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Register a new userNon-monotonic zero point entropy in diluted spin ice
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Water ice and spin ice are important model systems in which theory can directly account for zero point entropy associated with quenched configurational disorder. Spin ice differs from water ice in the important respect that its fundamental constituents, the spins of the magnetic ions, can be removed through replacement with non-magnetic ions while keeping the lattice structure intact. In order to investigate the interplay of frustrated interactions and quenched disorder, we have performed systematic heat capacity measurements on spin ice materials which have been thus diluted up to 90%. Investigations of both Ho and Dy spin ices reveal that the zero point entropy depends non-monotonically on dilution and approaches the value of Rln2 in the limit of high dilution. The data are in good agreement with a generalization of Paulings theory for the entropy of ice.
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Spin ice materials, such as Dy2Ti2O7 and Ho2Ti2O7, have been the subject of much interest for over the past fifteen years. Their low temperature strongly correlated state can be mapped onto the proton disordered state of common water ice and, consequently, spin ices display the same low temperature residual Pauling entropy as water ice. Interestingly, it was found in a previous study [X. Ke {it et. al.} Phys. Rev. Lett. {bf 99}, 137203 (2007)] that, upon dilution of the magnetic rare-earth ions (Dy^{3+} and Ho^{3+}) by non-magnetic Yttrium (Y^{3+}) ions, the residual entropy depends {it non-monotonically} on the concentration of Y^{3+} ions. In the present work, we report results from Monte Carlo simulations of site-diluted microscopic dipolar spin ice models (DSIM) that account quantitatively for the experimental specific heat measurements, and thus also for the residual entropy, as a function of dilution, for both Dy2Ti2O7 and Ho2Ti2O7. The main features of the dilution physics displayed by the magnetic specific heat data are quantitatively captured by the diluted DSIM up to, and including, 85% of the magnetic ions diluted (x=1.7). The previously reported departures in the residual entropy between Dy2Ti2O7 versus Ho2Ti2O7, as well as with a site-dilution variant of Paulings approximation, are thus rationalized through the site-diluted DSIM. For 90% (x=1.8) and 95% (x=1.9) of the magnetic ions diluted, we find a significant discrepancy between the experimental and Monte Carlo specific heat results. We discuss some possible reasons for this disagreement.
Frustrated Ising magnets host exotic excitations, such as magnetic monopoles in spin ice. The ground state (GS) in this case is characterized by an extensive degeneracy and associated residual entropy going back to the pioneering work by G. Wannier who established large residual entropy of nearly 50%Rln2 per mole spins in a triangular Ising antiferromagnet (TIAF) already in 1950. Here, we endeavor to verify this result experimentally using TmMgGaO4, a novel rare-earth-based frustrated antiferromagnet with Ising spins arranged on a perfect triangular lattice. Contrary to theoretical expectations, we find almost no residual entropy and ascribe this result to the presence of a weak second-neighbor coupling J2zz ~ 0.09J1zz that lifts the GS degeneracy and gives rise to several ordered states, the stripe order, 1/3-plateau, and 1/2-plateau. TmMgGaO4 gives experimental access to these novel phases of Ising spins on the triangular lattice.
It is a salient experimental fact that a large fraction of candidate spin liquid materials freeze as the temperature is lowered. The question naturally arises whether such freezing is intrinsic to the spin liquid (disorder-free glassiness) or extrinsic, in the sense that a topological phase simply coexists with standard freezing of impurities. Here, we demonstrate a surprising third alternative, namely that freezing and topological liquidity are inseparably linked. The topological phase reacts to the introduction of disorder by generating degrees of freedom of a new type (along with interactions between them), which in turn undergo a freezing transition while the topological phase supporting them remains intact.
Determining the fate of the Pauling entropy in the classical spin ice material Dy$_2$Ti$_2$O$_7$ with respect to the third law of thermodynamics has become an important test case for understanding the existence and stability of ice-rule states in general. The standard model of spin ice - the dipolar spin ice model - predicts an ordering transition at $Tapprox 0.15$ K, but recent experiments by Pomaranski $et al.$ suggest an entropy recovery over long time scales at temperatures as high as $0.5$ K, much too high to be compatible with theory. Using neutron scattering and specific heat measurements at low temperatures and with long time scales ($0.35$ K$/10^6$ s and $0.5$ K$/10^5$ s respectively) on several isotopically enriched samples we find no evidence of a reduction of ice-rule correlations or spin entropy. High-resolution simulations of the neutron structure factor show that the spin correlations remain well described by the dipolar spin ice model at all temperatures. Further, by careful consideration of hyperfine contributions, we conclude that the original entropy measurements of Ramirez $et al.$ are, after all, essentially correct: the short-time relaxation method used in that study gives a reasonably accurate estimate of the equilibrium spin ice entropy due to a cancellation of contributions.
Fractionalised excitations that emerge from a many body system have revealed rich physics and concepts, from composite fermions in two-dimensional electron systems, revealed through the fractional quantum Hall effect, to spinons in antiferromagnetic chains and, more recently, fractionalisation of Dirac electrons in graphene and magnetic monopoles in spin ice. Even more surprising is the fragmentation of the degrees of freedom themselves, leading to coexisting and a priori independent ground states. This puzzling phenomenon was recently put forward in the context of spin ice, in which the magnetic moment field can fragment, resulting in a dual ground state consisting of a fluctuating spin liquid, a so-called Coulomb phase, on top of a magnetic monopole crystal. Here we show, by means of neutron scattering measurements, that such fragmentation occurs in the spin ice candidate Nd$_2$Zr$_2$O$_7$. We observe the spectacular coexistence of an antiferromagnetic order induced by the monopole crystallisation and a fluctuating state with ferromagnetic correlations. Experimentally, this fragmentation manifests itself via the superposition of magnetic Bragg peaks, characteristic of the ordered phase, and a pinch point pattern, characteristic of the Coulomb phase. These results highlight the relevance of the fragmentation concept to describe the physics of systems that are simultaneously ordered and fluctuating.
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