • Zerdane, SerhaneSwissFEL, Paul Scherrer Institute, CH-5232 Villigen, Switzerland (author)
  • Mankowsky, RomanSwissFEL, Paul Scherrer Institute, CH-5232 Villigen, Switzerland (author)
  • Beaud, PaulSwissFEL, Paul Scherrer Institute, CH-5232 Villigen, Switzerland (author)
  • Nilsson, AndersDepartment of Physics, AlbaNova University Center, Stockholm University, SE-10691 Stockholm, Sweden; (author)
  • Stockholms universitetFysikum (creator_code:org_t)

Related titles

  • In:Proceedings of the National Academy of Sciences of the United States of America: Proceedings of the National Academy of Sciences118:60027-84241091-6490

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