wing-ho ko- novel magnetic and superconducting states in spin-1/2 kagome lattice and its doped...
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Novel Magnetic and Superconducting States inSpin-1/2 Kagome Lattice and its Doped Variant
Wing-Ho Ko
MIT
July 7, 2010
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Acknowledgments
Acknowledgments
Patrick A. Lee
Xiao-Gang WenSenthil TodadriTai-Kai NgYoung S. Lee
John D. JoannopoulosRobert JaffeMehran KardarWolfgang KetterleIssac ChuangLeonid Levitov
Washington TaylorIain StewartJohn McGreevyEdward Farhi
Margaret OMeara
Michael Hermele
Cody NaveYing RanZheng-Cheng GuK. T. LawSaeed SaremiMaissam Barkeshli
Nan GuJamal RahiBrian SwingleTarun GroverFa WangTim Chen
Abolhassan VaeziZheng-Xin LiuRahul NandkishoreJuven WangAlejandro Rodriguez
Anjan Soumyanarayanan
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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)
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Quantum Spin Liquid
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
Wing-Ho Ko (MIT) Novel states in spin-1/2 kagome July 7, 2010 4 / 41
Q S i Li id
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Quantum Spin Liquid
Strong Coulomb repulsion leads to Mott insulators withantiferromagnetic interactions.
Hubbard modelthe archetypal strongly correlated system:HHb = t
ij, c
icj + U
i nini
U large and
ni
1 =
t-J model:
HtJ =
ij JSi Sj 14 ninj
t
cicj + h.c.
;
ci ci 1
Half-filling (ni = 1) = antiferromagnetic spin system(Heisenberg model):
HHsb =
ij JSi Sj
Kinetic energy Coulomb interaction
Constraint
virtual hopping
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Q t S i Li id
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Quantum Spin Liquid
Under normal circumstances, the classical Neel order wins.
HHsb =
ij JSi Sj
The classical Neel state is not the true quantum ground state. But quantum fluctuation is usually not strong enough to destroy the
classical order.
Neel1970
Shull1994
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Quantum Spin Liquid
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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 superposingsinglets.
Unlike the Neel state, the elementary excitation in theRVB state are spin-1/2 spinons.
And in the doped case, an electron is fractionalizedinto a spinon and a holon. Anderson
= + +
= ||2
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Quantum Spin Liquid
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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 superposingsinglets.
Unlike the Neel state, the elementary excitation in theRVB state are spin-1/2 spinons.
And in the doped case, an electron is fractionalizedinto a spinon and a holon. Anderson
vs.
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Quantum Spin Liquid
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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 superposingsinglets.
Unlike the Neel state, the elementary excitation in theRVB state are spin-1/2 spinons.
And in the doped case, an electron is fractionalizedinto a spinon and a holon. Anderson
vs.
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Quantum Spin Liquid
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Quantum Spin Liquid
Two major classes of singlet states: valence bond solids(VBS) and spin liquid (SL)
In a SL, different bond configurationssuperpose, 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 aSL state can be gapped or gapless.
vs.
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Quantum Spin Liquid
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Q p q
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Quantum Spin Liquid
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Q p q
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Quantum Spin Liquid
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Theory of spin liquid: emergent gauge field
HMF = i
f
i(ii
0
F)f
i J
ij,(eiijf
ifj
+h.c.)
+
ihi (i
i0 B)hi t
ij
(eiijhi hj + h.c.)
The
field is an emergent gauge field, corresponding to gaugesymmetry f eif, h eih. At the lattice level is a compact gauge field (i.e., monopoles are
allowed).
But with Dirac fermions, the system can be in a deconfined phase(i.e., monopoles can be neglected) [Hermele et al., PRB 70, 214437 (2004)].
Neglecting fluctuation of, spinons and holons are decoupled. Mean-field ansatz for SL state can be specified by pattern of flux.
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Quantum Spin Liquid
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Factors favoring singlet states: small spin, lowdimensionality, and geometrical frustration
1D chain:
ENeel = S2J per bondEsinglet =
1
2
S(S + 1)J per bond
Higher dimensions = singlet lessfavorable.
Geometrical frustration: cant make all
bonds happy at the same time.= Classical order is weakened.
vs.
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Quantum Spin Liquid
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Factors favoring singlet states: small spin, lowdimensionality, and geometrical frustration
1D chain:
ENeel = S2J per bondEsinglet =
1
2
S(S + 1)J per bond
Higher dimensions = singlet lessfavorable.
Geometrical frustration: cant make all
bonds happy at the same time.= Classical order is weakened.
vs.vs.
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Quantum Spin Liquid
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Factors favoring singlet states: small spin, lowdimensionality, and geometrical frustration
1D chain:
ENeel = S2J per bondEsinglet =
1
2
S(S + 1)J per bond
Higher dimensions = singlet lessfavorable.
Geometrical frustration: cant make all
bonds happy at the same time.= Classical order is weakened.
vs.vs.
?
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Quantum Spin Liquid
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Factors favoring singlet states: small spin, lowdimensionality, and geometrical frustration
1D chain:
ENeel = S2J per bondEsinglet =
1
2
S(S + 1)J per bond
Higher dimensions = singlet lessfavorable.
Geometrical frustration: cant make all
bonds happy at the same time.= Classical order is weakened.
vs.vs.
?
vs.
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Quantum Spin Liquid
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Possible material realizations of quantum spin liquids
-(ET)2XTriangular lattice
Na4Ir3O8Hyperkagome lattice
ZnCu3(OH)6Cl2Kagome lattice
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The Spin-1/2 Kagome Lattice and the U(1) DSL State
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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
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The Spin-1/2 Kagome Lattice and the U(1) DSL State
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The nearest-neighbor antiferromagnetic Heisenberg modelis highly frustrated on the kagome lattice.
Kagome lattice = 2D lattice ofcorner-sharing triangles.
Kagome lattice is frustrated: nosimple Neel order.
Classical ground states:i Si = 0 .
# classical ground states eN.[Chalker et al., PRL 68, 855 (1992)].
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The Spin-1/2 Kagome Lattice and the U(1) DSL State
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Experimental realization ofS = 1/2 kagome:herbertsmithite ZnCu3(OH)6Cl2.
Herbertsmithite: layered structure with Cuforming an AF kagome lattice.
Caveats: Zn impurities and DzyaloshinskiiMoriya 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 downto 1.8 K.
SR: no spin freezing down to 50 K.
Heat capacity: vanishes as a power law asT 0. Spin susceptibility: diverges as T 0. NMR shift: power law as T 0.
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The Spin-1/2 Kagome Lattice and the U(1) DSL State
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Leading theoretical proposals: the 36-site VBS and theU(1) Dirac spin liquid
The 36-site VBS pattern is found in seriesexpansion [Singh and Huse, PRB 76, 180407 (2007)]and entanglement renormalization [Evenbly andVidal, arXiv:0904.3383].
From VMC, the U(1) Dirac spin liquid (DSL)state has the lowest energy among various SLstates, and is stable against small VBSperturbations [e.g., Ran et al., PRL 98, 117205 (2007)].
Exact diagonalization: initially found small( J/20) spin gap; now leaning towards agapless 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
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The Spin-1/2 Kagome Lattice and the U(1) DSL State
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U(1) DSL state: mean-field ansatz
HMF = i
f
i
(ii
0 F)fi
3J
8
ij,
(eiijf
i
fj+h.c.)
+
ihi (i
i0 B)hi t
ij
(eiijhi hj + h.c.)
Neglecting fluctuation of, spinonsand holons are decoupled.
Mean-field ansatz for SL state can bespecified by pattern of flux.
U(1) Dirac spin liquid state: flux perand 0 flux per . flux = unit cell doubled in band
structures.
0
0
0
0
0
0
0
0
0
0
0
0
0
0
0
Enlarged Cell; Original Cell
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The Spin-1/2 Kagome Lattice and the U(1) DSL State
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U(1) DSL state: mean-field ansatz
HMF = i
f
i
(ii
0 F)fi
3J
8
ij,
(eiijf
i
fj+h.c.)
+
ihi (i
i0 B)hi t
ij
(eiijhi hj + h.c.)
Neglecting fluctuation of, spinonsand holons are decoupled.
Mean-field ansatz for SL state can bespecified by pattern of flux.
U(1) Dirac spin liquid state: flux perand 0 flux per . flux = unit cell doubled in band
structures.teff = +t ; teff = t
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The Spin-1/2 Kagome Lattice and the U(1) DSL State
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Properties of the U(1) DSL state: band structure
Real space
teff = +t ; teff = t
k-space
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The Spin-1/2 Kagome Lattice and the U(1) DSL State
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Properties of the U(1) DSL state: band structure
Real space
teff = +t ; teff = t
k-space
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The Spin-1/2 Kagome Lattice and the U(1) DSL State
( )
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Properties of the U(1) DSL state: band structure
Real space
teff = +t ; teff = t
k-space
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The Spin-1/2 Kagome Lattice and the U(1) DSL State
f ( ) S
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Properties of the U(1) DSL state: thermodynamics andcorrelation
At low energy, the U(1) DSL state isdescribed by QED3.
i.e., gauge field coupled to Diracfermions in (2+1)-D.
Thermodynamics of the U(1) DSL stateis dominated by the spinon Fermi surface. Zero-field spin susceptibility: (T) T. Heat capacity: CV(T) T2.
U(1) DSL state is quantum criticalmany correlations decay algebraically[Hermele et al., PRB 77, 224413 (2008)].
Emergent SU(4) symmetry among Diracnodes = different correlations canhave the same scaling dimension.
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The Spin-1/2 Kagome Lattice and the U(1) DSL State
R h i i d i i f h i l
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Research motivation: deriving further experimentalconsequences of the U(1) DSL state
All experiments point to a state without magnetic order. But moredata is needed to tell if it is a VBS state or a SL state, and whichVBS/SL state it is.
Without concrete theory, the experimental data are hard to interpret. Without concrete theory, unbiased theoretical calculations are difficult. The U(1) Dirac spin-liquid state is a theoretically interesting exotic
state of matter.
Thus, our approach: assume the DSL state and considerfurther experimental consequences.
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Raman Scattering
O li
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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
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Raman Scattering
R tt i i M tt H bb d t th
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Raman scattering in Mott-Hubbard system: theShastryShraiman 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-filled Hubbard system, in the regimewhere
|i
f
| U and i
U.
Both initial and final states are spin states.= T-matrix can be written in terms of spin operators.
Intermediate states are dominated by the sector where
i nini = 1. The T-matrix can be organized as an expansion in t/(U i)
[Shastry & Shraiman, IJMPB 5, 365 (1991)].
T(2) t2UiSi Sj + . . .
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Raman Scattering
S i hi lit t i th Sh t Sh i f l ti
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Spin-chirality terms in the ShastryShraiman formulation
Because of holon-doublon symmetry, there is no t3 order contribution.
i
iiiii
i
iiiii+ = 0
For the square and triangular lattice, there is no t4 order contribution
to spin-chirality because of a non-trivial cancellation between 3-siteand 4-site pathways.
i
ii
iii
iv
i
ii
iii
iv
i
iiiii
iv
i
iiiii
iv+ + +
= 0
But such cancellation is absent in the kagome lattice.Wing-Ho Ko (MIT) Novel states in spin-1/2 kagome July 7, 2010 25 / 41
Raman Scattering
S i hi lit t s i th Sh st Sh i f l ti
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Spin-chirality terms in the ShastryShraiman formulation
Because of holon-doublon symmetry, there is no t3 order contribution.
i
iiiii
i
iiiii+ = 0
For the square and triangular lattice, there is no t4 order contribution
to spin-chirality because of a non-trivial cancellation between 3-siteand 4-site pathways.
i
ii
iii
iv
i
ii
iii
iv+ + +
t4(Ui)3
Si Sj Sk + . . . But such cancellation is absent in the kagome lattice.
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Raman Scattering
Raman T matrix for the kagome geometry
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Raman T-matrix for the kagome geometry
For kagome geometry, the Raman T-matrix decomposes into 3 irreps:
T = T(A1g)(xx+y y)+T(E(1)g )(xxy y)+T(E(2)g )(x y+y x)+T(A2g)(xyy x)
To lowest order in inelastic terms,
T(E(1)g ) =4t2
i
U14
ij
,/ +
ij
,
\2
ij
,
Si
Sj
T(E(2)g ) =4t2
iU3
4
ij,/
ij,\
Si Sj
T(A1g) =t4
(iU)3
2
ij +
ijSi Sj
T(A2g) =2
3it4
(iU)3
R
3 + 3 + +
+ + + +
(i j
k= Si Sj Sk, etc.)
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Raman Scattering
Raman signals: spinon antispinon pairs
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Raman signals: spinon-antispinon pairs
Si Sj ff ff and Si (Sj Sk) ff ff ff
= contributions from spinon-antispinon pairs,e.g.,
|f2pairs ff ff|i, f2pairs|ff ff|i = 0|f1pairs ff|i, f1pairs|ff ff|i = 0
This produces a continuum of signal:I() =
N
fNpairs|T|i2 DOS().
At low energy, one-pair states dominates.
For Dirac node, DOS1pair E, and matrix elementis suppressed in Eg and A1g, but not in A2g.
= Spinon-antispinon pairs contributeIA2g() Eand IEg/A1g() E3 at low energy.
E
3
IEg, IA1g
DOS,IA2g
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Raman Scattering
Raman signals: emergent gauge mode
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Raman signals: emergent gauge mode
However, an additional collective excitation isavailable in A2g:
Si Sj Sk ff ff ff i3 exp(i d) + h.c.
3
b d2x
= I(gauge)A2g bb + . . . q2 + . . .[Recall that fi fj exp(iij) ]
In our case (QED3 with Dirac fermions), turnsout that 1/ when q 0[Ioffe & Larkin, PRB 39, 8988 (1989)].
Analogy: plasmon mode vs. particle-holecontinuum in normal metal.
b
1/
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Raman Scattering
Raman signals: summary
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Raman signals: summary
A1g,
Eg
Energy shift
Intensity
3
A2g
Energy shift
Intensity
???
1/
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Raman Scattering
Experimental comparisons: some qualitative agreements
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Experimental comparisons: some qualitative agreements
Wulferding et al. [arXiv:1005.4831] have obtained Raman signal onherbertsmithite.
At low T, data shows a broad background with a near-linear piece atlow-energy.
Roughly agree with the theoretical picture presented previously.
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External Magnetic Field
Outline
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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
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External Magnetic Field
External magnetic field and the formation of Landau levels
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External magnetic field and the formation of Landau levels
In Mott systems, B-field causes only Zeemansplitting. This induces spinon and antispinon pockets
near the Dirac node.
However, with the emergent gauge field ,Landau levels can form spontaneously.
From VMC calculations,
ePrjFP 0.33(2)B3/2 + 0.00(4)B2
ePrj
LL 0.223(6)B3/2
+ 0.03(1)B2
eLLMF < eFPMF to leading order in n
= Landau level state is favored.
B
b
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External Magnetic Field
Sz density fluctuation as gapless mode
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Sz density fluctuation as gapless mode
b is an emergent gauge field.
= Its strength can fluctuate in space. The fluctuation of b is tied to thefluctuation of Sz density.
In long-wavelength limit, energy cost ofb fluctuation
0.
= The system has a gapless mode! Derivative expansion = linear
dispersion.
Other density fluctuations and
quasiparticle excitations are gapped.= Gapless mode is unique. Mathematical description given by
ChernSimons theory.
b
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External Magnetic Field
Sz density fluctuation as gapless mode
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Sz density fluctuation as gapless mode
b is an emergent gauge field.
= Its strength can fluctuate in space. The fluctuation of b is tied to thefluctuation of Sz density.
In long-wavelength limit, energy cost ofb fluctuation
0.
= The system has a gapless mode! Derivative expansion = linear
dispersion.
Other density fluctuations and
quasiparticle excitations are gapped.= Gapless mode is unique. Mathematical description given by
ChernSimons theory.
b
vs.
b
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External Magnetic Field
Sz density fluctuation as gapless mode
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Sz y g p
b is an emergent gauge field.
= Its strength can fluctuate in space. The fluctuation of b is tied to thefluctuation of Sz density.
In long-wavelength limit, energy cost ofb fluctuation
0.
= The system has a gapless mode! Derivative expansion = linear
dispersion.
Other density fluctuations and
quasiparticle excitations are gapped.= Gapless mode is unique. Mathematical description given by
ChernSimons theory.
b
vs.
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External Magnetic Field
Gapless mode and XY-ordering
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p g
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 aspontaneously broken XY order.
Analogy: Superfluid: =
ei, [, ] = i, gapless
fluctuation = ordered (SF) phase; XY model: S+ = ei, [Sz, ] = i, gapless
Sz fluctuation = XY ordered phase. VMC found the q = 0 order. S+ in XY model V in QED3.
= In-plane magnetization M B.(V monopole operator, its scaling dimension)
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Hole Doping
Outline
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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
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Hole Doping
Recap: band structure
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p
Real space
teff = +t ; teff = t
k-space
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Hole Doping
Hole doping and the formation of Landau levels
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Doping can in principle be achieved bysubstituting Cl with S.
In the slave-boson picture, hole dopingintroduces holons and antispinons.
As before, an emergent b field can open upLandau levels in the spinon and holon bands.
At mean-field, Espinon B3/2 whileEholon B2.= LL state favored.
At mean-field, b optimal when antispinonsform = 1 LL state.= Holons form = 1/2 Laughlin state.
dope
b
f, f h
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Hole Doping
Quasiparticle statisticsintuitions
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Quasiparticles are bound states of semionsin holon sectors and/or fermions in spinon
sector. For finite energy, bound states must be
neutral w.r.t. the gapless mode.
There are two types of elementaryquasiparticles:
1 semion-antisemion pair in holon sector;2 spinon-holon pair
( Bogoliubov q.p. in conventional SC).
All other quasiparticles can be built fromthese elementary ones.
Statistics can be derived by treatingdifferent species as uncorrelated.
Semions from holon sector = existenceof semionic (mutual) statistics.
1h1
h4
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Hole Doping
Quasiparticle statisticsintuitions
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Quasiparticles are bound states of semionsin holon sectors and/or fermions in spinon
sector. For finite energy, bound states must be
neutral w.r.t. the gapless mode.
There are two types of elementaryquasiparticles:
1 semion-antisemion pair in holon sector;2 spinon-holon pair
( Bogoliubov q.p. in conventional SC).
All other quasiparticles can be built fromthese elementary ones.
Statistics can be derived by treatingdifferent species as uncorrelated.
Semions from holon sector = existenceof semionic (mutual) statistics.
1h1
h4
2f
h4
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Hole Doping
Quasiparticle statisticsintuitions
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Quasiparticles are bound states of semionsin holon sectors and/or fermions in spinon
sector. For finite energy, bound states must be
neutral w.r.t. the gapless mode.
There are two types of elementaryquasiparticles:
1 semion-antisemion pair in holon sector;2 spinon-holon pair
( Bogoliubov q.p. in conventional SC).
All other quasiparticles can be built fromthese elementary ones.
Statistics can be derived by treatingdifferent species as uncorrelated.
Semions from holon sector = existenceof semionic (mutual) statistics.
1h1
h4
2f
h4
1
2
= 2
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Hole Doping
Quasiparticle statisticsintuitions
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Quasiparticles are bound states of semionsin holon sectors and/or fermions in spinon
sector. For finite energy, bound states must be
neutral w.r.t. the gapless mode.
There are two types of elementaryquasiparticles:
1 semion-antisemion pair in holon sector;2 spinon-holon pair
( Bogoliubov q.p. in conventional SC).
All other quasiparticles can be built fromthese elementary ones.
Statistics can be derived by treatingdifferent species as uncorrelated.
Semions from holon sector = existenceof semionic (mutual) statistics.
1h1
h4
1h1
h4
1
1
= + = 2
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Hole Doping
Quasiparticle statisticsintuitions
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Quasiparticles are bound states of semionsin holon sectors and/or fermions in spinon
sector. For finite energy, bound states must be
neutral w.r.t. the gapless mode.
There are two types of elementaryquasiparticles:
1 semion-antisemion pair in holon sector;2 spinon-holon pair
( Bogoliubov q.p. in conventional SC).
All other quasiparticles can be built fromthese elementary ones.
Statistics can be derived by treatingdifferent species as uncorrelated.
Semions from holon sector = existenceof semionic (mutual) statistics.
1h1
h4
1h1
h2
1
1
=
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Hole Doping
Crystal momenta of quasiparticleprojective symmetry
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group study
For spinon-holon pair, k is well-defined onthe original Brillouin zone.
These can be recovered using Projective
symmetry group (PSG).
In contrast, the semion is fractionalizedfrom a holon.=
semion-antisemion pair may not have
well-defined k.
+ +
+
+ + +
=
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Conclusions
Conclusions
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The U(1) Dirac spin-liquid state possess many unusual properties andmay 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 field, the DSL state forms Landau levels,which corresponds to a XY symmetry broken state with Goldstoneboson corresponding to Sz density fluctuation.
When the DSL state is doped, an analogous mechanism give rise toan AndersonHiggs scenario and hence superconductivity.
But minimal vortices carry hc/4e flux 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)
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