magnetic order refinement in high field

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Probing Matter with X-Rays and Probing Matter with X-Rays and Neutrons Tallahassee, May 10- Neutrons Tallahassee, May 10- 12, 2005 12, 2005 Magnetic order refinement in high Magnetic order refinement in high field field Outline Outline Magnetic field as a source of Luttinger liquid alternate route to “quantum” criticality Enhancing weak antiferromagnetism in coupled Haldane chains Magnetic order refinement in high field: challenges and caveats Igor Zaliznyak Igor Zaliznyak Neutron Scattering Group, Brookhaven National Laboratory

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Magnetic order refinement in high field. Igor Zaliznyak Neutron Scattering Group, Brookhaven National Laboratory. Outline Magnetic field as a source of Luttinger liquid alternate route to “quantum” criticality Enhancing weak antiferromagnetism in coupled Haldane chains - PowerPoint PPT Presentation

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Page 1: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Magnetic order refinement in high field Magnetic order refinement in high field

OutlineOutline

• Magnetic field as a source of Luttinger liquid

– alternate route to “quantum” criticality

• Enhancing weak antiferromagnetism in coupled Haldane chains

• Magnetic order refinement in high field: challenges and caveats

Igor ZaliznyakIgor Zaliznyak

Neutron Scattering Group, Brookhaven National Laboratory

Page 2: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Haldane chain in magnetic field.Haldane chain in magnetic field.3,5,…-particle continuum

3,5,…-particle continuum

H=0 H~Hc

H>Hc

?particles

holesparticles

Macroscopic quantum phase in the string operator at H>Hc results in the shift in q-space between fermions and magnons.

Haldane (Quantum) Critical

Luttinger Liquid

Page 3: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Haldane chain in magnetic field.Haldane chain in magnetic field.

L.P. Regnault, I. Zaliznyak, J.P. Renard, C. Vettier, PRB 50, 9174 (1994).

Luttinger Liquid

Page 4: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Coupled Haldane chains in (Cs,Rb)NiClCoupled Haldane chains in (Cs,Rb)NiCl33: weak : weak

antiferromagnetic order in zero fieldantiferromagnetic order in zero field

CsNiClCsNiCl33::J = 2.3 meV = 26 K J = 0.03 meV = 0.37 K = 0.014 JD = 0.002 meV = 0.023 K = 0.0009 J3D magnetic order below TN = 4.84 K

<<> > ≈ 1≈ 1BB

Page 5: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Coupled Haldane chains in (Cs,Rb)NiClCoupled Haldane chains in (Cs,Rb)NiCl33 in in

magnetic fieldmagnetic field

Field along easy axis: spin-flop + increase in magnetic order

Field perpendicular to easy axis: no spin-flop, just increase in magnetic order

Page 6: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Coupled Haldane chains: magnetic field enhances Coupled Haldane chains: magnetic field enhances antiferromagnetic order. antiferromagnetic order.

Hc

Spin-flop

Page 7: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Measuring the field dependence of magnetic Measuring the field dependence of magnetic Bragg peaks: challenges and caveats.Bragg peaks: challenges and caveats.

• Equivalent “Friedel” reflections have different intensities– non-uniform illumination of absorbing sample is a source of the

dominant systematic error– sample/wavelength optimization is vital

• Realignment of spins in the spin-flop process greatly impacts intensities– very sensitive to magnetic field orientation with respect to

crystallographic “easy” axis– sensitive to sample mosaicity– different bias for different reflections

Page 8: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Spin-flop is nothing new and is well understoodSpin-flop is nothing new and is well understood

J. W. Lynn, P. Heller, N. A. Lurie, PRB 16 (1977).

• ψ is misalignment of the magnetic field from the easy axis• φ is corresponding misalignment of staggered magnetization

• Eq. (14) is a venerable expression with long history dating back to L. Neel (J. Lynn et. al.)• It also is general: goes beyond simple quasiclassical approximation

Page 9: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Spin realignment: powder in magnetic fieldSpin realignment: powder in magnetic field

Page 10: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Brave attempt: refine on powderBrave attempt: refine on powder

Red:H = 6.8 TBlack:H = 0 T

Red:H = 6.8 TBlack:H = 1 T

Page 11: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

The right way: do the real thingThe right way: do the real thing

15 T magnet on D23 @ ILL(courtesy B. Grenier)

Page 12: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Cavalry approach: just follow the Bragg peaks Cavalry approach: just follow the Bragg peaks

Not satisfactory!

H perpendicular to the easy axis

single-domenization

Page 13: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Full refinement in mangetic field Full refinement in mangetic field

Page 14: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Full refinement in mangetic field Full refinement in mangetic field

Haldane gap in CsNiCl3

Page 15: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Compare to LCO superconductorsCompare to LCO superconductors

B. Khaykovich, Y. S. Lee, et. al., PRB 66 (2002).

E. Demler, S. Sachdev, and Y. Zhang, PRL 87 (2001).

Page 16: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Summary and conclusionsSummary and conclusions

• Magnetic field brings about fascinating new phases

– Luttinger-liquid (quantum) critical state

– tunes antiferromagnetism in weakly ordered systems

• Refining field dependence of magnetic order is a challenging experimental task

– field-dependent variation of intensity is often smaller than systematic (not statistical!) errors

– only one reciprocal lattice (hkl) plane is typically available

– spin realignment is often a complication: serious science requires serious refinement

This work was carried out under Contract DE-AC02-98CH10886, Division of Materials Sciences, US Department of Energy. The work on SPINS was supported by NSF through DMR-9986442

Page 17: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Acknowledgements: thanks go to Acknowledgements: thanks go to

• S. V. Petrov

• B. Grenier and L.-P. Regnault

• R. Erwin and C. Quang

• C. Broholm

• A. Savici

/ U. Maryland/ U. Maryland

Page 18: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

What is quantum spin liquid?What is quantum spin liquid?

• What is liquid?− no shear modulus− no elastic scattering = no static density-density correlation

‹ρq(0)ρ-q(t)› → 0t → ∞• What is quantum liquid?

− all of the above at T → 0 (i.e. at temperatures much lower than interactions between the particles in the system)

• Quantum liquid state for a system of Heisenberg spins

H = J|| SiSi+||+ JSiSi

D(Siz)2

• no static spin correlations

‹Sqα (0)S-

βq (t)› → 0, i.e. ‹Sq

α (0)S-β

q (t)› = 0

• hence, no elastic scattering (e.g. no magnetic Bragg peaks)

t → ∞

J||/J>> 1 (<<1) parameterize quasi-1D (quasi-2D) case

Page 19: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

What would be a “spin solid”What would be a “spin solid”

• Heisenberg antiferromagnet with classical spins, S >> 1S >> 1

− and quasiparticles that are gapless Goldstone magnons

(q) = 2J(S(S+1))1/2sin(q)

(q)

/J/(

S(S

+1)

)1/2

− has Neel-ordered ground state with elastic Bragg scattering at q=π

Page 20: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

1D quantum spin liquid: Haldane spin chain1D quantum spin liquid: Haldane spin chain

− short-range-correlated “spin liquid” Haldane ground state

• Heisenberg antiferromagnetic chain with S = 1S = 1

(q)

/J/(

S(S

+1)

)1/2

− quasiparticles with a gap ≈ 0.4J at q=π

2 (q) = 2 + (cq)2

Quantum Monte-Carlo for 128 spins.

Regnault, Zaliznyak & Meshkov, J. Phys. C (1993)

Page 21: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

weak interaction

2D quantum spin liquid: a lattice of frustrated 2D quantum spin liquid: a lattice of frustrated dimersdimers

M. B. Stone, I. Zaliznyak, et. al. PRB (2001)

(C4H12N2)Cu2Cl6 (PHCC)

− singlet disordered ground state

− gapped triplet spin excitation

strong interaction

Page 22: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

How do neutrons measure quasiparticles.How do neutrons measure quasiparticles.

E , kf f

sam pleE , ki i

Q =k -ki f

E , kf f

sam pleE , ki i

Q =k -ki f

s s

a ) b )

df

df

Typical geometry of a scattering experiment, (a) elastic, (b) inelastic.

M o n o ch ro m a to r

(2 s)

F o cu sin g an a ly ze r

S am p le

D e tec to r

M o n o ch ro m a to r

(2 s)

F o cu sin g an a ly ze r

S am p le

D e tec to r

(a ) (b )

R A

R

L S AL S A

L S DL S D

I. A. Zaliznyak and S.-H. Lee, in Modern Techniques for Characterizing Magnetic Materials, Ed. Y. Zhu, Springer (2005)

Page 23: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Spin-quasiparticles in Haldane chains in CsNiClSpin-quasiparticles in Haldane chains in CsNiCl33

J = 2.3 meV = 26 K J = 0.03 meV = 0.37 K = 0.014 J

D = 0.002 meV = 0.023 K = 0.0009 J

3D magnetic order below TN = 4.84 Kunimportant for high energies

q0 π

Page 24: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Spin-quasiparticles in Haldane chains in CsNiClSpin-quasiparticles in Haldane chains in CsNiCl33

Page 25: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Spectrum termination point in CsNiClSpectrum termination point in CsNiCl33

I. A. Zaliznyak, S.-H. Lee, S. V. Petrov, PRL 017202 (2001)

Page 26: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Quasiparticle spectrum termination line in PHCCQuasiparticle spectrum termination line in PHCC

max{E2-particle (q)}

min{E2-particle (q)}

E1-particle(q)

Spectrum termination line

Page 27: Magnetic order refinement in high field

Probing Matter with X-Rays and Neutrons Probing Matter with X-Rays and Neutrons Tallahassee, May 10-12, 2005 Tallahassee, May 10-12, 2005

Summary and conclusionsSummary and conclusions

• Quasiparticle spectrum termination at E > 2 is a generic property of the quantum Bose (spin) fluids

– observed in the superfluid 4He

– observed in the Haldane spin chains in CsNiCl3

– observed in the 2D frustrated quantum spin liquid in PHCC

• A real physical alternative to the ad-hoc “excitation fractionalization” explanation of scattering continua

• Implications for the high-Tc cuprates: spin gap induces disappearance of the coherent quasiparticles at high E

This work was carried out under Contract DE-AC02-98CH10886, Division of Materials Sciences, US Department of Energy. The work on SPINS was supported by NSF through DMR-9986442