Title: Inhomogeneous Level Splitting in PrxBi2xRu2O7
1Inhomogeneous Level Splitting in PrxBi2-xRu2O7
- Collin Broholm and Joost van Duijn
- Department of Physics and Astronomy
- Johns Hopkins University
2Collaborators
- Ruthenium pyrochlores
- K. H. Kim Rutgers
- N. Hur Rutgers
- D. Adroja ISIS
- Q. Huang NIST
- S.-W. Cheong Rutgers
- T. G. Perring ISIS
- Iridium pyrochlores
- Satoru Nakatsuji Kyoto
- Yo Machida Kyoto
- Yoshiteru Maeno Kyoto
- Toshiro Sakakibara ISSP
- Takashi Tayama ISSP
3Outline
- Introduction
- Bulk properties of 4dn and 5dn pyrochlores
- Spin correlations on TM sites
- Crystal field excitations on RE sites
- Level splitting in PrxBi2-xRu2O7
- Ground state doublet spin dynamics
- Model of inhomogeneous level splitting
- Discussion and Conclusions
- Possible relevance for other non-Kramers doublet
systems
4The pyrochlore structure A2B2O7
- A and B sites on vertices of corner-sharing
tetrahedra - A3 site is trivalent RE with 8-fold O2-
coordination - B4 site is tetravalent TM with 6-fold O2-
coordination - Can have both A3 and B4 magnetism
Nearest neighbor exchange selects a manifold of
states characterized by Zero-spin tetrahedra
5BRu site magnetism of Y2Ru2O7
Taira et al. (2000)
Taira et al. (1999)
- Neutron Diffraction reveals long range magnetic
order - ZFC/FC hysteresis suggests some form of disorder
that produces - glassy canted AFM
6Strong Coupling Transition in Y2Ru2O7
T90 K
7PM and AFM Spin Fluctuations
- Phase Transition pushes significant spectral
weight into resonance - The Q-dependence of scattering reflects the form
factor for AFM - cluster degrees of freedom
82 Magnetic Ions 2 Phase Transitions
R2Ru2O7
Er2Ru2O7
Pr3
M. Ito et al. (2001)
Yb3
N. Taira et al. (2003)
9Metal Insulator Transition
- Bi-doping increase bandwidth causing Mott Hubbard
MIT - Magnet order is found only in the insulating
state - Electronic DOS at EF is enhanced close to the MIT
Yoshii and Sato (1999)
10A Highly Entropic Metallic State
K. H. Kim et al.
11Praseodymium Crystal Field levels
116 meV
105 meV
5 K
Pr1.2Bi0.8Ru2O7
85 meV
50 meV
200 K
10 meV
0
Five transitions from GS implies it is doublet
12Fluctuations in metallic Pr1.2Bi0.8Ru2O7
13Inhomogeneous Level Splitting
- Broad Spectrum unchanged
- Upon heating to
- Wave vector dependence
- Follows Pr form factor2
Neutron Scattering measures the level splitting
spectrum
14Inhomogeneous two level system
- The level distribution function
- Singlet-singlet susceptibility
- Sample averaged susceptibility
- Fluctuation-dissipation theorem yields
15Data Collapse Confirms quenched broadening
16Specific heat of r(D)-split doublet
17Susceptibility of r(D)-split doublet
For gapless spectrum low T limiting form is lnT
18Clues to origins of level splitting
- T-independent distribution function r(D)
- Static not dynamic phenomenon
- Continuous not discrete spectrum
- Large rare defect or density wave producing
distribution of environments - Same distribution describes all xlt1.2
- Distribution may not come from Bi doping
- Magnetic field enters in quadrature
- Electrostatic not magnetostatic inhomogeneity
19Where else might this occur?
- Elements that can have non-Kramers doublet ground
states - Pr3 , Pm3, Sm2, Eu3, Tb3, Ho3, Tm3,
Yb2, and U4 - Nominally cubic and stoichiometric systems may
have clandestine level splitting disorder - Doping effects may be controlled by the induced
level splitting
20Other Materials to Reconsider
- Tb2Ti2O7 A non ordering magnet with mysterious
low energy mode - Ho2Ti2O7 Long range ordered with unusual
thermodynamics - YbBiPt Ultra heavy fermion system with
mysterious low E mode (Robinson et al (1995). - LiHoxY1-xF4 quantum spin glass. Strain induced
level splitting adds an effective transverse
field - TbxY2-xTi2O7 Dilution has added effect of
neutralizing Tb through level splitting
21Metal insulator transition in R2Ir2O7
Yanagishima and Maeno (2001)
Nakatsuji et al.
22Conclusions
- Ir and Ru pyrochlores offer MIT transitions with
frustrated magnetism - Y2Ru2O7 strong coupling transition
- Spectral weight pushed to finite E resonance
- Q-dependence unaffected by ordering
- PrxBi2-xRu2O7 static inhomogeneous distribution
of level splittings - Neutrons T-independent broad spectrum
- C(T)/T broadened Schottky anomaly
- c(T) possible logarithmic divergence at low T
- Watch out for level splitting in non-Kramers
ions, which are not really magnets