Composite Spin in Fluctuating Magnets

Collin Broholm
*
Johns Hopkins University and NIST Center for Neutron Research
* Supported by the National Science Foundation
M. Azuma
R. Bewley
W. J. L. Buyers
Ying Chen
S.-W. Cheong
G. Gasparovic
Guangyong Xu
G. Aeppli
J. F. DiTusa
D. V. Ferraris
W. Ratcliff II
D. H. Reich
J. Rittner
M. B. Stone
H. Takagi
M. Takano
M. E. Bisher
M. M. J. Treacy
R. Paul
H. Yardimci
C. D. Frost
Q. Huang
S. Ishiwata
T. Ito
T. H. Kim
T. Lectka
S.-H. Lee
K. Oka
T. G. Perring
Y. Qiu
Kent State 4/17/03
Outline
1. Introduction
a. Magnets, ordered and fluctuating
b. How to distinguish using neutrons
2. Whirlwind tour of fluctuating magnets
a. Spin trimer magnetism in La
4
Cu
3
MoO
12
b. Cooperative singlet in spin-1 chain
c. Frustrated spin liquid in organic magnet
d. Fluctuating spin directors in spinel oxide
3. Summary and Current Frontiers
Kent State 4/17/03
Filled shells non-magnetic
materials
Ti V Cr Mn Fe Co Ni Cu
Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm
U Np Pu Am Cm
Partially filled shell in solid:
Un-filled shells magnetic materials
Kent State 4/17/03
Magnetization of Solid with unfilled Shells
Susceptibility data for
paramagnetic salt

=
j
j B
g S H Q H
H S M G
Q
| =

j
j
B
V
g
)
T k
S S g
B
B
3
) 1 (
2

=
Q
H
M

Spin susceptibility diverges as T 0 Spin susceptibility diverges as T 0

FeBr(C
44
H
28
N
4
)
Dilute Fe in organic matrix
FeBr(C
44
H
28
N
4
)
Dilute Fe in organic matrix
Kent State 4/17/03
S=1/2
S=1/2
S=1/2
Coulomb + Pauli = Heisenberg
Coulomb interactions plus Pauli principle split 4-fold spin degeneracy
j i
J S S = H
The level scheme is reproduced by Heisenberg Exchange Hamiltonian
|J|
1 =
tot
S
0 =
tot
S
S=1/2
|J|
0 =
tot
S
1 =
tot
S
Singlet gnd. State: J > 0
Triplet gnd. State: J < 0
Kent State 4/17/03
Interactions orient moments
G
1
G
Ferromagnetic EuO Ferromagnetic EuO
G
1
G
Antiferromagnetic KNiF
3
Antiferromagnetic KNiF
3
CW N
T 5 }
?
Kent State 4/17/03
A brief story of Antiferromangetism
1970 Nobel Prize in Physics to
Hannes Alfvn and Louis Nel
L. Nel From Nobel lecture (1970).
L. Nel 1904-2000
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Staggered magnetization or QM singlet
1962 Nobel Prize in Physics
)
1
2
T+ +T
L. D. Landau from Phys. Zs. UdSSR (1933).
L. D. Landau 1908-1968
Kent State 4/17/03
Is Nels state possible?
C. G. Shull 1915-2001
1994 Nobel Prize in Physics to
B. N. Brockhouse and C. G. Shull
Kent State 4/17/03
Magnetic Neutron Diffraction
f
k
i f
= Q k k
Reciprocal Space
i
k
Real space
Nuclear Diffraction: * * * h k l = Q a b c Magnetic Diffraction: * * *
m m m
h k l = Q a b c
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Experimental Evidence for Nel order
1994 Nobel Prize in Physics to
B. N. Brockhouse and C. G. Shull
C. G. Shull 1915-2001
Kent State 4/17/03
Is Landaus vision of a AFM possible?
Kent State 4/17/03
Outline
1. Introduction
a. Magnets, ordered and fluctuating
b. How to distinguish using neutrons
2. Whirlwind tour of fluctuating magnets
a. Spin trimer magnetism in La
4
Cu
3
MoO
12
b. Cooperative singlet in spin-1 chain
c. Frustrated spin liquid in organic magnet
d. Fluctuating spin directors in spinel oxide
3. Summary and Current Frontiers
(Azuma et. al., PRB 62 R3588)
z=3/4 CuMoO plane
La
4
Cu
3
MoO
12
: A lattice of spin-1/2 trimers
Magnetic susceptibility Magnetic susceptibility
Kent State 4/17/03
Frustrated quantum spin triangles
)
1 3 3 2 2 1
S S S S S S = J H
J
J J
J
2
3
J
2
3
1 3 3 3 2 2 2 1 1
S S S S S S = J J J H
J
1
J
3
J
2
2 2
3 J
J
H

) ) ) )
2
1 3
2
3 2
2
2 1 2
1
J J J J J J J = H
J H
Yiming Qiu et al. cond-mat/0205018
Kent State 4/17/03
Inelastic Magnetic Neutron Scattering
f
k
i f
= Q k k
i
k
2 2
1 1
2 2 i f
mv mv [ = !
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Spectroscopy of spin trimers
Transition to quartet Transition to quartet
Yiming Qiu et al. cond-mat/0205018
70 K
10 K
0.0
0.1
0.0
0.1
0.2
J H
Kent State 4/17/03
Strongly fluctuating spin trimer AFM
Yiming Qiu et al. cond-mat/0205018
300K
2.6K
Kent State 4/17/03
Outline
1. Introduction
a. Magnets, ordered and fluctuating
b. How to distinguish using neutrons
2. Whirlwind tour of fluctuating magnets
a. Spin trimer magnetism in La
4
Cu
3
MoO
12
b. Cooperative singlet in spin-1 chain
c. Frustrated spin liquid in organic magnet
d. Fluctuating spin directors in spinel oxide
3. Summary and Current Frontiers
Kent State 4/17/03
Unconventional magnetism in NENP
K 91 } 5
CW
Negative Curie Weiss temperature indicates AFM interactions
No phase transition and
Negative Curie Weiss temperature indicates AFM interactions
No phase transition and 0 for small p p T G
G
1
G
Kent State 4/17/03
Haldane gap in Y
2
BaNiO
5
40
20
60
0
0 0.5 1
1.5 2
q (T)
h
[
(
m
e
V
)
Ba
Y
O
2-
Ni
T. Ito, K. Oka and H. Takagi
MAPS (ISIS)
Kent State 4/17/03
singlet ground state of S=1 chain
Magnets with 2S=nz have a nearest neighbor singlet covering
with full lattice symmetry.
Excited states are propagating bond triplets separated from the
ground state by an energy gap . J } (
Haldane PRL (1983)
Affleck, Kennedy, Lieb, and Tasaki PRL (1987)
Kent State 4/17/03
Cutting chains in Y
2
BaNi
1-x
Mg
x
O
5
Mg
2+
on Ni
2+
sites finite length chains
Kojima et al. (1995)
Pure
Ni
2+
Ni
2+
Mg
2+
Mg
2+
3
Mg
2+
Y
3+
O
2-
Kent State 4/17/03
Hole doping Y
2-x
Ca
x
BaNiO
5
Ca
2+
on Y
3+
sites mobile bond defects
Kojima et al. (1995)
Pure
Ca
2+
Ca
2+
Y
3+
Y
3+
FM
Ca
2+
Ni
O
2-
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Gap modes in 4% Ca-doped Y
2
BaNiO
5
q H
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Bond Impurities in a spin-1 chain: Y
2-x
Ca
x
BaNiO
5
Y
3+
Ni
O
FM
Ca
2+
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Gap modes in 4% Ca-doped Y
2
BaNiO
5
E H
q H
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Minimal model of spin polaron
' J ' J
)
)
)
) )
)
2 2 2
1
2
2 2 2
1
2
1
2
1
2
'
'
' 1
' 1
LR LOR
L R O L R
LR L R
LOR O LR
S S LR LR
LOR LOR
J J
J
J
E J J S S
J S S cst
=
=

=

S S S S S
S S S
S S S
H
3
2
' J
' J J
3
2
1
LOR LR
S S = =
1
2
1
LOR LR
S S = =
1
2
0
LOR LR
S S = =
1 1
2 2
0,1
LR LR LOR LR
S S S S =
J
L
S
R
S
O
S
Kent State 4/17/03
Outline
1. Introduction
a. Magnets, ordered and fluctuating
b. How to tell using neutrons
2. Whirlwind tour of fluctuating magnets
a. Spin trimer magnetism in La
4
Cu
3
MoO
12
b. Cooperative singlet in spin-1 chain
c. Frustrated spin liquid in organic magnet
d. Fluctuating spin directors in spinel oxide
3. Summary and Current Frontiers
Kent State 4/17/03
Unconventional magnetism in CuHpCl
Negative 5
CW
indicates AFM interactions
No phase transition and
Spin ladder model consistent with G(T)
Negative 5
CW
indicates AFM interactions
No phase transition and
Spin ladder model consistent with G(T)
0 for 0 p p T G
Kent State 4/17/03
Structure of CuHpCl
CuHpCl is hydrogen bonded crystal of Cu
2
(C
5
H
12
N
2
)
2
Cl
4
Molecules possess approximate centro symmetry
Exchange interaction within molecule |J|<1 meV
Two lattices from H-bond exchange
b
Kent State 4/17/03
Building an enigma
Dispersion throughout a-c plane Dispersion throughout a-c plane
Spin liquid on 3-dimensional lattice Spin liquid on 3-dimensional lattice
Magnetic scattering from CuHpCl
powder
Kent State 4/17/03
Detailed bond energy distribution
a*
c* (101)
(100)
(001)
Point size First moment
w
Bond ID
d 0 d
S S J

(meV)
1 0.42(3)
2 0.06(4)
3 -0.29(3)
4 -0.18(1)
5 0.06(2)
6 -0.05(4)
7 -0.09(7)
8 -0.15(3)

Kent State 4/17/03
Frustrated three dimensional spin liquid
Bond ID
d 0 d
S S J

(meV)
1 0.42(3)
2 0.06(4)
3 -0.29(3)
4 -0.18(1)
5 0.06(2)
6 -0.05(4)
7 -0.09(7)
8 -0.15(3)

Kent State 4/17/03
Outline
1. Introduction
a. Magnets, ordered and fluctuating
b. How to tell using neutrons
2. Whirlwind tour of fluctuating magnets
a. Spin trimer magnetism in La
4
Cu
3
MoO
12
b. Cooperative singlet in spin-1 chain
c. Frustrated spin liquid in organic magnet
d. Fluctuating spin directors in spinel oxide
3. Summary and Current Frontiers
Kent State 4/17/03
ZnCr
2
O
4
: Corner sharing tetrahedra
CW
5
Kent State 4/17/03
Signs of frustration: short range order for T<|5
CW
|
Points of interest:
2T/Qr
0
=1.4
=> nn. AFM correlations
No scattering at low Q
=> satisfied tetrahedra
S.-H. Lee et al. PRL (2000)
Kent State 4/17/03
Fluctuating spin directors
S.-H. Lee et al. Nature (2002)
2 2
i j
ij
tot i
i
J
JS J S
=
=

S S H
Tchernyshyov et al. PRL (2001)
Kent State 4/17/03
Summary:
Two visions for the behavior of substances with
AFM interactions between spins
Nel: Two interpenetrating anti-parallel ferromagnets
Landau: singlet formation, cooperative paramagnetism
Neutron diffraction shows that Nels state is
possible
Inelastic neutron scattering shows that quantum
magnetism is also possible when there is frustration
and/or weak connectivity
The concept of weakly interacting composite spin is
central for understanding strongly fluctuating
magnets
Viewgraphs and publications at http://www.pha.jhu.edu/~broholm/homepage
Outlook
1. Structural refinement of fluctuating objects
2. Applicability to a wide range of materials
3. Dynamic correlations under extreme
conditions
4. Spin polarons in high T
C
superconductors?
5. Magnetism of interacting spin polarons
Design by T. D. Pike
http://www.pha.jhu.edu/~broholm/MACS