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Register a new userOptical signature of the pressure-induced dimerization in the honeycomb iridate $alpha$-Li$_2$IrO$_3$
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Added by
Christine Kuntscher
Publication date
2019
fields
Physics
and research's language is
English
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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.
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A pressure-induced collapse of magnetic ordering in $beta$-Li$_2$IrO$_3$ at $P_msim1.5- 2$ GPa has previously been interpreted as evidence for possible emergence of spin liquid states in this hyperhoneycomb iridate, raising prospects for experimental realizations of the Kitaev model. Based on structural data obtained at emph{room temperature}, this magnetic transition is believed to originate in small lattice perturbations that preserve crystal symmetry, and related changes in bond-directional anisotropic exchange interactions. Here we report on the evolution of the crystal structure of $beta$-Li$_2$IrO$_3$ under pressure at low temperatures ($Tleq50$ K) and show that the suppression of magnetism coincides with a change in lattice symmetry involving Ir-Ir dimerization. The critical pressure for dimerization shifts from 4.4(2) GPa at room temperature to $sim1.5-2$ GPa below 50 K. While a direct $Fddd rightarrow C2/c$ transition is observed at room temperature, the low temperature transitions involve new as well as coexisting dimerized phases. Further investigation of the Ir ($L_3$/$L_2$) isotropic branching ratio in x-ray absorption spectra indicates that the previously reported departure of the electronic ground state from a $J_{rm{eff}}=1/2$ state is closely related to the onset of dimerized phases. In essence, our results suggest that the predominant mechanism driving the collapse of magnetism in $beta$-Li$_2$IrO$_3$ is the pressure-induced formation of Ir$_2$ dimers in the hyperhoneycomb network. The results further confirm the instability of the $J_{rm{eff}}=1/2$ moments and related non-collinear spiral magnetic ordering against formation of dimers in the low-temperature phase of compressed $beta$-Li$_2$IrO$_3$.
We report equilibrium and nonequilibrium optical measurements on the recently synthesized harmonic honeycomb iridate gamma-Li$_2$IrO$_3$ (LIO), as well as the layered honeycomb iridate Na$_2$IrO$_3$ (NIO). Using Fourier transform infrared microscopy we performed reflectance measurements on LIO, from which we obtained the optical conductivity below 2 eV. In addition we measured the photoinduced changed in reflectance, Delta R, as a function of time, t, temperature, T, and probe field polarization in both LIO and NIO. In LIO, Delta R(t,T) is anisotropic and comprised of three T dependent components. Two of these components are related to the onset of magnetic order and the third is related to a photoinduced population of metastable electronic excited states. In NIO, Delta R(t,T) has a single T dependent component that is strikingly similar to the electronic excitation component of Delta R in LIO. Through analysis and comparison of Delta R(t,T) for two compounds, we extract information on the onset of magnetic correlations at and above the transition temperature in LIO, the bare spin-flip scattering rate in equilibrium, the lifetime of low-lying quasiparticle excitations, and the polarization dependence of optical transitions that are sensitive to magnetic order.
Temperature-pressure phase diagram of the Kitaev hyperhoneycomb iridate $beta$-Li$_2$IrO$_3$ is explored using magnetization, thermal expansion, magnetostriction, and muon spin rotation ($mu$SR) measurements, as well as single-crystal x-ray diffraction under pressure and ab initio calculations. The Neel temperature of $beta$-Li$_2$IrO$_3$ increases with the slope of 0.9 K/GPa upon initial compression, but the reduction in the polarization field $H_c$ reflects a growing instability of the incommensurate order. At 1.4 GPa, the ordered state breaks down upon a first-order transition giving way to a new ground state marked by the coexistence of dynamically correlated and frozen spins. This partial freezing in the absence of any conspicuous structural defects may indicate classical nature of the resulting pressure-induced spin liquid, an observation paralleled to the increase in the nearest-neighbor off-diagonal exchange $Gamma$ under pressure.
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 present magnetization measurements on polycrystalline $beta$-Li$_2$IrO$_3$ under hydrostatic pressures up to 3 GPa and construct the temperature-pressure phase diagram of this material. The magnetically ordered phase with $T_{rm{N}}simeq 38$ K breaks down upon a pressure-induced first-order phase transition at $p_{rm{c}}$ $approx$ 1.4 GPa and gives way to a high-pressure phase, where a step-like feature in the magnetic susceptibility signals a structural dimerization with a loss of Ir$^{4+}$ magnetic moments. Nevertheless, magnetism manifests itself also above $p_{rm{c}}$ via the Curie-like susceptibility upturn with the effective moment of 0.7 $mu_B$. We suggest that a partially dimerized phase with a mixture of the magnetic and non-magnetic Ir$^{4+}$ sites develops above $p_{rm{c}}$. This phase is thermodynamically stable between 1.7 and 2.7 GPa according to our ab initio calculations. It confines the magnetic Ir$^{4+}$ sites to weakly coupled tetramers with the singlet ground state and no long-range magnetic order. Our results rule out the formation of a pressure-induced spin-liquid phase in $beta$-Li$_2$IrO$_3$ and reveal peculiarities of the magnetism collapse transition in a Kitaev material.
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