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High Field Electron Spin Resonance at the National Synchrotron Light Source (Brookhaven National Laboratory)

László Mihály

Stony Brook University & BNL National Synchrotron Light Source


Instrument

Quasi-optical detection: Measure transmission/reflection. Quantitative analysis in terms of the complex index of refraction, n=Öem=Öe(1+4pc)

Two major components: Spectrometer and magnet

  • Magnet: Oxford Instruments, 16Tesla, max 37 mm sample size
  • Temperature: 1.3K-300K
  • Spectrometer: Sciencetech, Martin-Puplett, 2cm-1 to 2000cm-1 , 0.01cm-1 resolution, works with internal and external sources
Also important:
  • Coupling to light source
  • Coupling between magnet and spectrometer
  • Sample holder, support structure, safety devices
Synchrotrom source is a must; brightness and absolute intensity advantage are needed to make measurements possible.


Material: LaMnO3

   

ESR at fixed frequencies

  • The resonance line in "pure" LaMnO3 is too broad for Q-band
  • In doped samples spin diffusion leads to motional narrowing, yields narrower line. Paramagnetic state studied in great detail by Oseroff, Muller and others.
  • High field ESR: Mitsudo, Pimenov's group
  • Budapest results: measured 3 frequencies: 75GHz, 150GHz, 225GHz
    • Paramagnetic state: g = 2 (& new lines, strongly temperature dependent)
    • AF state: More complex behavior
   
     

Theory of AF resonance

  • Large body of work in '50s, theory by Keffer, Kittel and others
  • Experiments: Richards, Tinkham, Foner
  • Fields in effective Hamiltonian (uniaxial anisotropy):
    Exchange (He), anisotropy (Ha), external (H0), excitation (Hrf)
  • Zero external field: 
  • Finite external field lifts degeneracy.
    Parallel to easy axis: two branches (circular polarization)

  • Perp to easy axis: one mode is independent of the external field (linear polariztion)

Mapping of H - w plane

  • Sample: Oriented single crystal, ~0.5 mm thick, 4.0mm diameter disk
  • Easy axis is perpendicular to surface (Susceptibility)
  • Incident EM waves perpendicular to surface
  • Measured absorption as a function of frequency at many fields; convert to map
  • Paramagnetic state: linear relationship, as for quasi-free spins
  • AF state
  • Temperature dependence

Material: La2CuO4

  • Parent compound of high Tc materials
  • CuO2 layered structure
  • Copper ions have localized spins, antiferromagnetic below ~120K
  • AF resonance has not been detected
  • Preliminary results on "powder" samples

Material: NaNiO2

  • Frustrated antiferromagnet
  • High temperature structure: rhombohedral, with triangular Ni lattice
  • Ni3+ ions in t62ge1g configuration
  • Cooperative JT distortion at 475K; becomes monoclinic
  • Magnetic order at 20K (Magnetization only - no evidence from neutrons)
  • H - w mapping was done on a powder sample
  • Next: LaNiO2, with no known JT distortion

Summary