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Register a new userNearly itinerant electronic groundstate in the intercalated honeycomb iridate Ag$_3$LiIr$_2$O$_6$
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Added by
Alberto de la Torre
Publication date
2021
fields
Physics
and research's language is
English
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We use x-ray spectroscopy at Ir L$_3$/L$_2$ absorption edge to study powder samples of the intercalated honeycomb magnet Ag$_3$LiIr$_2$O$_6$. Based on x-ray absorption and resonant inelastic x-ray scattering measurements, and exact diagonalization calculations including next-neighbour Ir-Ir electron hoping integrals, we argue that the intercalation of Ag atoms results in a nearly itinerant electronic structure with enhanced Ir-O hybridization. As a result of the departure from the local relativistic $j_{rm eff}! = !1/2$ state, we find that the relative orbital contribution to the magnetic moment is increased, and the magnetization density is spatially extended and asymmetric. Our results confirm the importance of metal - ligand hybridazation in the magnetism of transition metal oxides and provide empirical guidance for understanding the collective magnetism in intercalated honeycomb iridates.
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We investigate the structural and magnetic properties of a Kitaev spin liquid candidate material Ag$_3$LiIr$_2$O$_6$ based on $^7$Li nuclear magnetic resonance line shape, Knight shift and spin-lattice relaxation rate $1/T_1$. The first sample A shows signatures of magnetically ordered spins, and exhibits one sharp $^7$Li peak with FWHM increasing significantly below 14~K. $1/T_1^{stretch}$ of this sample displays a broad local maximum at 40~K, followed by a very sharp peak at $T_N = 9pm1$~K due to critical slowing down of Ir spin fluctuations, a typical signature of magnetic long range order. In order to shed light on the position-by-position variation of $1/T_1$ throughout the sample, we use Inverse Laplace Transform $T_1$ analysis based on Tikhonov regularization to deduce the density distribution function $P(1/T_1)$. We demonstrate that $sim 60%$ of Ir spins are statically ordered at the NMR measurement timescale but the rest of the sample volume remains paramagnetic even at 4.2~K, presumably because of structural disorder induced primarily by stacking faults. In order to further investigate the influence of structural disorder, we compare these NMR results with those of a second sample B, which has been shown by transmission electron microscope to have domains with unwanted Ag inclusion at Li and Ir sites within the Ir honeycomb planes. The sample B displays an additional NMR peak with relative intensity of $sim 17%$. The small Knight shift and $1/T_1$ of these defect-induced $^7$Li sites and the enhancement of bulk susceptibility at low temperatures suggest that these defects generate domains of only weakly magnetic Ir spins accompanied by free spins, leading to a lack of clear signatures of long-range order. The apparent lack of long-range order could be easily misinterpreted as evidence for the realization of a spin liquid ground state in highly disordered Kitaev lattice.
Detecting Majorana fermions in experimental realizations of the Kitaev honeycomb model is often complicated by non-trivial interactions inherent to potential spin liquid candidates, where the interplay of exotic forms of quantum magnetism often leads to false indications of novel spin excitations. In this letter, we propose several distinct thermodynamic signatures of massive, itinerant Majorana fermions within the well-established analytical paradigm of Landau-Fermi liquid theory. We find that all salient features of the theory are confirmed in the specific heat measurements of the Kitaev spin liquid candidate Ag$_3$LiIr$_2$O$_6$. Our study is the first of its kind to present strong evidence for a Fermi liquid-like ground state in the fundamental excitations of a honeycomb iridate, and opens new experimental avenues to detect itinerant Majorana fermions in condensed matter as a whole.
Recently H$_3$LiIr$_2$O$_6$ has been reported as a spin-orbital entangled quantum spin liquid (QSL) [K. Kitagawa et al., Nature {bf 554}, 341 (2018)], albeit its connection to Kitaev QSL has not been yet identified. To unveil the related Kitaev physics, we perform the first Raman spectroscopy studies on single crystalline H$_3$LiIr$_2$O$_6$ samples. We implement a soft chemical replacement of Li$^+$ with H$^+$ from $alpha$-Li$_2$IrO$_3$ single crystals to synthesize the single crystal samples of the iridate second generation H$_3$LiIr$_2$O$_6$. The Raman spectroscopy can be used to diagnose the QSL state since the magnetic Raman continuum arises from a process involving pairs of fractionalized Majorana fermionic excitation in a pure Kitaev model. We observe a broad dome-shaped magnetic continuum in H$_3$LiIr$_2$O$_6$, in line with theoretical expectations for the two-spin process in the Kitaev QSL. Our results establish the close connection to the Kitaev QSL physics in H$_3$LiIr$_2$O$_6$.
The silver ruthenium oxide AgRuO$_3$ consists of honeycomb [Ru$_2^{5+}$O$_6^{2-}$] layers, and can be considered an analogue of SrRu$_2$O$_6$ with a different intercalation stage. We present measurements of magnetic susceptibility and specific heat on AgRuO$_3$ single crystals which reveal a sharp antiferromagnetic transition at 342(3)K. The electrical transport in single crystals of AgRuO$_3$ is determined by a combination of activated conduction over an intrinsic semiconducting gap of $approx$ 100 meV and carriers trapped and thermally released from defects. From powder neutron diffraction data a Neel-type antiferromagnetic structure with the Ru moments along the $c$ axis is derived. Raman and muon spin rotation spectroscopy measurements on AgRuO$_3$ powder samples indicate a further weak phase transition or a crossover in the temperature range 125-200 K. The transition does not show up in magnetic susceptibility and its origin is argued to be related to defects but cannot be fully clarified. The experimental findings are complemented by DFT-based electronic structure calculations. It is found that the magnetism in AgRuO$_3$ is similar to that of SrRu$_2$O$_6$, however with stronger intralayer and weaker interlayer magnetic exchange interactions.
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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