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Title: Supercooled spin liquid state in the frustrated pyrochlore Dy2Ti2O7

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
 [1];  [1];  [2];  [3];  [3];  [4];  [5]
  1. Cornell Univ., Ithaca, NY (United States)
  2. Cornell Univ., Ithaca, NY (United States); Stanford Univ., Palo Alto, CA (United States)
  3. McMaster Univ., Hamilton, ON (Canada)
  4. McMaster Univ., Hamilton, ON (Canada); Canadian Institute for Advanced Research, Toronto, ON (Canada)
  5. Cornell Univ., Ithaca, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States); Univ. of St. Andrews, Fife (United Kingdom)

A “supercooled” liquid develops when a fluid does not crystallize upon cooling below its ordering temperature. Instead, the microscopic relaxation times diverge so rapidly that, upon further cooling, equilibration eventually becomes impossible and glass formation occurs. Classic supercooled liquids exhibit specific identifiers including microscopic relaxation times diverging on a Vogel–Tammann–Fulcher (VTF) trajectory, a Havriliak–Negami (HN) form for the dielectric function ε(ω,T), and a general Kohlrausch–Williams–Watts (KWW) form for time-domain relaxation. Recently, the pyrochlore Dy2Ti2O7 has become of interest because its frustrated magnetic interactions may, in theory, lead to highly exotic magnetic fluids. However, its true magnetic state at low temperatures has proven very difficult to identify unambiguously. Here, we introduce high-precision, boundary-free magnetization transport techniques based upon toroidal geometries and gain an improved understanding of the time- and frequency-dependent magnetization dynamics of Dy2Ti2O7. We demonstrate a virtually universal HN form for the magnetic susceptibility χ(ω,T), a general KWW form for the real-time magnetic relaxation, and a divergence of the microscopic magnetic relaxation rates with the VTF trajectory. Low-temperature Dy2Ti2O7 therefore exhibits the characteristics of a supercooled magnetic liquid. Lastly, one implication is that this translationally invariant lattice of strongly correlated spins may be evolving toward an unprecedented magnetic glass state, perhaps due to many-body localization of spin.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
GBMF4544
OSTI ID:
1261641
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Vol. 112, Issue 28; ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 22 works
Citation information provided by
Web of Science

References (43)

Magnetocaloric study of spin relaxation in dipolar spin ice Dy 2 Ti 2 O 7 journal March 2007
High-dimensional fractionalization and spinon deconfinement in pyrochlore antiferromagnets journal March 2007
Thermal Relaxation and Heat Transport in the Spin Ice Material Dy2Ti2O7 journal February 2011
Spin Ice, Fractionalization, and Topological Order journal March 2012
Theorie des elektrischen Rückstandes in der Leidener Flasche journal January 1854
Scenario for delocalization in translation-invariant systems journal October 2014
Evidence of impurity and boundary effects on magnetic monopole dynamics in spin ice journal November 2012
Magnetic anisotropy of the spin-ice compound Dy2Ti2O7 journal January 2002
Creation and measurement of long-lived magnetic monopole currents in spin ice journal February 2011
Low-temperature spin freezing in the Dy 2 Ti 2 O 7 spin ice journal February 2004
Dynamics in many-body localized quantum systems without disorder journal May 2015
Spin Dynamics at Very Low Temperature in Spin Ice Dy 2 Ti 2 O 7 journal December 2011
Supercooled liquids for pedestrians journal June 2009
Relationship between the time-domain Kohlrausch-Williams-Watts and frequency-domain Havriliak-Negami relaxation functions journal October 1991
Nonexponential relaxations in strong and fragile glass formers journal September 1993
The frustration-based approach of supercooled liquids and the glass transition: a review and critical assessment journal December 2005
Supercooled Liquids and Glasses journal January 1996
A complex plane representation of dielectric and mechanical relaxation processes in some polymers journal January 1967
Spin Ice: Magnetic Excitations without Monopole Signatures Using Muon Spin Rotation journal November 2011
Spin liquids in frustrated magnets journal March 2010
Magnetic pyrochlore oxides journal January 2010
Electrostatic correlations: from plasma to biology journal September 2002
Dirac Strings and Magnetic Monopoles in the Spin Ice Dy2Ti2O7 journal September 2009
Dy 2 Ti 2 O 7 Spin Ice: A Test Case for Emergent Clusters in a Frustrated Magnet journal July 2008
Zero-point entropy in ‘spin ice’ journal May 1999
Monte Carlo studies of the dipolar spin ice model journal October 2004
Crystal-field interaction in the pyrochlore magnet Ho2Ti2O7 journal May 2000
Magnetic monopole dynamics in spin ice journal April 2011
Spin dynamics in the frozen state of the dipolar spin ice material Dy 2 Ti 2 O 7 journal January 2012
Debye-Hückel theory for spin ice at low temperature journal October 2011
Liquid-Gas Critical Behavior in a Frustrated Pyrochlore Ferromagnet journal November 1998
Introduction to Frustrated Magnetism book January 2011
Quantum spin ice: a search for gapless quantum spin liquids in pyrochlore magnets journal May 2014
Spin Ice State in Frustrated Magnetic Pyrochlore Materials journal November 2001
Signature of magnetic monopole and Dirac string dynamics in spin ice journal March 2009
AC Susceptibility of the Dipolar Spin Ice Dy 2 Ti 2 O 7 : Experiments and Monte Carlo Simulations journal October 2013
Heterogeneous freezing in a geometrically frustrated spin model without disorder: Spontaneous generation of two time scales journal July 2012
Brownian motion and quantum dynamics of magnetic monopoles in spin ice journal February 2013
Specific heat of Dy2Ti2O7 in magnetic fields: comparison between single-crystalline and polycrystalline data journal June 2002
Magnetic monopoles in spin ice journal January 2008
Results from an unbiased analysis of nearly 1000 sets of relaxation data journal September 1994
Absence of Pauling’s residual entropy in thermally equilibrated Dy2Ti2O7 journal April 2013
Many-Body Localization in Dipolar Systems journal December 2014

Cited By (6)

Magnetic monopole noise journal July 2019
Emergence of nontrivial magnetic excitations in a spin-liquid state of kagomé volborthite journal July 2016
Supercooling and fragile glassiness in a dipolar kagome Ising magnet text January 2018
Supercooling and fragile glassiness in a dipolar kagome Ising magnet journal October 2018
Supercooling and fragile glassiness in a dipolar kagome Ising magnet text January 2018
Magnetic Monopole Noise text January 2019

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