The phase diagram of ice: a quasi-harmonic study based on a flexible water model

The phase diagram of ice is studied by a quasi-harmonic approximation. The free energy of all experimentally known ice phases has been calculated with the flexible q-TIP4P/F model of water. The only exception is the high pressure ice X, in which the presence of symmetric O-H-O bonds prevents its modeling with this empirical interatomic potential. The simplicity of our approach allows us to study ice phases at state points of the T-P plane that have been omitted in previous simulations using free energy methods based on thermodynamic integration. The effect in the phase diagram of averaging the proton disorder that appears in several ice phases has been studied. It is found particularly relevant for ice III, at least for cell sizes typically used in phase coexistence simulations. New insight into the capability of the employed water model to describe the coexistence of ice phases is presented. We find that the H-ordered ices IX and XIV, as well as the H-disordered ice XII, are particularly stable for this water model. This fact disagrees with experimental data. The unexpected large stability of ice IX is a property related to the TIP4P-character of the water model. Only after omission of these three stable ice phases, the calculated phase diagram becomes in reasonable qualitative agreement to the experimental one in the T-P region corresponding to ice Ih, II, III, V, and VI. The calculation of the phase diagram in the quantum and classical limits shows that the most important quantum effect is the stabilization of ice II due to its lower zero-point energy when compared to that one of ices Ih, III, and V.Comment: 13 pages, 8 figures, 5 table

Magnetic susceptibility of diluted pyrochlore and SCGO antiferromagnets

We investigate the magnetic susceptibility of the classical Heisenberg antiferromagnet with nearest-neighbour interactions on the geometrically frustrated pyrochlore lattice, for a pure system and in the presence of dilution with nonmagnetic ions. Using the fact that the correlation length in this system for small dilution is always short, we obtain an approximate but accurate expression for the magnetic susceptibility at all temperatures. We extend this theory to the compound SrCr_{9-9x}Ga_{3+9x}O_{19} (SCGO) and provide an explanation of the phenomenological model recently proposed by Schiffer and Daruka [Phys. Rev. B56, 13712 (1997)].Comment: 4 pages, Latex, 4 postscript figures automatically include

Ising pyrochlore magnets: Low temperature properties, ice rules and beyond

Pyrochlore magnets are candidates for spin-ice behavior. We present theoretical simulations of relevance for the pyrochlore family R2Ti2O7 (R= rare earth) supported by magnetothermal measurements on selected systems. By considering long ranged dipole-dipole as well as short-ranged superexchange interactions we get three distinct behaviours: (i) an ordered doubly degenerate state, (ii) a highly disordered state with a broad transition to paramagnetism, (iii) a partially ordered state with a sharp transition to paramagnetism. Thus these competing interactions can induce behaviour very different from conventional ``spin ice''. Closely corresponding behaviour is seen in the real compounds---in particular Ho2Ti2O7 corresponds to case (iii) which has not been discussed before, rather than (ii) as suggested earlier.Comment: 5 pages revtex, 4 figures; some revisions, additional data, additional co-authors and a changed title. Basic ideas of paper remain the same but those who downloaded the original version are requested to get this more complete versio

Thermodynamic Study of Excitations in a 3D Spin Liquid

In order to characterize thermal excitations in a frustrated spin liquid, we have examined the magnetothermodynamics of a model geometrically frustrated magnet. Our data demonstrate a crossover in the nature of the spin excitations between the spin liquid phase and the high-temperature paramagnetic state. The temperature dependence of both the specific heat and magnetization in the spin liquid phase can be fit within a simple model which assumes that the spin excitations have a gapped quadratic dispersion relation.Comment: 5 figure