Spin-liquid behavior in a classical Heisenberg kagom antiferromagnet

B. Fk, F.C. Coomer, A. Harrison, D. Visser, M.E. Zhitomirsky

(CEA Grenoble, ISIS, U. of Edinburgh)

An inelastic neutron scattering study of Deuteronium jarosite (D3O)Fe3(SO4)2(OD)6

UN

I VE R

IT

TH

O
F

Geometrical frustration
Antiferromagnetic NN interaction H = J Si.Sj , J>0 on a triangular lattice => frustration

Triangular (2D) (edge-sharing triangles)

Kagom (2D) (corner-sharing triangles)

Pyrochlore (3D) (corner-sharing tetrahedra)

Ideal kagom lattice

Roman mosaic, Empurias (c.a. -60)

Classical nearest-neighbor AF spins on a kagom lattice Strongly degenerate ground state No long-range order Co-planar states favored by thermal fluctuations S(Q) predicted by numerical simulations - but little is known about the dynamics, S()

Non-ideal kagom lattice

Additional interactions Vector chirality: Crystal anisotropy C = i,j Si x Sj Further neighbor interactions Dzyaloshinsky-Moriya interaction may lead to long-range order: k = 0 structure (left): uniform vector chirality k=(2/3,2/3) structure (3 x 3) (right): staggered vector chirality

Deuteronium jarosite (D3O)Fe3(SO4)2(OD)6

Well separated kagom layers of undistorted triangles Strong (NN) antiferromagnetic interactions (CW=-700 K) Small disorder (near full occupancy of Fe3+ ions) No long-range magnetic order (T>1 K) Wills EPL 42 (1998) 325 Gradual and partial spin freezing at Ts=13.8-17.5 K SR; Harrison PB 289-290 (2000) 217

IN16; D. Visser (unpubl.)

Has been classified as a topological spin glass

Unusual aging and memory effects Wills PRB 62 (2000) R9264 Specific heat ~T2 (rather than ~T) Wills EPL 42 (1998) 325

~50% of the moments are fluctuating: spin liquid !

Most other jarosites (replace H3O by K, ... or Fe by Cr, V,..) order at ~60 K with k=0 structure and doubling of unit cell along c (weak interlayer coupling)

Results from MARI

S(Q,E) = SN(Q,E) + SM(Q,E) Easy to subtract phonons Dynamic short-range correlations - characteristic of a spin liquid Non-dispersive S(Q,E)

Results from MARI

S(Q,E) = SN(Q,E) + SM(Q,E) Easy to subtract phonons Dynamic short-range correlations - characteristic of a spin liquid Non-dispersive S(Q,E)

Temperature dependence of S(Q)

Lines are Monte Carlo simulations:

Q-dependence

1.5

SM(Q)

1.0

0.5

0.0

2 Q (-1)

Q-dependence

10

(a) 1.5

SM(Q)

1.0

0.5

0.0

2 Q (-1)

Q-dependence

11

(b)

Fit <S0.Si>

Monte-Carlo simulation of NN AFM kagom

2 Q (-1)

The 3 x 3 structure has staggered vector chirality

Energy dependence

12

D3OFe3(SO4)2(OD)6

Continuum of gap-less excitations (gap<0.5 meV)

"(E) (mbarn/sr/meV)

150

T=14.5 K T=21 K T=36 K T=61 K T=121 K T=238 K

100

50

10 Energy (meV)

15

Quasielastic Lorentzian
8

13

0.4

(meV)
D3OFe3(SO4)2(OD)6 150 T=14.5 K T=21 K T=36 K T=61 K T=121 K T=238 K

'

"(E) (mbarn/sr/meV)

100

0 0
50

100 T (K)

200

0.0

(T) = 0 + T
0 5 10 Energy (meV) 15

/T scaling ? 2D AFM close to QCP (para -> LRO): expect /T scaling: "()T= F(/T) S. Sachdev, PRL 69 (1992) 2411 No /T scaling !
"T (K mbarn/SR/meV)

14

5000

D3OFe3(SO4)2(OD)6

2000 T=14.5 K T=21 K T=36 K T=61 K T=121 K T=238 K

1000

(T) = 0 + T

500

200

0.01

0.1 /T (meV/K)

Non-Lorentzian response
Deviations from a single Lorentzian at low energy

15

D3OFe3(SO4)2(OD)6 200 T=14.5 K T=21 K T=36 K T=61 K T=121 K T=238 K

"(E) (mbarn/sr/meV)

14.5 150 21 36

100

61

50 121 238 0 0 5 10 Energy (meV) 15

Scaling ?
2D AFM close to QCP (para -> spin-glass): expect "() ~ S. Sachdev, PRL 69 (1992) 2411 with D OFe (SO ) (OD) -1<<0
3 3 4 2

16

200

Here: =-0.68

"(E) (mbarn/sr/meV)

150

100

50

10 Energy (meV)

15

SCGO(x) = SrCr8-xGa4+xO19
Spin glass behavior in a pyrochlore slab [coupled (partially occupied) kagom planes]

17

C. Broholm, PRL 65 (1990) 3173

KCr3(SO4)2(OD)6
S=3/2, 76% site occupancy orders at 1.6 K shows gap-less spin fluctuations

18

S.-H. Lee, PRB 56 (1997) 8091

Y0.5Ca0.5BaCo4O7
CW=-2200 K Co2+ (S=3/2) forms kagom layers Co3+ (S=0) occupy interlayer sites

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Valence disorder?

S(Q) indicates staggered chirality

S(Q,E) from temperature difference 150-40 K

W. Schweika, PRL 98 (2007) 067201

ZnCu3Cl2(OH)6 Herbertsmithite or paratacamite

S=1/2 kagom with 90% occupancy and no gap (!)

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"() ~ 0.7

J.S. Helton, PRL 98 (2007) 107204

ZnxCu4-xCl2(OH)6
x<0.66 orders in distorted kagom (S=1/2) with sharp excitations x>0.66 diluted kagom (<90% occupancy) with broad excitations

21

See also: Mark A. de Vries, Poster Session

S.-H. Lee, Nat. Mat. 4 (2005) 323

Conclusions
Inelastic neutron scattering measurements on the classical Heisenberg kagom antiferromagnet (D3O)Fe3(SO4)2(OD)6 show clear spin-liquid behavior: dynamic short-range correlations S(Q) very similar to Monte-Carlo simulations of the NN AFM kagom 3 x 3 type correlations indirect evidence of staggered vector chirality "(E) continuum of (probably) gapless excitations (gap < 0.5 meV) that extends out to 20 meV single-Lorentzian component with (T)=1.5+aT meV and additional contributions (multiple time scales) or a non-Lorentzian line shape ("() ~ 0.68) no dynamic scaling behavior

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Key experimental features

These results were made possible because of Excellent deuteration (H/D<5%) High incoming energy Allows phonon subtraction (polarized neutrons not needed) Sufficient energy range Analysis of energy transfer Separate elastic from inelastic scattering Energy integration performed at constant Q To go further: need single crystal

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B. Fk et al, EPL 81 (2008) 17006