title: Anomalous Behavior of the Homogeneous Ice Nucleation Rate in "No-Man's Land".
abstract: We present an analysis of ice nucleation kinetics from near-ambient pressure water as temperature decreases below the homogeneous limitTHby cooling micrometer-sized droplets (microdroplets) evaporatively at 103-104K/s and probing the structure ultrafast using femtosecond pulses from the Linac Coherent Light Source (LCLS) free-electron X-ray laser. Below 232 K, we observed a slower nucleation rate increase with decreasing temperature than anticipated from previous measurements, which we suggest is due to the rapid decrease in water's diffusivity. This is consistent with earlier findings that microdroplets do not crystallize at <227 K, but vitrify at cooling rates of 106-107K/s. We also hypothesize that the slower increase in the nucleation rate is connected with the proposed "fragile-to-strong" transition anomaly in water.
authors.affiliation: PULSE Institute, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States.
authors.forename: Hartawan
authors.initials: H
authors.lastname: Laksmono
authors.affiliation: SUNCAT Ctr Interface Sci & Catalysis, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States ; Department of Chemistry, Stanford University , Stanford, California 94305, United States.
authors.forename: Trevor A
authors.initials: TA
authors.lastname: McQueen
authors.affiliation: SUNCAT Ctr Interface Sci & Catalysis, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States ; Department of Physics, AlbaNova University Center, Stockholm University , S-106 91 Stockholm, Sweden.
authors.forename: Jonas A
authors.initials: JA
authors.lastname: Sellberg
authors.affiliation: PULSE Institute, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States ; Center for Bio-Imaging Sciences, National University of Singapore , Singapore 117543.
authors.forename: N Duane
authors.initials: ND
authors.lastname: Loh
authors.affiliation: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States.
authors.forename: Congcong
authors.initials: C
authors.lastname: Huang
authors.affiliation: Department of Physics, AlbaNova University Center, Stockholm University , S-106 91 Stockholm, Sweden.
authors.forename: Daniel
authors.initials: D
authors.lastname: Schlesinger
authors.affiliation: PULSE Institute, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States.
authors.forename: Raymond G
authors.initials: RG
authors.lastname: Sierra
authors.affiliation: PULSE Institute, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States.
authors.forename: Christina Y
authors.initials: CY
authors.lastname: Hampton
authors.affiliation: Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States.
authors.forename: Dennis
authors.initials: D
authors.lastname: Nordlund
authors.affiliation: SUNCAT Ctr Interface Sci & Catalysis, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States ; Institute for Methods and Instrumentation in Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH , Wilhelm-Conrad-Röntgen Campus, Albert-Einstein-Strasse 15, 12489 Berlin, Germany.
authors.forename: Martin
authors.initials: M
authors.lastname: Beye
authors.affiliation: Center for Free-Electron Laser Science, DESY, Notkestrasse 85, 22607 Hamburg, Germany.
authors.forename: Andrew V
authors.initials: AV
authors.lastname: Martin
authors.affiliation: Center for Free-Electron Laser Science, DESY, Notkestrasse 85, 22607 Hamburg, Germany.
authors.forename: Anton
authors.initials: A
authors.lastname: Barty
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States.
authors.forename: M Marvin
authors.initials: MM
authors.lastname: Seibert
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States ; National Science Foundation BioXFEL Science and Technology Center, 700 Ellicott Street, Buffalo, New York 14203, United States.
authors.forename: Marc
authors.initials: M
authors.lastname: Messerschmidt
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States.
authors.forename: Garth J
authors.initials: GJ
authors.lastname: Williams
authors.affiliation: Linac Coherent Light Source, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States.
authors.forename: Sébastien
authors.initials: S
authors.lastname: Boutet
authors.affiliation: Department of Physics, AlbaNova University Center, Stockholm University , S-106 91 Stockholm, Sweden ; Institute of Physical Chemistry, University of Innsbruck , Innrain 80-82, A-6020 Innsbruck, Austria.
authors.forename: Katrin
authors.initials: K
authors.lastname: Amann-Winkel
authors.affiliation: Institute of Physical Chemistry, University of Innsbruck , Innrain 80-82, A-6020 Innsbruck, Austria.
authors.forename: Thomas
authors.initials: T
authors.lastname: Loerting
authors.affiliation: Department of Physics, AlbaNova University Center, Stockholm University , S-106 91 Stockholm, Sweden.
authors.forename: Lars G M
authors.initials: LG
authors.lastname: Pettersson
authors.affiliation: PULSE Institute, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States.
authors.forename: Michael J
authors.initials: MJ
authors.lastname: Bogan
authors.affiliation: SUNCAT Ctr Interface Sci & Catalysis, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States ; Department of Physics, AlbaNova University Center, Stockholm University , S-106 91 Stockholm, Sweden ; Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory , 2575 Sand Hill Road, Menlo Park, California 94025, United States.
authors.forename: Anders
authors.initials: A
authors.lastname: Nilsson