Ultrafast superheating and melting of bulk ice

Abstract

The superheating of a solid to a temperature beyond its melting point, without the solid actually melting, is a well-known phenomenon. It occurs with many substances, particularly those that can readily be produced as high-quality crystals. In principle, ice should also be amenable to superheating. But the complex three-dimensional network of hydrogen bonds that holds water molecules together and gives rise to unusual solid and liquid properties strongly affects the melting behaviour of ice; in particular, ice usually contains many defects owing to the directionality of its hydrogen bonds. However, simulations are readily able to 'create' defect-free ice that can be superheated. Here we show that by exciting the OH stretching mode of water, it is possible to superheat ice. When using an ice sample at an initial temperature of 270 K, we observe an average temperature rise of 20 +/- 2 K that persists over the monitored time interval of 250 ps without melting.

Ultrafast conversions between hydrogen bonded structures in liquid water observed by femtosecond x-ray spectroscopy

“…The heated water volume expands adiabatically on nanosecond time scales, similar to the behavior of ice. 24,38 This is evidenced by the partial absorption recovery at nanosecond delays, seen in Fig. 2 and the inset of Fig.…”

Two-dimensional infrared spectroscopy of isotope-diluted ice Ih

“…1 the linear absorption spectra of isotope diluted ice Ih, which agree with previously measured spectra. 34 The OH stretch of ice Ih is more narrow and red-shifted compared to that of liquid water. The spectral narrowing reflects the much smaller variability of local structural motives around the OH or OD chromophore in the crystalline phase, despite the existence of proton disorder.…”

“…[24][25][26][27] Furthermore, the linear IR and Raman spectra of ice Ih have been investigated throughout the whole frequency range. [28][29][30][31][32][33][34] Nonlinear spectroscopic studies such as pump-probe, hole-burning, photon-echo or 2D IR spectroscopy, on the other hand, remained much more scarce. In particular, the nonlinear infrared spectroscopy of the OH stretch vibration (or correspondingly the OD stretch vibration) is of interest, since the local molecular environment directly affects its frequency, line shape and dynamics.…”

The accurate calculation of the band gap of liquid water by means of GW corrections applied to plane-wave density functional theory molecular dynamics simulations

“…5 The variations of OÁ Á ÁH ordering in the tetragonal coordination create dozens of ice phases, which at present are still under discussion. [5][6][7][8][9][10][11][12] Obviously, there is no long-range ordering in liquid water. However, at short-range the structure of water is topologically the same as those of ice, but with flexible bond-lengths and angles of H 2 O tetragons.…”