IRIDATES Bill Flaherty Materials 286K, UCSB Dec. 8 th, 2014.

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Presentation transcript:

IRIDATES Bill Flaherty Materials 286K, UCSB Dec. 8 th, 2014

5D TRANSITION METALS: UNINTERESTING? “The properties of the 4d and 5d compounds tend to be less exotic” – Mattheiss, d transition metal oxides: localized states  Strong correlations  Narrow bands, large U/W 4d, 5d: spatially extended states  Wide bandwidth  Low on-site repulsion, smaller U/W  Predicted to be metallic, ferromagnetic

DISCOVERY OF “MORE EXOTIC” 4D, 5D TMO S Sr 2 IrO 4 - M. K. Crawford et al., Phys. Rev. B 49, 9198 (1994). Sr 2 IrO 4, Sr 2 RuO 4 - R. J. Cava et al., Phys. Rev. B 49, (1994) Ca 2-x Sr x RuO 4 - S. Nakatsuji and Y. Maeno, Phys. Rev. Lett. 84, 2666 (2000) Cd 2 Os 2 O 7 - D. Mandrus et al., Phys. Rev. B 63, (2001). Y, Ca, Sr, Bi Ruthenates - J. S. Lee et al., Phys. Rev. B 64, (2001).

SR-214 BAND STRUCTURE Sr 2 (2+) Ir (4+) O 4 Ir (4+) : 5d 5 system

SR-214: CORRECT BAND STRUCTURE Spin-Orbit Coupling (SOC) t 2g states → l = 1 states Strong SOC: t 2g splits into J eff = 3/2 and 1/2 Narrow Jeff = ½ band due to hopping integrals Novel J eff = 1/2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr 2 IrO 4 B. J. Kim et al., Phys. Rev. Lett 101, (2008)

OBSERVATION OF U + SOC ARPES, Optical Conductivity, XAS experiments DFT calculations (LDA, LDA + U) Novel Jeff = 1/2 Mott State Induced by Relativistic Spin-Orbit Coupling in Sr 2 IrO 4 B. J. Kim et al., Phys. Rev. Lett 101, (2008)

RESONANT X-RAY STUDIES Resonant X-ray Spectroscopy Contains information from quantum interference of different scattering paths Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr 2 IrO 4 B. J. Kim et al., Science 323, 1329 (2009)

PHASE-SENSITIVE MEASUREMENTS J eff = ½ states – linear combinations of xy, yz, zx that differ in phase No phase difference for simple t 2g states (real wave fns.) Scattering amplitudes depend on phase differences between states → Test J eff = ½ model vs. S = ½ Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr 2 IrO 4 B. J. Kim et al., Science 323, 1329 (2009)

RESULTS Phase-Sensitive Observation of a Spin-Orbital Mott State in Sr 2 IrO 4 B. J. Kim et al., Science 323, 1329 (2009)

TUNING THE I.-M.T. WITH STRUCTURE How can we tune U/W ? Bandwidth depends on number of Ir nearest neighbors Grow different Ruddelsden-Popper phases to change W and tune U/W

RUDDELSDEN-POPPER PHASES Sr n+1 Ir n O 3n+1 n = 1 Sr 2 IrO 4 four nearest neighbors n = 2 Sr 3 Ir 2 O 7 five nearest neighbors n → infinity SrIrO 3 (Perovskite on MgO substrate) six nearest neighbors Figure from D. A. Zocco et al., J. Phys.: Condens. Matter 26, (2014)

RESULTS – LDA + U Insulating Sr 2 IrO 4 Barely Insulating Sr 3 Ir 2 O 7 Correlated Metal SrIrO 3 U = 2 eV U typically much larger for a Mott Ins, 4-7 eV S. J. Moon et al., Phys. Rev. Lett. 101, (2008)

RESULTS Optical Conductivity S. J. Moon et al., Phys. Rev. Lett. 101, (2008)

TOPOLOGICAL MOTT INSULATORS SOC scales by atomic number as Z 4 Hg and Bi – strong SOC, weak correlation (s- and p-states)

TOPOLOGICAL INSULATORS Bulk is insulating Conducting surface states Robust against defects  topologically protected states Potential uses for quantum computing  Unusual particle statistics – Dirac fermions (SmB 6 – 2014)  Delocalized states resistant against decoherence

PYROCHLORE IRIDATES A 2 (3+) Ir 2 (4+) O 7 Spinons, quantum criticality TBI – Topological Band Ins GMI – Gapless Mott Ins TMI – Topological Mott Ins  Charge-spin separation  Spinons – gapless spin excitations  Insulating surface states