impurities and finite temperature effects in a one-dimensional spin-1 antiferromagnet coherent...

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dimensional spin-1 antiferromagnet Coherent excitations in Y 2 BaNiO 5 Loss of coherence for T>0 Chain-end spins in Y 2 BaNi 1-x Mg x O 5 AFM droplets in Y 2-x Ca x BaNiO 5 Conclusion Collin Broholm Hopkins University and NIST Center for Neutron Rese upported by the NSF through DMR-9453362

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Impurities and finite temperature effects in a one-dimensional spin-1

antiferromagnet

Coherent excitations in Y2BaNiO5

Loss of coherence for T>0 Chain-end spins in Y2BaNi1-xMgxO5

AFM droplets in Y2-xCaxBaNiO5

Conclusion

Collin BroholmJohns Hopkins University and NIST Center for Neutron Research

Supported by the NSF through DMR-9453362

CURREAC 8/20/99

Collaborators

Guangyong 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 NEC

Experiments performed at NIST and ISIS

CURREAC 8/20/99

Why does spin-1 AFM have a spin gap?

• For integer spin chains (S=n, z=2) this state is “close to” the ground state

• Magnets with 2S=nz have a nearest neighbor singlet covering.

• 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

CURREAC 8/20/99

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

Y2 B

aN

iO5

on

SPIN

SE

<1

0 m

eV

NIS

T co

ld n

eu

tron

gu

ide h

all

ISIS Experimental hall

Y2BaNiO5 on MARI5 meV<E<100 meV

CURREAC 8/20/99

Low T excitations in spin-1 AFM chain

Y2BaNiO5 T=10 KMARI chain ki

Points of interest:

•Haldane gap =8 meV

•Coherent mode

•S(q,)->0 for Q->2n

CURREAC 8/20/99

Probing anisotropy and inter-chain coupling in Y2BaNiO5

in

ten

sity

(co

utn

s p

er

15

min

.)

I(q

,w)

(1/m

eV

)

a b c Maintaining , we

•Derive polarization by rotating about chain

•Look for inter-chain coupling by varying

aQ

||

Q

Q

Weak anisotropy:

%10/ Highly one dimensional

4105' JJ

CURREAC 8/20/99

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

Then sum-rules link S(q) and (q)

)()(),( qqSqS

The dynamic spin correlation function obeys sum-rules:

CURREAC 8/20/99

Propagating triplet in alternating spin-1/2 chain Cu(NO3)2

.2.5D2O

The “incommensurate” size of spin dimers yields different periods fordispersion relation and structure factor. An effect captured by the

SMA.

IRIS data SMA model

0 2 4 0 2 4 6

h

(meV

)

0.4

0.5

Q/

CURREAC 8/20/99

Two magnon excitations in an alternating spin chain

Tennant, Nagler, Xu, Broholm, and Reich.

CURREAC 8/20/99

Haldane mode in Y2BaNiO5 at finite T

Effects of heating:

• Line-width increases

• Effective increases

CURREAC 8/20/99

T-dependence of relaxation rate and “resonance” energy

Parameter free comparison:

•Semi-classical theory of triplet scattering by Damle and Sachdev

•Quantum non linear model

Tk

TkT

B

B 0exp3

Tk

TkTB

B0

00 exp2

Derived from

Tc

T

0)(

Neglecting T-dependence of spin wave velocity c0

CURREAC 8/20/99

Q-scans versus T: energy resolved and energy

integrated

Probing spatialcoherence of Haldane mode

Probing equal time correlation length

CURREAC 8/20/99

Coherence and correlation lengths versus T

Equal-time correlation length saturates at =8.

Coherence length exceeds correlationlength for kBT<becoming very longas T 0

(Solid line from Quantum non linear model)

CURREAC 8/20/99

Properties of pure Y2BaNiO5

Anisotropy split Haldane gap: a=7.5 meV, b=8.6 meV, c=9.5 meVNo inter-chain coupling detected: |J’/J|<5.10-4

Coherent mode described by SMA for T<</kB

Activated relaxation rate of q= mode is described by semi-classical theory of interacting triplet wave packets.

Activated increase in resonance energy is significantly less than predicted by Qnl-model

Coherence length exceeds correlation length for T< /kB and exceeds 40 lattice spacings for kBT/=0.1

CURREAC 8/20/99

Effects of finite chain length on Haldane mode

•Mode shifts towards J as in numerical work on finite length chains

•Peak Broadens because of chain length distribution

4% Mg

Pure

q= T=10 K

CURREAC 8/20/99

Zeeman resonance of chain-end spins

I(H

=9 T

)-I(

H=

0 T

) (

cts.

per

min

.)

h (meV)

Hg B

h

(m

eV

)

H (Tesla)0 2 4 6 8

g=2.16

0 0.5 1 1.5 2

-5

0

10

15

20

Hg B

CURREAC 8/20/99

Structure factor of chain-end spins

Q-dependence revealsthat resonating objectis AFM.

The structure factoris indistinguishablefrom S(Q) for puresystem.

Chain end spin carryAFM spin polarizationof length back into chain

CURREAC 8/20/99

Vacancy doping a Haldane spin chain

q= mode shifts towards Jq= mode broadens due to random

chain length distributionApplied field induces Zeeman

resonance below Haldane gapResonating chain end spins have

AFM form factor resembling S(q) for pure system.

CURREAC 8/20/99

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:

CURREAC 8/20/99

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

Charge ordering yields incommensurate spin order

Quasi-particle Quasi-hole pair excitations in a one dimensional hole liquid

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

xq

q is single impurity prop.Indep. of

x

CURREAC 8/20/99

Does q vary with calcium concentration?

q is independent of

Double peak is predominantly asingle impurity effect

9.5% Ca

14% Ca

q

14.0;095.0x

CURREAC 8/20/99

(b)

Ca

Ba

Ni

Y

c

b

a

(e)

(f)

(c)

(d)

a

O

Bond Impurities in a spin-1 chain: Y2-

xCaxBaNiO5

(a)

CURREAC 8/20/99

Form-factor for FM-coupled chain-end spins- AFM droplets

9.5% Ca

14% Ca

2/)(Re2)( iqeqMqS

A symmetric AFM droplet

22/*2/ )()()(

ll

iql

iqlll eqMeqMPqS

Ensemble of independent randomly truncated AFM droplets

CURREAC 8/20/99

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 0.095<x<0.14 and T<100 K

Current interpretation: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

CURREAC 8/20/99

Broader Conclusions:

Dilute impurities in the Haldane spin chain create sub-gap composite spin degrees of freedom.

Composite spins have an AFM wave function that extends into the bulk over distances of order the Haldane length.

Neutron scattering can detect the structure of composite impurity spins in quantum magnets when the corresponding states exist at energies where the bulk magnetic density of states vanishes.