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GEOMETRICALLY FRUSTRATED MAGNETS John Chalker Physics Department, Oxford University
33

GEOMETRICALLY FRUSTRATED MAGNETS

Feb 02, 2022

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Page 1: GEOMETRICALLY FRUSTRATED MAGNETS

GEOMETRICALLY FRUSTRATED MAGNETS

John Chalker

Physics Department, Oxford University

Page 2: GEOMETRICALLY FRUSTRATED MAGNETS

Outline

How are geometrically frustrated magnets special?

What they are not

Evading long range order

Degeneracy and fluctuations - models and experiment

Statistical physics of underconstrained systems

Emergent degrees of freedom and classical fractionalizati on

Page 3: GEOMETRICALLY FRUSTRATED MAGNETS

Condensed matter at low temperature

Symmetry breaking as the norm

Crystalline solids

Page 4: GEOMETRICALLY FRUSTRATED MAGNETS

Broken symmetry in Bose liquids

Quantum fluctuations suppress crystalisation

4He phase diagram

Page 5: GEOMETRICALLY FRUSTRATED MAGNETS

Ordering in ferromagnets

High temperature

Ground state

Susceptibility

c

T

χ

T

Page 6: GEOMETRICALLY FRUSTRATED MAGNETS

Unfrustrated antiferromagnetic order

Neel order

Inverse susceptibility

N

T

χ

θ T

−1

CW

Neutron diffraction

Shull and Smart (1949)

Page 7: GEOMETRICALLY FRUSTRATED MAGNETS

Alternative to symmetry breaking # 1

. . . a unique ground state

In the Fermi gas

low T

n(p)

phigh T

Momentum distribution

Page 8: GEOMETRICALLY FRUSTRATED MAGNETS

Spin system with unique ground state

J

Weakly coupled singlet pairsχ vs T

SrCu2(BO3)2

Page 9: GEOMETRICALLY FRUSTRATED MAGNETS

Alternative to symmetry breaking # 2

. . . strong fluctuations

Frustration and degeneracy

?

Anderson 1956, Villain 1979

Page 10: GEOMETRICALLY FRUSTRATED MAGNETS

Antiferromagnetic spin clusters- frustration and degeneracy

Ising triangle

?

Heisenberg tetrahedron

34

1 2

Ground states: cluster spin L ≡∑

i Si minimised

H = J∑

pairs

Si · Sj ≡J

2|L|2 + c

Page 11: GEOMETRICALLY FRUSTRATED MAGNETS

Examples of frustrated lattices

Building block: corner-sharing frustrated units

2D: kagome lattice 3D: pyrochlore lattice

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Page 12: GEOMETRICALLY FRUSTRATED MAGNETS

Frustrated lattices beyond physics . . .

Page 13: GEOMETRICALLY FRUSTRATED MAGNETS

Characteristics of frustrated magnets

SrGa12−xCrxO19 (SCGO) as an example

Paramagnetic even for T ≪ |ΘCW|

χ−1 vs TMartinez et al, PRB 46, 10786 (1992)

Strong short-range correlations

Elastic neutron scatteringS.H. Lee et al, Europhys Lett 35, 127 (1996)

Page 14: GEOMETRICALLY FRUSTRATED MAGNETS

Selected examples of frustrated magnets

Layered materials

SCGO

pyrochlore slabs

Cr3+ S = 3/2

ΘCW ∼ 500K TF ∼ 4K

hydromium iron jarosite

kagome layers

Fe3+ S = 5/2

ΘCW ∼ 700K TF ∼ 14K

Herbertsmithite

kagome layers

Cu2+ S = 1/2

ΘCW ∼ 300K

Pyrochlore antiferromagnets

Y2Mo2O7

Mo4+ S = 1

ΘCW ∼ 200K TF ∼ 22K

Cs Ni Cr F 6

Ni2+ S = 1 Cr3+ S = 3/2

ΘCW ∼ 70K TF ∼ 2.3K

Spin ice materials

Dy2Ti2O7 and Ho 2Ti2O7

ferromagnets with single-ion anisotropy— hence frustration

Jeff ∼ 1K − 2K

Page 15: GEOMETRICALLY FRUSTRATED MAGNETS

Ground state degeneracy in classicalHeisenberg models

Maxwellian constraint-counting

Page 16: GEOMETRICALLY FRUSTRATED MAGNETS

Ground state degeneracy inHeisenberg pyrochlore AFM

H = J∑

bonds

Si · Sj ≡J

2

units

|Lα|2 + c

Total number of degrees of freedom: F = 2 × (number of spins)

Constraints satisfied in ground state: K = 3 × (number of units)

Ground state dimension:

D=F-K

Geometric Frustration → Macroscopic D

Page 17: GEOMETRICALLY FRUSTRATED MAGNETS

Schematics of behaviour at low temperature

Classical cooperative paramagnet: JS ≪ kBT ≪ JS2

������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������

������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������������

Ground statemanifold

Accessible states at low T

Phase space

Page 18: GEOMETRICALLY FRUSTRATED MAGNETS

Ground state selection by fluctuations?‘Order by disorder’ Villain (1980), Shender (1982)

Some states have soft modes

δθ δθ

E = J2|L|2 ∝ (δθ)4

Others don’t

δθ δθ

E = J2|L|2 ∝ (δθ)2

Page 19: GEOMETRICALLY FRUSTRATED MAGNETS

Ground state selection?

Thermal fluctuations

Probability distribution onground states

xy

dy e−ωy2/kBT ∝

kBT

ω

P (x) ∝∏

l

(

kBT

ωl(x)

)

Thermal fluctuations

kagome → coplanar

pyrochlore → disordered

Page 20: GEOMETRICALLY FRUSTRATED MAGNETS

Dynamics of Heisenberg systemsHow does system explore ground state manifold?

Equation of motion: ~dSi

dt = Si × Hi = −JSi ×∑

j Sj

Harmonic approximation

ρ(ω)

ω

zero modes

spinwaves

Normal mode frequencies ω

Anharmonic interactions

Brownianmotion betweengroundstates

finite spinwave lifetime

randomfluctuations

in H i

Langevin: dS/dt(0) = S × h(t)

〈S(0) · S(t)〉 ≈ exp(−ckBTt/~)

Page 21: GEOMETRICALLY FRUSTRATED MAGNETS

Quasielastic neutron scattering in Y 2Ru2O7

Scattering vs Q & ω

ΘCW = −1100K

TN = 77K

Linewidth vs temperature

~Γ = CkBT

C = 1.17

van Dujin et al (2008)

Page 22: GEOMETRICALLY FRUSTRATED MAGNETS

Frustration and residual entropy

Spin ice

Anisotropy +

ferromagnetic exchange

Water ice

Pauling 1935

Ground states: ‘two-in, two-out’

Page 23: GEOMETRICALLY FRUSTRATED MAGNETS

Pauling’s entropy estimate

One tetrahedron

Total number of states: 16

Fraction that are ground states: 616

Pyrochlore lattice

Estimate for number of ground states:

(total # states) ×(

616

)(# tetrahedra)=

(

32

)(# spins/2)

Page 24: GEOMETRICALLY FRUSTRATED MAGNETS

Pauling entropy in experiment

Dy2Ti2O7, Ramirez et al, Nature 399, 333 (1999).

Page 25: GEOMETRICALLY FRUSTRATED MAGNETS

Correlations induced by ground stateconstraints

Local constraints

tet Si = 0

Long range correlations

Sharp structure in〈S−q · Sq〉

Page 26: GEOMETRICALLY FRUSTRATED MAGNETS

Gauge theory of ground state correlationsYoungblood et al (1980), Huse et al (2003), Henley (2004)

Map spin configurations . . .

‘two-in two out’ groundstates . . .

. . . to vector fields B(r)

. . . map to divergenceless B(r)

Page 27: GEOMETRICALLY FRUSTRATED MAGNETS

Ground states as flux loops

Entropic distribution: P [B(r)] ∝ exp(−κ∫

B2(r)d3r)

Power-law correlations: 〈Bi(r)Bj(0)〉 ∝ r−3

Page 28: GEOMETRICALLY FRUSTRATED MAGNETS

Low T correlations from neutron diffractionBramwell and Harris, unpublished

Ho2Ti2O7

Page 29: GEOMETRICALLY FRUSTRATED MAGNETS

Classical fractionalised excitations

Fractionalisation in one dimension

Ground state

An excited state

. . . two separated excitations

Page 30: GEOMETRICALLY FRUSTRATED MAGNETS

Fractionalisation in spin ice

Monopole excitations

Ground state

Castelnovo, Moessner and Sondhi (2008)

Excited states

−+

+−

Page 31: GEOMETRICALLY FRUSTRATED MAGNETS

Candidate quantum Spin Liquids

κ-(ET)2Cu2(CN)3

Interaction scale J ∼ 250K

No order to T = 30mK

Herbertsmithite

ZnCu3(OH)6Cl2

Interaction scale J ∼ 200K

No order to T = 50mK

K

J

Page 32: GEOMETRICALLY FRUSTRATED MAGNETS

Metallic characteristics in an insulator

κ-(ET)2Cu2(CN)3

Interaction scale J ∼ 250K

No order to T = 30mK

Finite low- T susceptibility Heat capacity ∼ aT + bT 3

Page 33: GEOMETRICALLY FRUSTRATED MAGNETS

Summary

Geometric frustration

macroscopic classical degeneracies

long-range order avoided

Frustrated magnets at low T

soft modes and slow dynamics

emergent degrees of freedom

exotic excitations

CollaboratorsM. J. Bhaseen

R. Coldea

P. Conlon

J. F. G. Eastham

P.C.W. Holdsworth

L. D. C. Jaubert

R. Moessner

T. S. Pickles

T. E. Saunders

E. F. Shender

S. E. Palmer

S. Powell

M. Y. Veillette