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Title: How Cubic Can Ice Be?

Using an X-ray laser, we investigated the crystal structure of ice formed by homogeneous ice nucleation in deeply supercooled water nanodrops (r ≈ 10 nm) at ~225 K. The nanodrops were formed by condensation of vapor in a supersonic nozzle, and the ice was probed within 100 μs of freezing using femtosecond wide-angle X-ray scattering at the Linac Coherent Light Source free-electron X-ray laser. The X-ray diffraction spectra indicate that this ice has a metastable, predominantly cubic structure; the shape of the first ice diffraction peak suggests stacking-disordered ice with a cubicity value, χ, in the range of 0.78 ± 0.05. The cubicity value determined here is higher than those determined in experiments with micron-sized drops but comparable to those found in molecular dynamics simulations. Lastly, the high cubicity is most likely caused by the extremely low freezing temperatures and by the rapid freezing, which occurs on a ~1 μs time scale in single nanodroplets.
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;  [3] ; ORCiD logo [4] ;  [2] ;  [5] ;  [6] ;  [7] ;  [8] ;  [6] ;  [2] ;  [9] ; ORCiD logo [2] ; ORCiD logo [10]
  1. The Ohio State Univ., Columbus, OH (United States). William G. Lowrie Dept. of Chemical and Biomolecular Engineering
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); National Univ. of Singapore (Singapore). Dept. of Physics
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stockholm Univ. (Sweden). AlbaNova Univ. Center, Dept. of Physics; KTH Royal Inst. of Technology, Stockholm (Sweden). AlbaNova Univ. Center, Dept. of Applied Physics, Biomedical and X-ray Physics; SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science & Catalysis
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science & Catalysis; Stanford Univ., CA (United States). Dept. of Chemistry
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); Brookhaven National Lab. (BNL), Upton, NY (United States)
  8. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); National Science Foundation (NSF), Buffalo, NY (United States). BioXFEL Science and Technology Center
  9. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stockholm Univ. (Sweden). AlbaNova Univ. Center, Dept. of Physics; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  10. The Ohio State Univ., Columbus, OH (United States). William G. Lowrie Dept. of Chemical and Biomolecular Engineering; The Ohio State Univ., Columbus, OH (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Grant/Contract Number:
CHE-1213959; CHE-1464924; AC02-76SF00515; AC02-06CH11357
Type:
Published Article
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1368595
Alternate Identifier(s):
OSTI ID: 1368366; OSTI ID: 1372318

Amaya, Andrew J., Pathak, Harshad, Modak, Viraj P., Laksmono, Hartawan, Loh, N. Duane, Sellberg, Jonas A., Sierra, Raymond G., McQueen, Trevor A., Hayes, Matt J., Williams, Garth J., Messerschmidt, Marc, Boutet, Sébastien, Bogan, Michael J., Nilsson, Anders, Stan, Claudiu A., and Wyslouzil, Barbara E.. How Cubic Can Ice Be?. United States: N. p., Web. doi:10.1021/acs.jpclett.7b01142.
Amaya, Andrew J., Pathak, Harshad, Modak, Viraj P., Laksmono, Hartawan, Loh, N. Duane, Sellberg, Jonas A., Sierra, Raymond G., McQueen, Trevor A., Hayes, Matt J., Williams, Garth J., Messerschmidt, Marc, Boutet, Sébastien, Bogan, Michael J., Nilsson, Anders, Stan, Claudiu A., & Wyslouzil, Barbara E.. How Cubic Can Ice Be?. United States. doi:10.1021/acs.jpclett.7b01142.
Amaya, Andrew J., Pathak, Harshad, Modak, Viraj P., Laksmono, Hartawan, Loh, N. Duane, Sellberg, Jonas A., Sierra, Raymond G., McQueen, Trevor A., Hayes, Matt J., Williams, Garth J., Messerschmidt, Marc, Boutet, Sébastien, Bogan, Michael J., Nilsson, Anders, Stan, Claudiu A., and Wyslouzil, Barbara E.. 2017. "How Cubic Can Ice Be?". United States. doi:10.1021/acs.jpclett.7b01142.
@article{osti_1368595,
title = {How Cubic Can Ice Be?},
author = {Amaya, Andrew J. and Pathak, Harshad and Modak, Viraj P. and Laksmono, Hartawan and Loh, N. Duane and Sellberg, Jonas A. and Sierra, Raymond G. and McQueen, Trevor A. and Hayes, Matt J. and Williams, Garth J. and Messerschmidt, Marc and Boutet, Sébastien and Bogan, Michael J. and Nilsson, Anders and Stan, Claudiu A. and Wyslouzil, Barbara E.},
abstractNote = {Using an X-ray laser, we investigated the crystal structure of ice formed by homogeneous ice nucleation in deeply supercooled water nanodrops (r ≈ 10 nm) at ~225 K. The nanodrops were formed by condensation of vapor in a supersonic nozzle, and the ice was probed within 100 μs of freezing using femtosecond wide-angle X-ray scattering at the Linac Coherent Light Source free-electron X-ray laser. The X-ray diffraction spectra indicate that this ice has a metastable, predominantly cubic structure; the shape of the first ice diffraction peak suggests stacking-disordered ice with a cubicity value, χ, in the range of 0.78 ± 0.05. The cubicity value determined here is higher than those determined in experiments with micron-sized drops but comparable to those found in molecular dynamics simulations. Lastly, the high cubicity is most likely caused by the extremely low freezing temperatures and by the rapid freezing, which occurs on a ~1 μs time scale in single nanodroplets.},
doi = {10.1021/acs.jpclett.7b01142},
journal = {Journal of Physical Chemistry Letters},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {6}
}