Wing-Ho Ko - Novel Magnetic and Superconducting States in Spin-1/2 Kagome Lattice and Its Doped Variant

Novel Magnetic and Superconducting States in
Spin-1/2 Kagome Lattice and its Doped Variant

Wing-Ho Ko
MIT
July 7, 2010
Acknowledgments
Acknowledgments
Patrick A. Lee
Xiao-Gang Wen
Senthil Todadri
Tai-Kai Ng
Young S. Lee
John D. Joannopoulos
Robert Jae
Mehran Kardar
Wolfgang Ketterle
Issac Chuang
Leonid Levitov
Washington Taylor
Iain Stewart
John McGreevy
Edward Farhi
Margaret OMeara
Michael Hermele
Cody Nave
Ying Ran
Zheng-Cheng Gu
K. T. Law
Saeed Saremi
Maissam Barkeshli
Nan Gu
Jamal Rahi
Brian Swingle
Tarun Grover
Fa Wang
Tim Chen
Abolhassan Vaezi
Zheng-Xin Liu
Rahul Nandkishore
Juven Wang
Alejandro Rodriguez
Anjan Soumyanarayanan
Wing-Ho Ko (MIT) Novel states in spin-1/2 kagome July 7, 2010 2 / 41
Outline
Outline
1 Quantum Spin Liquid
2 The Spin-1/2 Kagome Lattice and the U(1) DSL State
3 Raman Scattering
4 External Magnetic Field
5 Hole Doping
Reference: Ran, Ko, Lee, & Wen, PRL 102, 047205 (2009)
Ko, Lee, & Wen, PRB 79, 214502 (2009)
Ko, Liu, Ng, & Lee, PRB 81, 024414 (2010)
Quantum Spin Liquid
Outline
3 Raman Scattering
5 Hole Doping
Quantum Spin Liquid
Strong Coulomb repulsion leads to Mott insulators with
antiferromagnetic interactions.
Hubbard modelthe archetypal strongly correlated system:
H
Hb
=
t
ij ,
c
i
c
j + U
i
n
i
n
i
U large and n
i
1 = t-J model:
H
tJ
=
ij
J
_
S
i
S
j

1
4
n
i
n
j
_
t
_
c
i
c
j
+ h.c.
_
;
i
c
i
1
Half-lling (n
i
= 1) = antiferromagnetic spin system
(Heisenberg model):
H
Hsb
=
ij
JS
i
S
j
Kinetic energy Coulomb interaction
Constraint
virtual hopping
Quantum Spin Liquid
Under normal circumstances, the classical Neel order wins.
H
Hsb
=
ij
JS
i
S
j
The classical Neel state is not the true quantum ground state.
But quantum uctuation is usually not strong enough to destroy the
classical order.
Neel
1970
Shull
1994
Quantum Spin Liquid
However, the Neel order is not the only possibility.
In 1973, Anderson proposed the resonating valence
bond (RVB) state, which is formed by superposing
singlets.
Unlike the Neel state, the elementary excitation in the
RVB state are spin-1/2 spinons.
And in the doped case, an electron is fractionalized
into a spinon and a holon. Anderson
=
+ +
=
||
2
Quantum Spin Liquid
singlets.
vs.
Quantum Spin Liquid
singlets.
vs.
Quantum Spin Liquid
Two major classes of singlet states: valence bond solids
(VBS) and spin liquid (SL)
In a SL, dierent bond congurations
superpose, which results in a state that breaks
no lattice symmetry.
In a VBS, certain singlet bonds are preferred,
which results in a symmetry-broken state.
A VBS state generally has a spin gap, while a
SL state can be gapped or gapless.
vs.
Quantum Spin Liquid
L.D. Landau, E.M. Lifshitz and X.G. Wen
Long Lost English Edition
Course of Theoretical Physics
Volume 11
Topological and
Quantum Order
Quantum Spin Liquid
Quantum Spin Liquid
Theory of spin liquid: slave boson formulation
Start with the Heisenberg (or more generally the tJ) model:
H
tJ
=
ij
J
_
S
i
S
j

1
4
n
i
n
j
_
t
_
c
i
c
j
+ h.c.
_
;
i
c
i
1
Apply the slave boson decomposition [Lee et al., RMP 78, 17 (2006)]:
S
i
=
1
2
,
f

i
,
f
i
; c
i
= f

i
h
i
; f

i
f
i
+ f

i
f
i
+ h
i
h
i
= 1
Decouple four-operator terms by a HubbardStratonovich
transformation, with the following self-consistency conditions:
ij

f

i
f
j
;
ij
f

i
f
j
f

i
f
j
Spin liquid corresponds to [

ij
[ = and [
ij
[ = . Letting
ij
= e
i
ij
and assuming also
ij
= 0, we get....
spinon
holon
Constraint enforced by
Lagrange multiplier
i
0
Quantum Spin Liquid
Theory of spin liquid: emergent gauge eld
H
MF
=
i
f

i
(i
i
0
F
)f
i
J
ij ,
(e
i
ij
f

i
f
j
+h.c.)
+
i
h
i
(i
i
0
B
)h
i
t
ij
(e
i
ij
h
i
h
j
+ h.c.)
The eld is an emergent gauge eld, corresponding to gauge
symmetry f

e
i
f

, h e
i
h.
At the lattice level is a compact gauge eld (i.e., monopoles are
allowed).
But with Dirac fermions, the system can be in a deconned phase
(i.e., monopoles can be neglected) [Hermele et al., PRB 70, 214437 (2004)].
Neglecting uctuation of , spinons and holons are decoupled.
Mean-eld ansatz for SL state can be specied by pattern of ux.
Quantum Spin Liquid
Factors favoring singlet states: small spin, low
dimensionality, and geometrical frustration
1D chain:
E
Neel
= S
2
J per bond
E
singlet
=
1
2
S(S + 1)J per bond
Higher dimensions = singlet less
favorable.
Geometrical frustration: cant make all
bonds happy at the same time.
= Classical order is weakened.
vs.
vs.
?
vs.
Quantum Spin Liquid
1D chain:
E
Neel
= S
2
J per bond
E
singlet
=
1
2
S(S + 1)J per bond
favorable.
vs. vs.
?
vs.
Quantum Spin Liquid
1D chain:
E
Neel
= S
2
J per bond
E
singlet
=
1
2
S(S + 1)J per bond
favorable.
vs. vs.
?
vs.
Quantum Spin Liquid
1D chain:
E
Neel
= S
2
J per bond
E
singlet
=
1
2
S(S + 1)J per bond
favorable.
vs. vs.
?
vs.
Quantum Spin Liquid
Possible material realizations of quantum spin liquids
-(ET)
2
X
Triangular lattice
Na
4
Ir
3
O
8
Hyperkagome lattice
Cu O H
Zn Cl
ZnCu
3
(OH)
6
Cl
2
Kagome lattice
The Spin-1/2 Kagome Lattice and the U(1) DSL State
Outline
3 Raman Scattering
5 Hole Doping
The nearest-neighbor antiferromagnetic Heisenberg model
is highly frustrated on the kagome lattice.
Kagome lattice = 2D lattice of
corner-sharing triangles.
Kagome lattice is frustrated: no
simple Neel order.
Classical ground states:
i
S
i
= 0 .
# classical ground states e
N
.
[Chalker et al., PRL 68, 855 (1992)].
Experimental realization of S = 1/2 kagome:
herbertsmithite ZnCu
3
(OH)
6
Cl
2
.
Herbertsmithite: layered structure with Cu
forming an AF kagome lattice.
Caveats: Zn impurities and Dzyaloshinskii
Moriya interactions.
Experimental results [e.g., Helton et al., PRL 98,
107204 (2007); Bert et al., JP:CS 145, 012004 (2009)]:
Neutron scattering: no magnetic order down
to 1.8 K.
SR: no spin freezing down to 50 K.
Heat capacity: vanishes as a power law as
T 0.
Spin susceptibility: diverges as T 0.
NMR shift: power law as T 0.
Cu O H
Zn Cl
Leading theoretical proposals: the 36-site VBS and the
U(1) Dirac spin liquid
The 36-site VBS pattern is found in series
expansion [Singh and Huse, PRB 76, 180407 (2007)]
and entanglement renormalization [Evenbly and
Vidal, arXiv:0904.3383].
From VMC, the U(1) Dirac spin liquid (DSL)
state has the lowest energy among various SL
states, and is stable against small VBS
perturbations [e.g., Ran et al., PRL 98, 117205 (2007)].
Exact diagonalization: initially found small
( J/20) spin gap; now leaning towards a
gapless proposal [Waldtmann et al., EPJB 2, 501
(1998); arXiv:0907.4164].
vs.
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
U(1) DSL state: mean-eld ansatz
H
MF
=
i
f

i
(i
i
0
F
)f
i
3J
8
ij ,
(e
i
ij
f

i
f
j
+h.c.)
+
i
h
i
(i
i
0
B
)h
i
t
ij
(e
i
ij
h
i
h
j
+ h.c.)
Neglecting uctuation of , spinons
and holons are decoupled.
Mean-eld ansatz for SL state can be
specied by pattern of ux.
U(1) Dirac spin liquid state: ux per
and 0 ux per .
ux = unit cell doubled in band
structures.
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
Enlarged Cell; Original Cell
U(1) DSL state: mean-eld ansatz
H
MF
=
i
f

i
(i
i
0
F
)f
i
3J
8
ij ,
(e
i
ij
f

i
f
j
+h.c.)
+
i
h
i
(i
i
0
B
)h
i
t
ij
(e
i
ij
h
i
h
j
+ h.c.)
Neglecting uctuation of , spinons
and holons are decoupled.
Mean-eld ansatz for SL state can be
specied by pattern of ux.
U(1) Dirac spin liquid state: ux per
and 0 ux per .
ux = unit cell doubled in band
structures.
t
e
= +t ; t
e
= t
Properties of the U(1) DSL state: band structure
Real space
t
e
= +t ; t
e
= t
k-space
k
y
2/3
/3
2/3
/3
x2
k
x

/ 2 / 2
x2
k
x
/ 2 / 2
Real space
t
e
= +t ; t
e
= t
k-space
k
y
2/3
/3
2/3
/3
x2
k
x

/ 2 / 2
x2
k
x
/ 2 / 2
Real space
t
e
= +t ; t
e
= t
k-space
k
y
2/3
/3
2/3
/3
x2
k
x

/ 2 / 2
x2
k
x
/ 2 / 2
Properties of the U(1) DSL state: thermodynamics and
correlation
At low energy, the U(1) DSL state is
described by QED
3
.
i.e., gauge eld coupled to Dirac
fermions in (2+1)-D.
Thermodynamics of the U(1) DSL state
is dominated by the spinon Fermi surface.
Zero-eld spin susceptibility: (T) T.
Heat capacity: C
V
(T) T
2
.
U(1) DSL state is quantum critical
many correlations decay algebraically
[Hermele et al., PRB 77, 224413 (2008)].
Emergent SU(4) symmetry among Dirac
nodes = dierent correlations can
have the same scaling dimension.
Research motivation: deriving further experimental
consequences of the U(1) DSL state
All experiments point to a state without magnetic order. But more
data is needed to tell if it is a VBS state or a SL state, and which
VBS/SL state it is.
Without concrete theory, the experimental data are hard to interpret.
Without concrete theory, unbiased theoretical calculations are dicult.
The U(1) Dirac spin-liquid state is a theoretically interesting exotic
state of matter.
Thus, our approach: assume the DSL state and consider
further experimental consequences.
Raman Scattering
Outline
3 Raman Scattering
5 Hole Doping
Raman Scattering
Raman scattering in Mott-Hubbard system: the
ShastryShraiman formulation
Raman scattering = inelastic scattering of photon.
Good for studying excitations of the system.
Probe only excitations with q 0.
We are concerned with a half-lled Hubbard system, in the regime
where [
i

f
[ U and
i
U.
Both initial and nal states are spin states.
= T-matrix can be written in terms of spin operators.
Intermediate states are dominated by the sector where
i
n
i
n
i
= 1.
The T-matrix can be organized as an expansion in t/(U
i
)
[Shastry & Shraiman, IJMPB 5, 365 (1991)].
T
(2)
t
2
U
i
S
i
S
j
+. . .
Raman Scattering
Spin-chirality terms in the ShastryShraiman formulation
Because of holon-doublon symmetry, there is no t
3
order contribution.
i
ii iii
i
ii iii
+
= 0
For the square and triangular lattice, there is no t
4
order contribution
to spin-chirality because of a non-trivial cancellation between 3-site
and 4-site pathways.
i
ii
iii
iv
i
ii
iii
iv
i
ii
iii
iv
i
ii
iii
iv
+ + +
= 0
But such cancellation is absent in the kagome lattice.
Raman Scattering
Spin-chirality terms in the ShastryShraiman formulation
Because of holon-doublon symmetry, there is no t
3
order contribution.
i
ii iii
i
ii iii
+
= 0
For the square and triangular lattice, there is no t
4
order contribution
to spin-chirality because of a non-trivial cancellation between 3-site
and 4-site pathways.
i
ii
iii
iv
i
ii
iii
iv
+ + +
t
4
(U
i
)
3
S
i
S
j
S
k
+. . .
But such cancellation is absent in the kagome lattice.
Raman Scattering
Raman T-matrix for the kagome geometry
For kagome geometry, the Raman T-matrix decomposes into 3 irreps:
T = T(A
1g
)( xx+ yy)+T(E
(1)
g
)( xx yy)+T(E
(2)
g
)( xy+ yx)+T(A
2g
)( xy yx)
To lowest order in inelastic terms,
T(E
(1)
g
) =
4t
2
i
U
1
4
_
ij ,/
+
ij ,\
2
ij ,
_
S
i
S
j
T(E
(2)
g
) =
4t
2
i
U
3
4
_
ij ,/
ij ,\
_
S
i
S
j
T(A
1g
) =
t
4
(
i
U)
3
_
2
ij
+
ij
_
S
i
S
j
T(A
2g
) =
2
3it
4
(
i
U)
3
R
_
3 + 3 + +
+ + + +
_
(
i
j
k
= S
i
S
j
S
k
, etc.)
Raman Scattering
Raman signals: spinon-antispinon pairs
S
i
S
j
f

f f

f and S
i
(S
j
S
k
) f

f f

f f

f
= contributions from spinon-antispinon pairs,
e.g.,
[f
2pairs
f

f f

f [i , f
2pairs
[f

f f

f [i ,= 0
[f
1pairs
f

f [i , f
1pairs
[f

f f

f [i ,= 0
This produces a continuum of signal:
I
() =
f
Npairs
[T
[i
2
DOS().
At low energy, one-pair states dominates.
For Dirac node, DOS
1pair
c, and matrix element
is suppressed in E
g
and A
1g
, but not in A
2g
.
= Spinon-antispinon pairs contribute
I
A
2g
() c and I
E
g
/A
1g
() c
3
at low energy.
c

3
I
E
g
, I
A
1g

DOS,I
A
2g
Raman Scattering
Raman signals: emergent gauge mode
However, an additional collective excitation is
available in A
2g
:
S
i
S
j
S
k
f

f f

f f

f
i
3
exp(i
_
d) + h.c.

3
__
b d
2
x
= I
(gauge)
A
2g

b
b
+. . . q
2
+. . .
[Recall that f

i
f
j
exp(i
ij
) ]
In our case (QED
3
with Dirac fermions), turns
out that 1/ when q 0
[Ioe & Larkin, PRB 39, 8988 (1989)].
Analogy: plasmon mode vs. particle-hole
continuum in normal metal.
b
1/
Raman Scattering
Raman signals: summary
A
1g
, E
g
Energy shift
Intensity

3
A
2g
Energy shift
Intensity
???

1/
Raman Scattering
Experimental comparisons: some qualitative agreements
Wulferding et al. [arXiv:1005.4831] have obtained Raman signal on
herbertsmithite.
At low T, data shows a broad background with a near-linear piece at
low-energy.
Roughly agree with the theoretical picture presented previously.
External Magnetic Field
Outline
3 Raman Scattering
5 Hole Doping
External magnetic eld and the formation of Landau levels
In Mott systems, B-eld causes only Zeeman
splitting.
This induces spinon and antispinon pockets
near the Dirac node.
However, with the emergent gauge eld ,
Landau levels can form spontaneously.
From VMC calculations,
e
Prj
FP
0.33(2)B
3/2
+ 0.00(4)B
2
e
Prj
LL
0.223(6)B
3/2
+ 0.03(1)B
2
e
LL
MF
< e
FP
MF
to leading order in n
= Landau level state is favored.
B
b
S
z
density uctuation as gapless mode
b is an emergent gauge eld.
= Its strength can uctuate in space.
The uctuation of b is tied to the
uctuation of S
z
density.
In long-wavelength limit, energy cost of
b uctuation 0.
= The system has a gapless mode!
Derivative expansion = linear
dispersion.
Other density uctuations and
quasiparticle excitations are gapped.
= Gapless mode is unique.
Mathematical description given by
ChernSimons theory.
b
vs.
S
z
uctuation of S
z
density.
b uctuation 0.
dispersion.
ChernSimons theory.
b
vs.
b
S
z
uctuation of S
z
density.
b uctuation 0.
dispersion.
ChernSimons theory.
b
vs.
Gapless mode and XY-ordering
Recap: we found a single linearly-dispersing
gapless mode, which looks like...
A Goldstone boson! And indeed it is.
Corresponding to this Goldstone mode is a
spontaneously broken XY order.
Analogy:
Superuid:

=
e
i

, [ ,

] = i , gapless
uctuation = ordered (SF) phase;
XY model:

S
+
= e
i

, [

S
z
,

] = i , gapless
S
z
uctuation = XY ordered phase.
VMC found the q = 0 order.
S
+
in XY model V
in QED
3
.
= In-plane magnetization M B
.
(V

monopole operator, its scaling dimension)
0.00(1)
0.67(1)
0.67(1)
0.66(1)
0.65(1)
0.01(1)
0.65(1)
0.65(1)
0
Hole Doping
Outline
3 Raman Scattering
5 Hole Doping
Hole Doping
Recap: band structure
Real space
t
e
= +t ; t
e
= t
k-space
k
y
2/3
/3
2/3
/3
x2
k
x

/ 2 / 2
x2
k
x
/ 2 / 2
Hole Doping
Hole doping and the formation of Landau levels
Doping can in principle be achieved by
substituting Cl with S.
In the slave-boson picture, hole doping
introduces holons and antispinons.
As before, an emergent b eld can open up
Landau levels in the spinon and holon bands.
At mean-eld, E
spinon
B
3/2
while
E
holon
B
2
.
= LL state favored.
At mean-eld, b optimal when antispinons
form = 1 LL state.
= Holons form = 1/2 Laughlin state.
dope
b
f
, f
h
Hole Doping
Charge uctuation, Goldstone mode, and superconductivity
b uctuation holon density uctuation
charge density uctuation.
Long-wavelength b uctuation cost
c 0 if real EM-eld is turned o.
= a single linearly-dispersing mode
Goldstone boson.
This time the Goldstone boson is eaten
up by the EM-eld to produce a
superconductor.
This superconducting state breaks
T-invariance.
Intuitively, four species of holon binded
together = expects
EM
= hc/4e for
a minimal vortex.
Conrmed by ChernSimons
formulation.
f
1,...,2
h
1,...,4
b
Hole Doping
Quasiparticle statisticsintuitions
Quasiparticles are bound states of semions
in holon sectors and/or fermions in spinon
sector.
For nite energy, bound states must be
neutral w.r.t. the gapless mode.
There are two types of elementary
quasiparticles:
1 semion-antisemion pair in holon sector;
2 spinon-holon pair
( Bogoliubov q.p. in conventional SC).
All other quasiparticles can be built from
these elementary ones.
Statistics can be derived by treating
dierent species as uncorrelated.
Semions from holon sector = existence
of semionic (mutual) statistics.
1
h
1
h
4
1
h
1
h
4
2
f
h
4
1
h
1
h
4
2
f
h
4
2
= 2
1
h
1
h
4
1
h
1
h
4
1
= + = 2
1
h
1
h
4
1
h
1
h
2
1
=
Hole Doping
sector.
quasiparticles:
2 spinon-holon pair
1
h
1
h
4
1
h
1
h
4
2
f
h
4
1
h
1
h
4
2
f
h
4
2
= 2
1
h
1
h
4
1
h
1
h
4
1
= + = 2
1
h
1
h
4
1
h
1
h
2
1
=
Hole Doping
sector.
quasiparticles:
2 spinon-holon pair
1
h
1
h
4
1
h
1
h
4
2
f
h
4
1
h
1
h
4
2
f
h
4
2
= 2
1
h
1
h
4
1
h
1
h
4
1
= + = 2
1
h
1
h
4
1
h
1
h
2
1
=
Hole Doping
sector.
quasiparticles:
2 spinon-holon pair
1
h
1
h
4
1
h
1
h
4
2
f
h
4
1
h
1
h
4
2
f
h
4
2
= 2
1
h
1
h
4
1
h
1
h
4
1
= + = 2
1
h
1
h
4
1
h
1
h
2
1
=
Hole Doping
sector.
quasiparticles:
2 spinon-holon pair
1
h
1
h
4
1
h
1
h
4
2
f
h
4
1
h
1
h
4
2
f
h
4
2
= 2
1
h
1
h
4
1
h
1
h
4
1
= + = 2
1
h
1
h
4
1
h
1
h
2
1
=
Hole Doping
Crystal momenta of quasiparticleprojective symmetry
group study
For spinon-holon pair, k is well-dened on
the original Brillouin zone.
These can be recovered using Projective
symmetry group (PSG).
In contrast, the semion is fractionalized
from a holon.
= semion-antisemion pair may not have
well-dened k.
+ +
+
+ +
+
+ +
+
+ +
+
+ +
+
+ +
+

=
*
* *
*
* *
*
*
* = k of spinon-holon pairs
Hole Doping
Crystal momenta of quasiparticleprojective symmetry
group study
For spinon-holon pair, k is well-dened on
the original Brillouin zone.
These can be recovered using Projective
symmetry group (PSG).
In contrast, the semion is fractionalized
from a holon.
= semion-antisemion pair may not have
well-dened k.
+ +
+
+ +
+
+ +
+
+ +
+
+ +
+
+ +
+

=
*
* *
*
* *
*
*
* = k of spinon-holon pairs
Conclusions
Conclusions
The U(1) Dirac spin-liquid state possess many unusual properties and
may be experimentally realized in herbertsmithite.
The Raman signal of the DSL state has a broad background
(contributed by spinon-antispinon continuum) and a 1/ singularity
(contributed by collective [gauge] excitations).
Under external magnetic eld, the DSL state forms Landau levels,
which corresponds to a XY symmetry broken state with Goldstone
boson corresponding to S
z
density uctuation.
When the DSL state is doped, an analogous mechanism give rise to
an AndersonHiggs scenario and hence superconductivity.
But minimal vortices carry hc/4e ux and the system contains exotic
quasiparticle having semionic mutual statistics.
Reference: Ran, Ko, Lee, & Wen, PRL 102, 047205 (2009)
Ko, Lee, & Wen, PRB 79, 214502 (2009)
Ko, Liu, Ng, & Lee, PRB 81, 024414 (2010)

Wing-Ho Ko - Novel Magnetic and Superconducting States in Spin-1/2 Kagome Lattice and Its Doped Variant

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Wing-Ho Ko - Novel Magnetic and Superconducting States in Spin-1/2 Kagome Lattice and Its Doped Variant

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Novel Magnetic and Superconducting States in

Spin-1/2 Kagome Lattice and its Doped Variant

Spin liquid corresponds to [

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