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Title: Temperature-Independent Nuclear Quantum Effects on the Structure of Water

Nuclear quantum effects (NQEs) have a significant influence on the hydrogen bonds in water and aqueous solutions and have thus been the topic of extensive studies. However, the microscopic origin and the corresponding temperature dependence of NQEs have been elusive and still remain the subject of ongoing discussion. Previous x-ray scattering investigations indicate that NQEs on the structure of water exhibit significant temperature dependence. Here, by performing wide-angle x-ray scattering of H 2O and D 2O droplets at temperatures from 275 K down to 240 K, we determine the temperature dependence of NQEs on the structure of water down to the deeply supercooled regime. The data reveal that the magnitude of NQEs on the structure of water is temperature independent, as the structure factor of D 2O is similar to H 2O if the temperature is shifted by a constant 5 K, valid from ambient conditions to the deeply supercooled regime. Analysis of the accelerated growth of tetrahedral structures in supercooled H 2O and D 2O also shows similar behavior with a clear 5 K shift. The results indicate a constant compensation between NQEs delocalizing the proton in the librational motion away from the bond and in the OH stretchmore » vibrational modes along the bond. In conclusion, this is consistent with the fact that only the vibrational ground state is populated at ambient and supercooled conditions.« less
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [1] ;  [1]
  1. Stockholm Univ., Stockholm (Sweden)
  2. KTH Royal Institute of Technology, Stockholm (Sweden)
  3. Japan Synchrotron Radiation Research Institute, Hyogo (Japan)
  4. The Univ. of Tokyo, Chiba (Japan)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515; 667205; 2013-8823; 2016B8055
Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 119; Journal Issue: 7; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
OSTI Identifier:
1390302

Kim, Kyung Hwan, Pathak, Harshad, Spah, Alexander, Perakis, Fivos, Mariedahl, Daniel, Sellberg, Jonas A., Katayama, Tetsuo, Harada, Yoshihisa, Ogasawara, Hirohito, Pettersson, Lars G. M., and Nilsson, Anders. Temperature-Independent Nuclear Quantum Effects on the Structure of Water. United States: N. p., Web. doi:10.1103/physrevlett.119.075502.
Kim, Kyung Hwan, Pathak, Harshad, Spah, Alexander, Perakis, Fivos, Mariedahl, Daniel, Sellberg, Jonas A., Katayama, Tetsuo, Harada, Yoshihisa, Ogasawara, Hirohito, Pettersson, Lars G. M., & Nilsson, Anders. Temperature-Independent Nuclear Quantum Effects on the Structure of Water. United States. doi:10.1103/physrevlett.119.075502.
Kim, Kyung Hwan, Pathak, Harshad, Spah, Alexander, Perakis, Fivos, Mariedahl, Daniel, Sellberg, Jonas A., Katayama, Tetsuo, Harada, Yoshihisa, Ogasawara, Hirohito, Pettersson, Lars G. M., and Nilsson, Anders. 2017. "Temperature-Independent Nuclear Quantum Effects on the Structure of Water". United States. doi:10.1103/physrevlett.119.075502. https://www.osti.gov/servlets/purl/1390302.
@article{osti_1390302,
title = {Temperature-Independent Nuclear Quantum Effects on the Structure of Water},
author = {Kim, Kyung Hwan and Pathak, Harshad and Spah, Alexander and Perakis, Fivos and Mariedahl, Daniel and Sellberg, Jonas A. and Katayama, Tetsuo and Harada, Yoshihisa and Ogasawara, Hirohito and Pettersson, Lars G. M. and Nilsson, Anders},
abstractNote = {Nuclear quantum effects (NQEs) have a significant influence on the hydrogen bonds in water and aqueous solutions and have thus been the topic of extensive studies. However, the microscopic origin and the corresponding temperature dependence of NQEs have been elusive and still remain the subject of ongoing discussion. Previous x-ray scattering investigations indicate that NQEs on the structure of water exhibit significant temperature dependence. Here, by performing wide-angle x-ray scattering of H2O and D2O droplets at temperatures from 275 K down to 240 K, we determine the temperature dependence of NQEs on the structure of water down to the deeply supercooled regime. The data reveal that the magnitude of NQEs on the structure of water is temperature independent, as the structure factor of D2O is similar to H2O if the temperature is shifted by a constant 5 K, valid from ambient conditions to the deeply supercooled regime. Analysis of the accelerated growth of tetrahedral structures in supercooled H2O and D2O also shows similar behavior with a clear 5 K shift. The results indicate a constant compensation between NQEs delocalizing the proton in the librational motion away from the bond and in the OH stretch vibrational modes along the bond. In conclusion, this is consistent with the fact that only the vibrational ground state is populated at ambient and supercooled conditions.},
doi = {10.1103/physrevlett.119.075502},
journal = {Physical Review Letters},
number = 7,
volume = 119,
place = {United States},
year = {2017},
month = {8}
}