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Communication: Probable scenario of the liquid–liquid phase transition of SnI4
6.The LLCP of water is supposed to be located below its homogeneous nucleation temperature, i.e., in a “no-man's land” (O. Mishima and H. E. Stanley, Nature (London) 396, 329 (1998)).
9.Compare the SFs shown in Fig. 2(a) with those in Fig. 2 of Ref. 1 obtained from measurements at 0.7, 1.8, and 3.2 GPa. The quality of the SF at the highest temperature is worse than those at other temperatures. This was caused by leakage of the liquid as a result of holding for a long time (more than a day), thereby reducing the intensities of the scattered x rays. This then reduced the amplitude of oscillation of the measured SF. However, the oscillation, whose period is determined by rSn-I, is still in phase with that of the MFF.
10.A subsidiary peak at ∼1 Å−1 in the SF of the reference LDL, observed by the angle-dispersive diffraction method (Ref. 8) could not be detected by the energy-dispersive diffraction method at low scattering angles because of appreciably large x-ray intensities scattered from the pressure-transmitting medium. A slight shift of the principal peak to a larger wavenumber with increasing pressure reflects an increase in the density.
11.We have already shown that the part of the SF with wavenumbers larger than ∼2.7 Å−1 can be well explained by the intramolecular correlation, see Ref. 1.
15.The positive value of the slope is not entirely virtual, but was based somewhat on the measurements performed by Hamaya et al. (unpublished work).
16.The set of values is one possible set; other sets are probably obtainable depending on the initial guesses for the parameters. In fact, it seems doubtful whether a critical phenomenon appears when the two models with a first-order transition are mixed. Hence, the individual values should not be taken seriously. However, they make sense when treated as pairs, such as in Eq. (1).
19.A one-order-of-magnitude reduction in the volume difference with increasing pressure is expected from the result of the MD simulation. See Figs. 3 and 4 in K. Fuchizaki, S. Sugiyama, and Y. Fujii, J. Chem. Phys. 112, 10379 (2000).
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We have shown from in situ synchrotron x-ray diffraction measurements that there are two thermodynamically stable liquid forms of SnI4, depending on the pressure. Based on the liquid–liquidcritical point scenario, our recent measurements suggest that the second critical point, if it exists, may be located in a region close to the point at which the melting curve of the crystalline phase abruptly breaks. This region is, unlike that of water, experimentally accessible with relative ease.
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