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Philippe Mendels Laboratoire de Physique des Solides, Universit Paris-Sud, Orsay, France
F. Bert
A. Olariu
A. Zorko
- J. C. Trombe, F. Duc, CEMES, Toulouse, P. Strobel, Grenoble , France - M. de Vries, G. Nilsen, A. Harrison, Edinburgh, UK - S. Nakamae, F. Ladieu, D. LHote, P. Bonville, CEA Saclay, France
Querelles
r r H = J ij S i .S j , J ij < 0
Introduction
0 200 400
T
1/
600
800
-200
200
T
400
600
800
Class.
C A B
r r r r S A + S B + SC = 0
RVB =
Introduction
C A
...
...
...
...
Macroscopic degeneracy
Soft modes
Exact diagonalizations
S=0 1
S=0
Fundamental spin liquid Nel RVB ? Mila, PRL 81, 2356 (2000)
Introduction
- Heisenberg spins - S=1/2 (quantum spins) - Corner sharing geometry: Kagom (2D) or pyrochlore (3D) lattice - No perturbation (anisotropy, dipolar interaction, n.n. interactions, dilution) - For kagom: stacking should keep the 2D kagom planes uncoupled
Kagom bilayers
(Cr3+,
S =3/2)
Materials
~6.4
Exotic spin glass at only low T High frustration ratio /Tg Fluctuations at low T Short correlation length Field independant Cv >3% spinless defects
2.0
~1/a
(s )
T=70 mK
1.5
Spin glass
-1
1.0
0.5
0.0
T (K)
Jarosite Family
AB3(SO4)2(OH)6 A= Na+, K+, Ag+, Rb+, H3O+, NH4+, Pb2+, Ba2+ B = Fe3+ (S=5/2), Cr3+ (S=3/2), V3+ (S=1)
Volborthite, Cu3V2O7(OH)22H2O
Tg (K)
Cu Zn
OH Cl
Herbertsmithite is the first example of a quantum kagome antiferromagnet perfect kagom lattice no freezing at least down to J/4000 -> renewal ofthe search for scenarios for the kagome ground state
VBC : R.R.P. Singh and D.A. Huse, PRB (2007, 2008) Dirac spin liquid : Y. Ran et al, PRL (2007), PRB (2008) ....
Cu ZnxCu1-x
Cu III Cu II Cu I Cu I Cu I
Zn/Cu II Cu I Cu I Cu I
Zn Cu I Cu I
Clinoatacamite Cu2(OH)3Cl
Zn-paratacamite ZnxCu4-x(OH)6Cl2
ZnxCu4-x(OH)6Cl2
Curie Weiss behavior for all x -> antiferromagnetic correlations
J (AF,F?) J (AF)
J : in-plane coupling AF ~ 175 K J: inter-plane coupling small, maybe Ferro 97 no transition for T<<J -> highly frustrated antiferromagnets 119
P. Shores et al, JACS (2005)
ZnxCu4-x(OH)6Cl2
0.016 0.014
(cm3/mol Cu)
0.012 0.010 0.008 0.006 0.004 0.002 0 50 100 150 200 250 300
x=1
Herbersmithite x=1 -No sign of transition for T>2K -Low T Curie like upturn for T<50K
temperature (K)
+
S=1/2
chantillon
SR : ZnCu3(OH)6Cl2 , x=1
1.0
0.8
Polarisation
0.6
At 50mK, no sign of ordering relaxation arises from small static nuclear fields. upper limit of a frozen moment for Cu2+, if any : 6x10-4 B
0.4
0.2
H
0.0
50 mK
0 5 10
time ( s)
Also: ac- Helton et al, PRL 98 107204 (2007) SR O. Ofer et al, cond-mat/0610540
x = 0.66
0.6
x = 0.33
0.3
T=1.5K, Zero Field
x = 0.15 x=0
When x increases from 0 to 1 : -Oscillations are smeared out -A paramagnetic (x=1 type) component emerges at the expense of the frozen one
Polarization
0.0
0.3
0.6
time (s)
Large domain of stability 0.66<x<1 of a dynamical ground state -> surprisingly small influence of interlayer coupling
P. Mendels et al, PRL 98, 077204 (2007)
-> need for additional terms to the KAF Hamiltonian to account for Herbertsmithite macroscopic susceptibility
0.0030 0.0025
i H
M/Msat (%)
(cm3/mol Cu)
Mdefect~Brillouin(H/T)
-~7% of interlayer Cu2+ - i << macro at low T
50
100
150
200
250
1.7 K
2 0
10
12
14
H (T)
Dzyaloshinskii-Moriya interactions
D Si Sj
HDM=D.(SiSj)
Broad room T ESR line <- magnetic anisotropy from DM |Dz|=0.08J, |Dp|~0.01J
Dzyaloshinskii-Moriya interactions
For classical spins, DM stabilizes ordered phases (cf jarosites)
M. Elhajal et al, PRB 66, 014422 (2002)
NMR: principles
K
r r H = HZ + A I . S
-5 -4 -3 -2 -1 0
17O
17O:
Zn Cu Cl
1.0
ref
300 K
0.5
150 K 200 K 250 K
0.0 6.4
300 K
6.6
6.8
6.70
Zn
Cu Zn Cu
O
H
17O 17O
Cu
175 K
0.5
= 55
0.0 6.4
6.5
6.6
6.7
6.8
6.9
6.5
6.6
6.7
6.8
6.9
7.0
H(Tesla)
20
1.3 K 0.47 K
O lineshift (%)
10
10 K 15 K 20 K 30 K
17
5K
100 T (K)
200
300
M D
40 K 50 K 60 K 85 K 175 K
-Susceptibility decreases below 50 K -> enhancement of short range correlations -> new energy scale
6.4
6.5
6.9
7.0
10
(1/T1) (ms )
1 T1 (ms )
-1
-1
35
63
0.1 0
63Cu
O Cu 35 Cl
63
17
-1
17
-1
T1 ~ T
0.1 0 1 T (K )
-1 -1
-1
0.7+/-0.1
15
30 45 Temperature (K)
60
0.1
and
35Cl
() 0.7(3)
Helton et al, PRL 98 107204 (2007)
Exact Diagonalization
Lecheminant, PRB 56, 2521 (1997) Waldtmann et al., EPJB 2, 501 (1998).
<J/20 gap between singlet ground state and 1st triplet state if any...
Defect line
rfrence
1.5
1.3 K 0.47 K
O Cu
1.0
Cu Zn O
O Zn Cu
5K 10 K 15 K 20 K 30 K
0.5
0.0
100
200 T (K)
300
M D
40 K 50 K 60 K 85 K 175 K
6.4
6.5
6.9
7.0
Dommange et al., PRB 68, 224416 (2003); Lauchli et al. Phys. Rev. B 76, 144413 (2007)
-Dimers next to the impurity survive up to D~J -DM interaction removes the singlet nature of the ground state
Conclusions on Herbertsmithite
- first S=1/2 antiferromagnet with perfect kagome lattice (3 fold symmetry) - no order or frozen disorder down to 50mK despite J=175K and perturbations
Quantum spins on a perfect kagome lattice -> allows close comparison with theory -> renewed interest in understanding the GS
VBC : R.R.P. Singh and D.A. Huse, PRB (2007, 2008) Dirac spin liquid : Y. Ran et al, PRL (2007), PRB (2008) ....
- magnetic defects (rather complex, in plane and out of plane) which impact the low T thermodynamic measurements -> local probe techniques -> second sample generation : controlled (or no) defects - sizeable DM interaction : D/J~0.1: probe criticality: on-going - Local susceptiblity determined from 17O NMR: ground state appears to be gap-less with a finite susceptibility intrinsic to Heisenberg kagome model or DM interaction closes the gap ? (no field effect)
Kagome
Volborthite, CEMES, Toulouse
Bert et al, PRL 2005
Triangular
Cr,
Pyrochlore
Tb2Sn2O7 LLB, Saclay
Bert et al, PRL 2006
Thank you!