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In Eu2ZnIrO6, effectively two atoms are active i.e. Ir is magnetically active, which results in complex magnetic ordering within the Ir sublattice at low temperature. On the other hand, although Eu is a van-vleck paramagnet, it is active in the elect ronic channels involving 4f 6 crystal-field split levels. Phonons, quanta of lattice vibration, involving vibration of atoms in the unit cell, are intimately coupled with both magnetic and electronic degrees of freedom (DoF). Here, we report a comprehensive study focusing on the phonons as well as intra-configurational excitations in double-perovskite Eu2ZnIrO6. Our studies reveal strong coupling of phonons with the underlying magnetic DoF reflected in the renormalization of the phonon self-energy parameters well above the spin-solid phase (TN ~ 12 K) till temperature as high as ~ 3TN, evidences broken spin rotational symmetry deep into the paramagnetic phase. In particular, all the observed first-order phonon modes show softening of varying degree below ~3TN, and low-frequency phonons become sharper, while the high-frequency phonons show broadening attributed to the additional available magnetic damping channels. We also observed a large number of high-energy modes, 39 in total, attributed to the electronic transitions between 4f-levels of the rare-earth Eu3+ ion and these modes shows anomalous temperature evolution as well as mixing of the crystal-field split levels attributed to the strong coupling of electronic and lattice DoF.
We report comprehensive Raman-scattering measurements on a single crystal of double-perovskite Nd2ZnIrO6 in temperature range of 4-330 K, and spanning a broad spectral range from 20 cm-1 to 5500 cm-1. The paper focuses on lattice vibrations and elect ronic transitions involving Kramers doublets of the rare-earth Nd3+ ion with local C1 site symmetry. Temperature evolution of these quasi-particle excitations have allowed us to ascertain the intricate coupling between lattice and electronic degrees of freedom in Nd2ZnIrO6. Strong coupling between phonons and crystal-field excitation is observed via renormalization of the self-energy parameter of the phonons i.e. peak frequency and line-width. The phonon frequency shows abrupt hardening and line-width narrowing below ~ 100 K for the majority of the observed first-order phonons. We observed splitting of the lowest Kramers doublets of ground state (4I9/2) multiplets i.e. lifting of the Kramers degeneracy, prominently at low-temperature (below ~ 100 K), attributed to the Nd-Nd/Ir exchange interactions and the intricate coupling with the lattice degrees of freedom. The observed splitting is of the order of ~ 2-3 meV and is consistent with the estimated value. We also observed a large number of high-energy modes, 46 in total, attributed to the intra-configurational transitions between 4f3 levels of Nd3+ coupled to the phonons reflected in their anomalous temperature evolution.
109 - M. Vogl , R. Morrow , A.A. Aczel 2019
In this work, we report on the synthesis and magnetic properties of a series of double perovskites Ln$_2$ZnIrO$_6$ with Ln = Nd, Sm, Eu & Gd. These compounds present new examples of the rare case of double perovskites (general formula A$_2$BBO$_6$) w ith a magnetic 4f -ion on the A-site in combination with the strongly spin-orbit coupled 5d-transition metal ion Ir$^{4+}$ on the B-sublattice. We discuss the impact of different rare earths on the macroscopic magnetic properties. Gd$_2$ZnIrO$_6$ and Eu$_2$ZnIrO$_6$ show weak canted antiferromagnetic order below T$_N$ = 23 K and T$_N$ = 12 K, respectively. Sm$_2$ZnIrO$_6$ orders antiferromagnetically at T$_N$ = 13 K. Nd$_2$ZnIrO$_6$ exhibits complex magnetic properties with strong field dependence ranging from a two-step behavior at H = 0.01 T to an antiferromagnetic ground state at intermediate external fields and a spin-flop phase at H$geq$4 T, which suggests complex interplay between Nd$^{3+}$ and Ir$^{4+}$ . To further shed light on this magnetic interaction, the magnetic structure of Nd$_2$ZnIrO$_6$s ground state is examined via neutron powder diffraction.
64 - M. Vogl , G. Bastien , R. Sarkar 2019
The synthesis and characterization of the previously unknown material LaCaScIrO$_6$ is reported. LaCaScIrO$_6$ presents a new example of the rare case of a double perovskite with the strongly spin-orbit coupled 5textit{d}-ion Ir$^{4+}$ as its only ma gnetic species, forming a monoclinically distorted version of the frustrated fcc lattice. Magnetization measurements show a weak anomaly at 8~K. The Curie-Weiss temperature Theta$_{CW}$ and effective magnetic moment mu$_{eff}$ of LaCaScIrO$_6$ are in close proximity to the related compound La$_2$MgIrO$_6$ but differ from La$_2$ZnIrO$_6$. This suggests that the nature of the non-magnetic textit{B}-ion, namely its textit{d}-orbital filling has a strong influence on the magnetic properties. The textit{d}$^{0}$-ions Sc$^{3+}$ and Mg$^{2+}$ allow a different kind of exchange interactions within the Ir-sublattice than the textit{d}$^{10}$-ion Zn$^{2+}$. In addition, ac-susceptibility data does not show signs of a spin-glass ground state. The nature of the magnetism in LaCaScIrO$_6$ has been further elucidated using muon spin relaxation measurements. The zero-field measurements reveal the absence of well defined oscillations down to 1.6,K, while temperature dependent $mu$SR studies show an anomaly at 8,K. Overall, our results suggest the presence of two different magnetic environments or domains in LaCaScIrO$_6$, which is likely related to its structural features.
We investigate precursors of critical behavior in the quasienergy spectrum due to the dynamical instability in the kicked top. Using a semiclassical approach, we analytically obtain a logarithmic divergence in the density of states, which is analogou s to a continuous excited state quantum phase transition in undriven systems. We propose a protocol to observe the cusp behavior of the magnetization close to the critical quasienergy.
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