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Discovery of dynamical heterogeneity in a supercooled magnetic monopole fluid

Abstract:
Dynamical heterogeneity, in which transitory local fluctuations 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 fluids (Proc. Nat. Acad. Sci. 112, 8549 (2015)), we searched for such phenomena in Dy2Ti2O7. By measuring its microsecond-resolved spontaneous magnetization fluctuations M(t, T) we detected a sharp bifurcation in monopole noise characteristics below T≈1,500 mK, with the appearance of powerful spontaneous monopole current bursts. This intense dynamics emerges upon entering the supercooled monopole fluid regime, reaches maximum strength near T≈750 mK and then collapses along with coincident loss of ergodicity approaching Tg≈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). This overall phenomenology greatly expands our empirical knowledge of supercooled monopole fluids 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 vitrification studies.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1073/pnas.2528457123

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Role:
Author
ORCID:
0009-0002-5349-3446
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Institution:
University of Oxford
Role:
Author
ORCID:
0000-0001-8672-0233


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Funder identifier:
10.13039/501100000288
Grant:
R64897
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Funder identifier:
10.13039/501100000781
Grant:
DLV-788932
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Funder identifier:
10.13039/100000936
Grant:
GBMF9457
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Funder identifier:
10.13039/100014013
Grant:
EP/X025861/1


Publisher:
National Academy of Sciences
Journal:
Proceedings of the National Academy of Sciences More from this journal
Volume:
123
Issue:
23
Article number:
e2528457123
Publication date:
2026-06-05
Acceptance date:
2026-05-05
DOI:
EISSN:
1091-6490
ISSN:
0027-8424


Language:
English
Keywords:
Source identifiers:
4147662
Deposit date:
2026-06-05
ARK identifier:
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