holes in a quantum spin liquid gapped phases in condensed matter gapped spin chains pure systems...

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Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Hopkins University and NIST Center for Neutron Rese Viewgraphs posted at http://www.pha.jhu.edu/~broholm/canada/index.htm Ca 2+ Y 2-x Ca x BaNiO 5 Ca 2+

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Page 1: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Holes in a Quantum Spin Liquid

Gapped phases in condensed matterGapped spin chains

Pure systems Doped systems

Conclusions

Collin BroholmJohns Hopkins University and NIST Center for Neutron Research

Viewgraphs posted at http://www.pha.jhu.edu/~broholm/canada/index.htm

Ca2+ Y2-xCaxBaNiO5

Ca2+

Page 2: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

CollaboratorsGuangyong Xu JHU -> University of ChicagoG. Aeppli NECJ. F. DiTusa Louisiana State University I. A. Zaliznyak JHU -> BNLC. D. Frost ISIST. Ito Electro-Technical Lab JapanK. Oka Electro-Technical Lab JapanH. Takagi ISSP and CREST-JST M. E. Bisher NECM. M. J. Treacy NECR. Paul NIST Center for Neutron Research

Publication on Y2-xCaxBaNiO5 to appear in Science (2000)

Page 3: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Quantum effects in atoms and in solids

Atom (He)Line spectrum

Solid (Mo)continuous spectrumif Q not specified

G. Dieke et al. (1968)

Christensen(1980)

Page 4: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Quantum effects from a gap

No gap Metal

Gap Insulator

Band gap only possible for even number of electrons per cell

Filled

Empty

Te

Page 5: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Impurities create states in the gap

0 0.2 0.4 0.6 0.8 1/T (K-1)

Res

isti

vity

(oh

m-c

m)

10-3

10-1

10

10 3

10 5

10 7

10 9

1011

“Dirty” sample

Cleaner sampleTe

1

Insulator

Metal

From Aschroft & Mermin

Page 6: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Other gapped phases in condensed matter

High energy physics yields low energy gap Band insulator Band semiconductorDimerized spin systems

Phase transition to gapped phase Superconductor Rotons in superfluid 4He Mott Metal-Insulator transitionSpin Peierls transition

Cross over to gapped phase for T<< Quantum Hall effectsUniform integer spin chains

Page 7: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

The beauty of magnetic dielectrics

Well defined low energy Hamiltonian

Chemistry provides qualitatively different HVary H with pressure, magnetic fieldEfficient experimental techniques

lllB

l

zl

llll

ll

g

SD

J

SH

SS

2

''

'H Exchange interaction

Single ion anisotropy

Dipole in magnetic field (Zeeman)

Page 8: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Spin systems of recent interest

Material Dim. Lattice Spin Anisot. J(meV)

T=0 state

Y2BaNiO5 1 chain 1 no 25 spin liq.NENP 1 chain 1 planar 4.1 spin liq.Cu-Nitrate 1 dimerized 1/2 no 0.5 spin liq.PHCC 2 dimerized 1/2 no 3 spin liq.La2CuO4 2 square 1/2 no 132 NeelK2NiF4 2 square 1 no NeelCr-Jarosite 2 kagome' 3/2 no 1.2 NeelMnF2 3 tetragonal 5/2 easy axis NeelZnCr2O4 3 spinel 3/2 no 4 NeelY2Mo2O7 3 pyrochlore 1 no 1-10 spin glass

Page 9: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Varying the dimensionality of spin systems

The crystals are actually three dimensionalExchange links spins on low-D network only

Non-magnetic “spacer” molecules in NDMAP

Anisotropic bonding in cubic KCuF3

Chain

dir

ect

ion

Page 10: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Susceptibility of gapped spin system

l

llB

B SSTk

g

H

M

2

Measure magnetization versus T in infinitesimal field:

Tatsuo et al. (1995)Renard et al (1988)

Te

Page 11: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Magnetization of gapped spin system

Ajiro et al. (1989)

Page 12: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Specific heat of gapped spin chain

A way to probe the low energy density of states

1/

TEe

dEE

dT

d

TC

H

NENC Orendac et al. (1995) NENP Tatsuo et al. (1995)

E

TeC

Page 13: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Magnetic Neutron Scattering

fi kkQ

fi EE

The scattering cross section is proportional to the Fourier transformed dynamic spin correlation function

ik fk

Q

2

''R

)'( )0(S)(S1

2

1),(

RRR

RRQiti teN

edtQ

S

Page 14: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

NIST Center for Neutron Research

Page 15: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Page 16: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Detection system on SPINS neutron spectrometer

Page 17: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Neutron scattering from gapped spin chain

gap

Nuclear incoherent scattering Triplet creation peakProton extraction pulse

Copper nitrateT=0.3 K

Xu et al. IRIS, ISIS

Page 18: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Dispersion relation for triplet waves

Dimerized spin-1/2 system: copper nitrate

JTkB

Xu et al PRL May 2000

Page 19: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

A spin-1/2 pair has a singlet - triplet gap:

Weak inter-dimer coupling cannot close gap

Bond alternation is relevant operator for quantum critical uniform spin chaininfinitesimal bond alternation yields gap

Why a gap in spectrum of dimerized spin system

J0totS

1totS

JJ

J

Page 20: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Gapped phases in isotropic spin systems?

n = number of spins per primitive unit cell S = the spin quantum number m = the magnetization per spin

n(S-m)=

Oshikawa, Yamanaka, and Affleck (1997) and Oshikawa (2000)

gaps in non-magnetized spin chains? Alternating spin-1/2 chain 2.1/2=1 perhaps Uniform spin-1/2 chain 1.1/2 =1/2 no Uniform spin-1 chain 1.1 =1 perhaps

Integer: gap possible

Non-Integer: gap impossible

Page 21: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Low T excitations in spin-1 AFM chain

Y2BaNiO5 T=10 KMARI chain ki

•Haldane gap =8 meV

•Coherent mode

•S(q,)->0 for Q->2n

pure

Page 22: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

AKLT state for spin-1 chain

• This is exact ground state for spin projection Hamiltonian

• 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 1983Affleck, Kennedy, Lieb, and Tasaki PRL 1987

i

iii

iiiii

toti SP 12

131

12 SSSSSSH

Page 23: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Sum rules and the single mode approximation

'cos1SS1

3

2),(

)(SS1

),(

'

2

)'(

''

ddqJN

qSd

qSeN

qSd

dddd

dd

ddqi

ddd

d

When a coherent mode dominates the spectrum:

)(

'cos1SS1

3

2

)(

),()(

'2

q

ddqJN

q

qSdqS

dddd

dd

Sum-rules link S(q) and (q)

)()(),( qqSqS

The dynamic spin correlation function obeys sum-rules:

Page 24: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Single mode approximation for spin-1 chain

Dispersion relation

Equal time correlation function

Page 25: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Haldane mode in Y2BaNiO5 at finite T

•Relaxation rate increases with T due to triplet interactions

•Resonance energy increases with T due to decreasing correlation length

Low T fine structure from spin anisotropy

Page 26: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Q-scans versus T: energy resolved and energy

integrated

Probing spatialcoherence of Haldane mode

Probing equal time correlation length

Page 27: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Pure quantum spin chains- at zero and finite T

Gap is possible when n(S-m) is integer gapped systems: alternating spin-1/2 chain, integer chain,…

gapless systems: uniform spin-1/2 chain

gapped spin systems have coherent collective mode

For appreciable gap SMA applies: S(q) ~ 1/(q)

Thermally activated relaxation due to triplet interactions

Thermally activated increase in resonance energy

Coherence length exceeds correlation length for T< /kB

Page 28: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Impurities in Y2BaNiO5

Ca2+

Y3+

• Mg2+on Ni2+ sites finite length chains• Ca2+ on Y3+ sites mobile bond defectsMg

Ni

Kojima et al. (1995)

Page 29: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Zeeman resonance of chain-end spinsI(

H=

9 T

)-I(

H=

0 T

) (

cts.

per

min

.)

Hg B

h (

meV

)

H (Tesla)0 2 4 6 8

g=2.16

0 0.5 1 1.5 2

-5

0

10

15

20

Hg B

meV)(

Page 30: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Form factor of chain-end spins

Q-dependence revealsthat resonating objectis AFM.

The peak resemblesS(Q) for pure system.

Chain end spin carryAFM spin polarizationof length back into chain

Y2BaNi1-xMgxO5 x=4% Hg B

Page 31: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

New excitations in Ca-doped Y2BaNiO5

Pure 9.5% Ca

•Ca-doping creates states below the gap

•sub-gap states have doubly peaked structure factor

Y2-xCaxBaNiO5:

Page 32: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Why a double ridge below the gap in Y2-xCaxBaNiO5 ?

Charge ordering yields incommensurate spin order

Quasi-particle Quasi-hole pair excitations in Luttinger liquid

Anomalous form factor for independent spin degrees of freedom associated with each donated hole

xq

q is single impurity prop.Indep. of

x

Page 33: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Does q vary with calcium concentration?

q not strongly dependent on x

Double peak is single impurity effect

Page 34: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

(b)

Ca

Ba

Ni

Y

c

b

a

(e)

(f)

(c)

(d)

a

O

Bond Impurities in a spin-1 chain: Y2-

xCaxBaNiO5

(a)

Page 35: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Form-factor for FM-coupled chain-end spins

2/)(Re2)( iqeqMqS

A symmetric AFM droplet

22/*2/ )()()(

ll

iql

iqlll eqMeqMPqS

Ensemble of independent randomly truncated AFM droplets

Page 36: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Calcium doping Y2BaNiO5

Experimental facts:Ca doping creates sub-gap excitations with

doubly peaked structure factor and bandwidth The structure factor is insensitive to

concentration and temperature for 0.04<x<0.14 (and T<100 K)

Analysis:Ca2+ creates FM impurity bonds which nucleate AFM droplets with doubly peaked structure factorAFM droplets interact through intervening chain

forming disordered random bond 1D magnet

Page 37: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

What sets energy scale for sub gap scattering ?

0

5

10

Possibilities:

•Residual spin interactions through Haldane state. A Random bond AFM.

•Hole motion induces additional interaction between static AFM droplets

•AFM droplets move with holes: scattering from a Luttinger liquid of holes.

How to distinguish:

• Neutron scattering in an applied field

• Transport measurements

• Theory

?

q~

h

(meV

)

Page 38: Holes in a Quantum Spin Liquid Gapped phases in condensed matter Gapped spin chains Pure systems Doped systems Conclusions Collin Broholm Johns Hopkins

Canada 4/12-13/00

Conclusions: Dilute impurities in the Haldane spin chain create sub-

gap composite spin degrees of freedom. Edge states have an AFM wave function that extends

into the bulk over distances of order the Haldane length. Holes in Y2-xCaxBaNiO5 are surrounded by AFM spin

polaron with central phase shift of

Neutron scattering can detect the structure of composite impurity spins in gapped quantum magnets.

The technique may be applicable to probe impurities in other gapped systems eg. high TC superconductors.

Microscopic details of gapped spin systems may help understand related systems where there is no direct info.

Viewgraphs posted at http://www.pha.jhu.edu/~broholm/canada/index.htm