Discovery of dynamical heterogeneity in a supercooled magnetic monopole fluid

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dc.contributor.authorDasini, Jahnatta
dc.contributor.authorCarroll, Chaia
dc.contributor.authorMurphy, Jack
dc.contributor.authorDawson, Catherine
dc.contributor.authorTakahashi, Hiroto
dc.contributor.authorSharma, Sudarshan
dc.contributor.authorJerzembeck, Fabian
dc.contributor.authorBlundell, Stephen J.
dc.contributor.authorLuke, Graeme M.
dc.contributor.authorDavis, J. C.Séamus
dc.contributor.authorWard, Jonathan
dc.contributor.funderTaighde Éireann - Research Ireland
dc.contributor.funderHorizon Europe
dc.contributor.funderGordon and Betty Moore Foundation
dc.contributor.funderEuropean Research Council
dc.contributor.funderUK Royal Society-Newton Advanced Fellowship
dc.date.accessioned2026-09-14T13:15:01Z
dc.date.available2026-09-14T13:15:01Z
dc.date.issued2026-06-05
dc.description.abstractDynamical heterogeneity, in which transitory local fuctuations occur in the conformation and dynamics of constituent particles, is widely hypothesized to be essential to the evolution of supercooled liquids into the structural glass state. Yet its microscopic spatiotemporal phenomenology is challenging to detect directly in molecular glass forming liquids. Because recent theoretical advances predict that corresponding dynamical heterogeneity could occur in supercooled magnetic monopole fuids (Proc. Nat. Acad. Sci. 112, 8549 (2015)), we searched for such phenomena in Dy2Ti2O7. By measuring its microsecond-resolved spontaneous magnetization fuctuations M(t, T ) we detected a sharp bifurcation in monopole noise characteristics below ≈ 1,500 mK, with the appearance of powerful spontaneous monopole current bursts. Tis intense dynamics emerges upon entering the supercooled monopole fuid regime, reaches maximum strength near ≈ 750 mK and then collapses along with coincident loss of ergodicity approaching g ≈ 250 mK. Moreover, when the four-point dynamical susceptibility χ4(τ, T )is determined directly from temperature dependence of correlations in M(t, T ), it evolves as predicted when dynamical heterogeneity is present, revealing its simultaneously and rapidly escalating length and time scales, ξ(T ) and τ4(T ). Tis overall phenomenology greatly expands our empirical knowledge of supercooled monopole fuids and, more generally, demonstrates techniques for detection of the time sequence, magnitude, statistics, and correlations of dynamical heterogeneity, access to which may greatly accelerate fundamental vitrifcation studies.en
dc.description.sponsorshipTaighde Éireann - Research Ireland|17/RP/5445
dc.description.sponsorshipTaighde Éireann - Research Ireland|25/RP-2TF/13559
dc.description.sponsorshipTaighde Éireann - Research Ireland|GOIPG/2023/4014
dc.description.sponsorshipHorizon Europe EP/X025861/1
dc.description.sponsorshipGordon and Betty Moore Foundation|GBMF9457
dc.description.sponsorshipEuropean Research Council|DLV-788932
dc.description.sponsorshipUK Royal Society|R64897
dc.description.sponsorshipUK Royal Society|RSRP\R25\1002
dc.description.versionPublished Version
dc.format.extent8
dc.format.mimetypeapplication/pdfen
dc.identifier.articleide2528457123
dc.identifier.authororcidDasini, Jahnatta
dc.identifier.authororcidCarroll, Chaia
dc.identifier.authororcidMurphy, Jack
dc.identifier.authororcidDawson, Catherine§0009-0002-5349-3446
dc.identifier.authororcidTakahashi, Hiroto
dc.identifier.authororcidSharma, Sudarshan
dc.identifier.authororcidJerzembeck, Fabian
dc.identifier.authororcidBlundell, Stephen J.
dc.identifier.authororcidLuke, Graeme M.
dc.identifier.authororcidDavis, J. C.Séamus
dc.identifier.authororcidWard, Jonathan
dc.identifier.citationDasini, J, Carroll, C, Murphy, J, Dawson, C, Takahashi, H, Sharma, S, Jerzembeck, F, Blundell, S J, Luke, G M, Davis, J C S & Ward, J 2026, 'Discovery of dynamical heterogeneity in a supercooled magnetic monopole fluid', Proceedings of the National Academy of Sciences of the United States of America, vol. 123, no. 23, e2528457123, pp. 1-8. https://doi.org/10.1073/pnas.2528457123
dc.identifier.doi10.1073/pnas.2528457123
dc.identifier.endpage8
dc.identifier.issn0027-8424
dc.identifier.issued23
dc.identifier.journaltitleProceedings of the National Academy of Sciences of the United States of America
dc.identifier.otherORCID: /0009-0002-5349-3446/work/226728552
dc.identifier.startpage1
dc.identifier.urihttps://hdl.handle.net/10468/19245
dc.identifier.volume123
dc.language.isoen
dc.publisherNational Academy of Sciences
dc.relation.urihttps://www.scopus.com/pages/publications/105041251839
dc.rights© 2026, the Author(s). Published by PNAS. This open access article is distributed under Creative Commons Attribution License 4.0 (CC BY)
dc.rights.accessrightsopen access
dc.rights.licensenameAttribution 4.0 International
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/
dc.statusPeer reviewed
dc.subjectDynamical heterogeneity
dc.subjectEmergent magnetic monopoles
dc.subjectSpin-ice
dc.subjectSupercooled liquids
dc.subjectVitrification
dc.subject[Physics]
dc.titleDiscovery of dynamical heterogeneity in a supercooled magnetic monopole fluiden
dc.typeArticle (peer-reviewed)
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