Letter abstract


Nature Physics 2, 249 - 253 (2006)
doi:10.1038/nphys270

Subject Categories: Condensed-matter physics | Materials physics | Chemical physics

Zero-point entropy in stuffed spin-ice

G. C. Lau1, R. S. Freitas2, B. G. Ueland2, B. D. Muegge1, E. L. Duncan1, P. Schiffer2 and R. J. Cava1

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The third law of thermodynamics dictates that the entropy of a system in thermal equilibrium goes to zero as its temperature approaches absolute zero. In ice, however, a 'zero point' or residual entropy can be measured—attributable to a high degeneracy in the energetically preferred positions of hydrogen ions associated with the so-called 'ice rules'1, 2. Remarkably, the spins in certain magnetic materials with the pyrochlore structure of corner-sharing tetrahedra, called 'spin ice', have an equivalent degeneracy of energetically preferred states, and also have a zero-point entropy3, 4, 5, 6, 7. Here, we chemically alter Ho2Ti2O7 spin ice by 'stuffing' extra Ho magnetic moments into otherwise non-magnetic Ti sites surrounding the Ho tetrahedra. The resulting series, Ho2(Ti2-xHox)O7-x/2, provides a unique opportunity to study the effects of increased connectivity between spins on a frustrated lattice. Surprisingly, the zero-point entropy per spin measured appears unchanged by these excess spins. The results suggest a chemical approach for studying ice-like frustration and other properties of the broad family of geometrically frustrated magnets based on the pyrochlore structure.

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  1. Department of Chemistry, Princeton University, Princeton, New Jersey 08544, USA
  2. Department of Physics and Materials Research Institute, Pennsylvania State University, University Park, Pennsylvania 16802, USA

Correspondence to: G. C. Lau1 e-mail: glau@princeton.edu

Correspondence to: P. Schiffer2 e-mail: schiffer@phys.psu.edu

Correspondence to: R. J. Cava1 e-mail: rcava@princeton.edu


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