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quantum magnetism

Radu Coldea

Oxford

Outline

- principles of (magnetic) neutron scattering

- spin waves in a Heisenberg ferromagnet

- spin waves in square-lattice AFM La2CuO4

Hamiltonian triangular AFM S = 1/2 Cs2CuCl4

- quantum phase transition in the Ising chain CoNb2O6 in

transverse field

Neutron reactors

(Institute Laue Langevin)

ki

kf

Q

ki kf = Q

Ei Ef = E

neutron

guide

spectrometers

Clifford

Shull

Bertram

Brockhouse

- evaporation when fast protons

hit a heavy nucleus (Ta)

proton synchrotron

accelerator ~800MeV

p+

neutron

guide

time-of-flight

spectrometer

LET@ISIS

count simultaneously (timestamp each arriving neutron

Neutrons have

- no charge

- spin-1/2 moment

kf

ki

dipole moment M

t

=> magnetic Bragg peaks

at Q = t q

magnetic

unit cell

- Intensity ~

Fourier transform of magnetic

moment density (perp to

scattering wavevector Q)

structural

Bragg peak t

magnetic

kf

ki

sample

excited

state

ground state

Fourier transform of magnetic

moment density M a

Fourier transform of

magnetic e- density

polarization factor

La2CuO4

Cs2CuCl4

(solution growth)

CoNb2O6

(mirror furnace growth)

4 cm

2.5 cm

(flux growth)

H = - Jij SiSj if all Jij > 0 T=0 ground state is

ij

S-

magnon

energy

(q) = -J(q)

(0) +- J(0) + h

1

iqrij

2

Fourier transform

of magnetic couplings

J(q) = _ ijJij e

ij

i

ij

ij 2

hopping

(if Hamiltonian conservs Sz)

magnon

manifold

S-

exact

result

Zeeman

energy

Wavevector (q)

(q)

Energy

Gap

0

|q> =

e iqr |

1

N i

i>

scattered

incident

neutron

ki

kf

S z = + 1/2

S z = -1/2

Magnon

k

ki - kf = k

Ei - Ef = w(k)

Wavevector k

L (rlu)

Sz = -1

Ground state has Neel order

(<S> reduced by quantum fluctuations)

J antiferromagnetic

(approximate eigenstates)

La2CuO4

Magnetic Bragg peak (1/2,1/2,0)

- insulating parent of

high-TC cuprates

- square-lattice of CuO2

planes, Cu2+ S=1/2

Keimer at al, PRB (1992)

ki

S=1

magnon

kf

RC et al, PRL 86, 5377 (2001)

Collect maps of magnetic scattering in the whole

2D Brillouin zone (h,k) at increasing energies E

Energy

325 meV

275 meV

75 meV

RC et al, PRL 86, 5377 (2001)

Dispersion relations

La2CuO4, T=293 K

Antiferromagnetic

Bragg peak

position

RC et al, PRL 86, 5377 (2001)

- dispersion shape is a direct fingerprint of the magnetic interactions

for a cyclic-exchange between the 4 spins on a

plaquette in addition to the main exchange J

Expand up to 4

electron hops

A.H. MacDonald (1990),

Takahashi (1977)

- dispersions and intensities

well described by linear spinwave theory

t = 0.30(2) eV, U = 2.2 (4) eV

U/t = 7.3 1.3 (10 K)

Intensity renormalization factor

Zc = 0.51 +/- 0.13 (predicted 0.61)

- sharp spin-wave mode only very small

weight

strongly-dispersive boundaries

=> Quantum fluctuations very strong, spinwave theory inadequate

1.5

1.25

(0,0.5,l)

Intensity (a.u.)

J'

0.1

0.2

E (meV)

0.8

0

0.0

0.2

0.4

0.6

Energy (meV)

0.8

1.0

1.2

via spin waves in the fully-polarized state in high field

RC et al, PRL 88,137203 (2002)

B=0

B >> J

J antiferromagnetic

Fully-polarized

state

State with AF

correlations

BC

Magnetically

ordered, spin

liquid etc.

gapped

magnons

Applied

Field

Exact eigenstate if

Hamiltonian

conserves Sz

Bose condensation

of magnons at Bc

transform of exchange

couplings

(k) = J (k) - J (0) + h

J (k) = 1

S Jd

2 d

exp( i k d)

T=60 mK

1.0

0.8

Bc = 8.42 T

0.6

0.4

0.2

Magnetization ()

0.4

0.3

30

0.2

0.1

20

0.0

10

0.0

magnon excitations

T=60 mK

10

0

Field // a (Tesla)

10

0.4

Field // a (Tesla)

(021)

2.0

1.5

0.5

0.6

Energy (meV)

(010)

(020)

1.0

0.0

0.5

(021)

[0,2,l]

[0,,-1]

1.5

Energy (meV)

(0,1.447,0)

1.0

1.0

Fourier transform of

couplings J(q)

J=0.374(5) meV

J=0.128(5) meV

_J ~ _1

J

3

J'

0.5

2D Hamiltonian

B = 12 T || a

T < 0.2 K

0.0

1.0

1.5

[0,k,0]

RC et al, PRL 88,137203 (2002)

2.0

J= 0.017(2) meV

interlayer coupling

Da = 0.020(0) meV DM anisotropy _| bc plane

B<Bc

B=Bc

B>Bc

magnon

dispersion

Gap

B (T) || a

4

12

0)

2

0

(

(a)

1.25

1.5

0)

1

(0

1.00

1.0

+

)

1

7,

4

4

.

(0,

)

1

7,

4

4

.

(0,

0.75

0.50

0.25

0.00

Peak intensity

(arb. units)

10

(b) CONE

0.04

FERRO

0.03

0.02

0.5

where the gap closes

D

150

0.0

1.00 1.25 1.50 1.75 2.00

[0,k,0]

Intensity a.u.)

Energy (meV)

1.50

Energy (meV)

B > Bc

B < Bc

100

50

0.01

0.00

0

B (T) || a

10

12

0

1.40

1.45

K (rlu)

1.50

Energy (meV)

(000)

Alternating layers

counter-rotate

+D

1.0

-D

0.5

-Q

Sense

selected by

DM couplings

+Q

0.0

-0.5

0.0

0.5

[0 k 0]

D(Si x Sj)

2 condensates at

+Q and -Q

1.6

1.0

1.4

1.2

0.5

1.0

0.0

1.00 1.25 1.50 1.75 2.00

B (T) || a

[0,k,0]

magnon wavefunctions

Energy (meV)

Asymmetry <Sb>/<Sc>

1.5

B=Bc

Incommensuration

(2/b)

Q

B<Bc

mean-field

result

0.05

Bc= 8.44(1)T

c=0.0536(5)

0.04

(0,1.5-,0)

(0,0.5-,1)

0.03

0.02

0

10

Strong quantum

renormalization

20 e0/ecl=0.56

Energy

Collinear

spins

RC et al, PRL 88,137203 (2002)

10

B (T) || a

Wave

vector k

Quantum Classical

Spin-1/2 instability

large-S

12

into pairs of S=1/2 spinons

J'

S=1/2

Spinons

J'

La2CuO4

spiral order coexisting with strong quantum fluctuations

- renormalization of Q-vector and zone-boundary energy

measured by quenching quantum fluctuations via field and

revealing classical behaviour

- dominant continuum scattering (spin-waves fractionalize

into pairs of spinons)

Headings, Hayden, RC , PRL (2010)

Classical

thermally-driven

continuous phase

transition

z

H = - J Si z S j +

i,j

<Sz>

0

<Sz>

quantum fluctuations

add transverse field

- B Sx

quantum tunneling

- B (S++S-) / 2

TC

Temperature

Quantum fluctuations

driven continuous

phase transition

BC

B field

z

H = - J Si Si+1 +- B S ix

i

T

TC

Quantum

paramagnet

Ferromagnet

0

z

- transverse field

- B Sx = - B (S++S-) / 2

generates quantum fluctuations

that melt the spontaneous

magnetic order at BC ~ J/2

BC

Ordered

moment

Field

x

Magnetization

and opportunities

Temperature

Critical

Phase 2

Phase 1

BC

Tuning

parameter

quantum fluctuations that drive transition ?

- how quasiparticles evolve near critical point ?

- what are the fundamental symmetries that govern physics of QCP ?

- what are finite-T properties (interplay of thermal and quantum

fluctuations, under what conditions universal scaling ?

z

i

flips spins

Bx

=> propagating solitons

(Jordan Wigner fermions)

classical soliton

(large-S limit)

Gap D

Ferromagnet

solitons

BC

Quantum

paramagnet

spin-flip

quasiparticle

gapless linear (Dirac) spectrum

w = c|k|

for critical solitons

- different universality class from Luttinger liquids (1D Heisenberg and XY

AFM chains)

Experimental requirements

1) good 1D character to see solitons

2) low-exchange J ~ 1 meV to access critical field BC ~ J/2 < 10 T

3) strong uniaxial anisotropy (Ising character) but not perfect to still

have transverse g-factor

l LS

Strong Crystal field + Spin Orbit

lowest Kramers doublet effective spin-1/2 Ising-like

2D Ising AF

1D Ising AF

CsCoCl3 (Goff 95) also CsCoBr3 (Nagler)

J ~ 12 meV BC > 50 T not accessible

Oxygen

Ferromagnetic

superexchange

~ 90 bond Co-O-Co

~ 20K ~ 2meV

Strong easy-axis (Ising) in ac plane

Single crystal

of CoNb2O6

(Oxford

image

furnace)

Co2+

4 cm

T= 5 K, 1D phase above TN

neutron scattering

k1

incident

scattered

2-soliton excitations

RC et al, Science 327, 177 (2010)

k2

k1

k2

TC

ordered

T= 5 K, 1D phase above TN

1D phase

3D phase

+ sharp modes (bound states)

RC et al, Science 327, 177 (2010)

BC

no measurable dispersion chains

|| chain direction

H=-2.5

H=-2.0

H=-1.5

0.4

0.3

0.2

0.1

0

1.1

chain direction

1.2

1.3

1.4

Energy (meV)

1.5

T=5K

T =40 mK

0.04 K

5K

1

0.3

L = 0.00(5)

2

0.2

3

4

0.1

0.0

1.0

1.2

1.4

1.6

Energy (meV)

Continuum of

Bound states in

free 2-soliton

confining potential

states

E

2

1

x x x x

Soliton separation

costs energy

V(x) = l x

l ~ J Sz

T=5K

T =40 mK

0.04 K

5K

1

0.3

L = 0.00(5)

2

0.2

3

4

0.1

0.0

1.0

1.2

1.4

1.6

Energy (meV)

Continuum of

Bound states in

free 2-soliton

confining potential

states

E

2

1

x x x x x

Soliton separation

costs energy

V(x) = l x

l ~ J Sz

T=5K

T =40 mK

0.04 K

5K

1

0.3

L = 0.00(5)

2

0.2

3

4

0.1

0.0

1.0

1.2

1.4

1.6

Energy (meV)

Continuum of

Bound states in

free 2-soliton

confining potential

states

E

2

1

x x x x x x

Soliton separation

costs energy

V(x) = l x

l ~ J Sz

Soliton confinement

0.04 K

5K

McCoy&Wu (78)

Schrdingers equation

1

0.3

L = 0.00(5)

2

0.2

3

4

0.1

0.0

kinetic energy

string tension

Ai(z)

0.5

-0.5

-10

-5

Airy function

zn = 2.33, 4.08, 5.52, 6.78

1.0

1.2

1.4

Energy (meV)

1.6

- work perturbatively around the Ising limit

(spin clusters)

J

2-soliton states

=J

-a

-b d n,1

a 2 soliton state

z

gap

from Ising J Siz Si+1

+

i+1

soliton hopping

from XY term

i-1

x + Sy Sy

+ S- + S - S+

- Jxy ( Six Si+1

)

~

S

i i+1

i i+1 i i+1

T = 40 mK

Gap:

J ~ 1.94 meV

Bandwidth

[ microscopic origin SzSx ?]

Kinetic bound state : transverse couplings for nn bond SxSx + SySy , J / J z = 0.24

and 2-nd neighbour AFM along chain J z' = - 0.15 J z

Weak confinement term: hz ~ 0.02 J longitudinal field includes interchain mean-field

S.B. Rutkevich, J. Stat. Phys (2010)

0T

4T

Energy

3.25 T

Gap decreases

with field

B

t

torque

wavevector

CoNb2O6

crystal

prevent movement under high torque

BxSx = (S++S-)/2

4T

6T

Magnetic 3D LRO

Bragg peak

Two-soliton states

Ordered

Single sharp

mode

Paramagnetic

1000

Excitations change

character above

critical field

800

Intensity (a.u.)

7T

600

400

200

0

0.5

1.0

1.5

Energy(meV)

2.0

Excitations in

transverse field

2-soliton continuum

RC et al, Science 327, 177 (2010)

Summary

- realized experimentally field-tuned quantum phase transition in

quasi 1D Ising magnet CoNb2O6

- observed transmutation of quasiparticles at critical point

ordered

paramagnet

2-soliton

states

spin-flip

Conclusions

- neutron scattering is a very versatile probe of magnetic ordering and

dynamics (meV->eV, magnetic field (15 T->25 T), low T (mK)

- quantitative: probe dispersions of excitations through wellunderstood matrix element (quantitative comparison with theories)

- sample size limited, large crystals needed (advanced crystal growth)

- new neutron sources (ISIS 2nd target station, USA + JAPAN, ESS) will

bring new opportunities: higher flux, higher resolution, wider coverage

50 detectors,

2D data set

40,000 detectors,

4D data set, 4

energies measured

simultaneously,

(samples 10s of mm, resolution >30 meV, T > few K beam heating)

Collaborators

La2CuO4

CoNb2O6

G. Aeppli (UCL)

T.G. Perring(ISIS)

C.D. Frost (ISIS)

T.E. Mason (Oak Ridge)

M. Telling (ISIS)

Z. Fisk (Florida)

D. Prabhakaran (Oxford)

Cs2CuCl4

D. A. Tennant (HZB)

A.M. Tsvelik (Brookhaven)

Jordan Thompson (Oxford)

R. Bewley, T. Guidi (ISIS)

Z. Tylczynski (Poland)

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