Abstract
The induction of homogeneous and oriented ice nucleation has to date not been achieved. Here, we report induced nucleation of ice from millimeter sized supercooled water drops illuminated by ns-optical laser pulses well below the ionization threshold making use of particular laser beam configurations and polarizations. Employing a 100 ps synchrotron x-ray pulse 100 ns after each laser pulse, an unambiguous correlation was observed between the directions and the symmetry of the laser fields and that of the H-bonding arrays of the induced ice crystals. Moreover, an analysis of the x-ray diffraction data indicates that, in the main, the induced nucleation of ice is homogeneous at temperatures well above the observed and predicted values for supercooled water.
Highlights
The phenomenon of ice nucleation from supercooled water, which has far-reaching ramifications for the living and nonliving world, commonly involves heterogeneous interfaces
Employing a 100 ps synchrotron x-ray pulse 100 ns after each laser pulse, an unambiguous correlation was observed between the directions and the symmetry of the laser fields and that of the H-bonding arrays of the induced ice crystals
We have provided CCD images and x-ray diffraction patterns of ice nucleation that occurred at significantly higher temperatures only under the effect of the laser pulses
Summary
The phenomenon of ice nucleation from supercooled water, which has far-reaching ramifications for the living and nonliving world, commonly involves heterogeneous interfaces. Homogeneous ice nucleation, i.e., far from a pre-existing interface, on the other hand, has remained a challenge to induce and explore. It involves a stochastic element whereby the initial time and location of nucleation are a priori unknown. Attempts by Stan et al. to induce homogeneous ice nucleation with an alternating electric field (3 kHz–100 kHz) at 105 V/m were unsuccessful. Insight on homogeneous nucleation indicating that ice-forming nuclei last ∼100 ns has been gleaned from molecular dynamic (MD) simulations.
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