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Register a new userPressure-driven collapse of the relativistic electronic ground state in a honeycomb iridate
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James Patrick Clancy
Publication date
2018
fields
Physics
and research's language is
English
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The electronic ground state in many iridate materials is described by a complex wave-function in which spin and orbital angular momenta are entangled due to relativistic spin-orbit coupling (SOC). Such a localized electronic state carries an effective total angular momentum of $J_{eff}=1/2$. In materials with an edge-sharing octahedral crystal structure, such as the honeycomb iridates Li2IrO3 and Na2IrO3, these $J_{eff}=1/2$ moments are expected to be coupled through a special bond-dependent magnetic interaction, which is a necessary condition for the realization of a Kitaev quantum spin liquid. However, this relativistic electron picture is challenged by an alternate description, in which itinerant electrons are confined to a benzene-like hexagon, keeping the system insulating despite the delocalized nature of the electrons. In this quasi-molecular orbital (QMO) picture, the honeycomb iridates are an unlikely choice for a Kitaev spin liquid. Here we show that the honeycomb iridate Li2IrO3 is best described by a $J_{eff}=1/2$ state at ambient pressure, but crosses over into a QMO state under the application of small (~ 0.1 GPa) hydrostatic pressure. This result illustrates that the physics of iridates is extremely rich due to a delicate balance between electronic bandwidth, spin-orbit coupling, crystal field, and electron correlation.
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We report a combined muon spin relaxation/rotation, bulk magnetization, neutron scattering, and transport study of the electronic properties of the pyrochlore iridate Nd2Ir2O7. We observe the onset of strongly hysteretic behavior in the temperature dependent magnetization below 120 K, and an abrupt increase in the temperature dependent resistivity below 8 K. Zero field muon spin relaxation measurements show that the hysteretic magnetization is driven by a transition to a magnetically disordered state, and that below 8 K a complex magnetically ordered ground state sets in, as evidenced by the onset of heavily damped spontaneous muon precession. Our measurements point toward the absence of a true metal-to-insulator phase transition in this material and suggest that Nd2Ir2O7 lies either within or on the metallic side of the boundary of the Dirac semimetal regime within its topological phase diagram.
We report results of our study of a newly synthesized honeycomb iridate NaxIrO3 (0.60 < x < 0.80). Single-crystal NaxIrO3 adopts a honeycomb lattice noticeably without distortions and stacking disorder inherently existent in its sister compound Na2IrO3. The oxidation state of the Ir ion is a mixed valence state resulting from a majority Ir5+(5d4) ion and a minority Ir6+(5d3) ion. NaxIrO3 is a Mott insulator likely with a predominant pseudospin = 1 state. It exhibits an effective moment of 1.1 Bohr Magneton/Ir and a Curie-Weiss temperature of -19 K but with no discernable long-range order above 1 K. The physical behavior below 1 K features two prominent anomalies at Th = 0.9 K and Tl = 0.12 K in both the heat capacity and AC magnetic susceptibility. Intermediate between Th and Tl lies a pronounced temperature linearity of the heat capacity with a large slope of 77 mJ/mole K2, a feature expected for highly correlated metals but not at all for insulators. These results along with comparison drawn with the honeycomb lattices Na2IrO3 and (Na0.2Li0.8)2IrO3 point to an exotic ground state in a proximity to a possible Kitaev spin liquid.
Hyperhoneycomb iridate $beta$-Li$_2$IrO$_3$ is a three-dimensional analogue of two-dimensional honeycomb iridates, such as $alpha$-Li$_2$IrO$_3$, which recently appeared as another playground for the physics of Kitaev-type spin liquid. $beta$-Li$_2$IrO$_3$ shows a non-collinear spiral ordering of spin-orbital-entangled $J_{rm eff}$ = 1/2 moments at low temperature, which is known to be suppressed under a pressure of $sim$2 GPa. With further increase of pressure, a structural transition is observed at $P_{rm S}$ $sim$ 4 GPa at room temperature. Using the neutron powder diffraction technique, the crystal structure in the high-pressure phase of $beta$-Li$_2$IrO$_3$ above $P_{rm S}$ was refined, which indicates the formation of Ir$_2$ dimers on the zig-zag chains, with the Ir-Ir distance even shorter than that of metallic Ir. We argue that the strong dimerization stabilizes the bonding molecular orbital state comprising the two local $d_{zx}$-orbitals on the Ir-O$_2$-Ir bond plane, which conflicts with the equal superposition of $d_{xy}$-, $d_{yz}$- and $d_{zx}$- orbitals in the $J_{rm eff}$ = 1/2 wave function produced by strong spin-orbit coupling. The results of resonant inelastic x-ray scattering (RIXS) measurements and the electronic structure calculations are fully consistent with the collapse of the $J_{rm eff}$ = 1/2 state. A subtle competition of various electronic phases is universal in honeycomb-based Kitaev materials.
We studied the effect of external pressure on the electrodynamic properties of $alpha$-Li$_2$IrO$_3$ single crystals in the frequency range of the phonon modes and the Ir $d$-$d$ transitions. The abrupt hardening of several phonon modes under pressure supports the onset of the dimerized phase at the critical pressure $P_c$=3.8 GPa. With increasing pressure an overall decrease in spectral weight of the Ir $d$-$d$ transitions is found up to $P_c$. Above $P_c$, the local (on-site) $d$-$d$ excitations gain spectral weight with increasing pressure, which hints at a pressure-induced increase in the octahedral distortions. The non-local (intersite) Ir $d$-$d$ transitions show a monotonic blue-shift and decrease in spectral weight. The changes observed for the non-local excitations are most prominent well above $P_c$, namely for pressures $geq$12 GPa, and only small changes occur for pressures close to $P_c$. The profile of the optical conductivity at high pressures ($sim$20 GPa) appears to be indicative for the dimerized state in iridates.
We study the effect of isoelectronic doping and external pressure in tuning the ground state of the honeycomb iridate Na$_2$IrO$_3$ by combining optical spectroscopy with synchrotron x-ray diffraction measurements on single crystals. The obtained optical conductivity of Na$_2$IrO$_3$ is discussed in terms of a Mott insulating picture versus the formation of quasimolecular orbitals and in terms of Kitaev-interactions. With increasing Li content $x$, (Na$_{1-x}$Li$_x$)$_2$IrO$_3$ moves deeper into the Mott insulating regime and there are indications that up to a doping level of 24% the compound comes closer to the Kitaev-limit. The optical conductivity spectrum of single crystalline $alpha$-Li$_2$IrO$_3$ does not follow the trends observed for the series up to $x=0.24$. There are strong indications that $alpha$-Li$_2$IrO$_3$ is less close to the Kitaev-limit compared to Na$_2$IrO$_3$ and closer to the quasimolecular orbital picture. Except for the pressure-induced hardening of the phonon modes, the optical properties of Na$_2$IrO$_3$ seem to be robust against external pressure. Possible explanations of the unexpected evolution of the optical conductivity with isolectronic doping and the drastic change between $x=0.24$ and $x=1$ are given by comparing the pressure-induced changes of lattice parameters and the optical conductivity with the corresponding changes induced by doping.
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