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Register a new userCrystalline Electric-Field Excitations in Quantum Spin Liquids Candidate $NaYbSe_{2}$
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Very recently we revealed a large family of triangular lattice quantum spin liquid candidates named rare-earth chalcogenides, which features a high-symmetry structure without structural/charge disorders and spin impurities, and may serve as an ideal platform exploring spin liquid physics. The knowledge of crystalline electric-field (CEF) excitations is an essential step to explore the fundamental magnetism of rare-earth spin systems. Here we employed inelastic neutron scattering (INS) and Raman scattering (RS) to carry out a comprehensive CFE investigation on $NaYbSe_{2}$, a promising representative of the family. By comparison with its nonmagnetic compound $NaLuSe_{2}$, we are able to identify the CEF excitations at 15.8, 24.3 and 30.5 meV at 5K. The selected cuts of the INS spectra are well re-produced with a large anisotropy of $g$ factors ($g_{ab}:g_{c}sim3:1$). Further, the CEF excitations are explained well by our calculations based on the point charge model. Interestingly, $NaYbSe_{2}$ exhibits an unusual CEF shift to higher energies with increasing temperatures, and the Raman mode close to the first CEF excitation shows an anomalously large softening with decreasing temperatures. The absence of the anomalies in $NaLuSe_{2}$ clearly demonstrates a CEF-phonon coupling not reported in the family. It can be understood in term of the weaker electronegativity of Se. The fact that the smallest first CEF excitation in the sub-family of $NaYbCh_{2}$ is $sim$ 180K (Ch=O, S, Se), guarantees that the sub-family can be strictly described with an effective S=1/2 picture at sufficiently low temperatures. Interestingly the CEF-phonon coupling revealed here may present alternative possibilities to manipulate the spin systems.
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In this paper, we performed thermodynamic and electron spin resonance (ESR) measurements to study low-energy magnetic excitations, which were significantly affected by crystalline electric field (CEF) excitations due to relatively small gaps between the CEF ground state and the excited states. Based on the CEF and mean-field (MF) theories, we analyzed systematically and consistently the ESR experiments and thermodynamic measurements including susceptibility, magnetization, and heat capacity. The CEF parameters were successfully extracted by fitting high-temperature (> 20 K) susceptibilities in the ab-plane and along the c-axis, allowing to determine the Lande factors ($g_{ab,calc}$ = 5.98(7) and $g_{c,calc}$ = 2.73(3)). These values were consistent with the values of Lande factors determined by ESR experiments ($g_{ab,exp}$ = 5.69 and $g_{c,exp}$ = 2.75). By applying the CEF and MF theories to the susceptibility and magnetization results, we estimated the anisotropic spin-exchange energies and found that the CEF excitations in ce{KErTe2} played a decisive role in the magnetism above 3 K, while the low-temperature magnetism below 10 K was gradually correlated with the anisotropic spin-exchange interactions. The CEF excitations were demonstrated in the low-temperature heat capacity, where both the positions of two broad peaks and their magnetic field dependence well corroborated our calculations. The present study provides a basis to explore the enriched magnetic and electronic properties of the QSL family.
We investigate the crystal structure, magnetic properties, and crystalline-electric field of tetragonal, $I4_1/amd$, NaCeO$_2$. In this compound, Ce$^{3+}$ ions form a tetragonally elongated diamond lattice coupled by antiferromagnetic interactions ($Theta_{CW} = -7.69$ K) that magnetically order below $T_N = 3.18$ K. The Ce$^{3+}$ $J = 5/2$ crystalline-electric field-split multiplet is studied via inelastic neutron scattering to parameterize a $J_{eff} = 1/2$ ground state doublet comprised of states possessing mixed $|m_z rangle$ character. Neutron powder diffraction data reveal the onset of $A$-type antiferromagnetism with $mu=0.57(2)$ $mu_B$ moments aligned along the $c$-axis. The magnetic structure is consistent with the expectations of a frustrated Heisenberg $J_1$-$J_2$ model on the elongated diamond lattice with effective exchange values $J_1 > 4 J_2$ and $J_1 > 0$.
The crystalline electric field (CEF) energy level scheme of the heavy fermion superconductor CeCoIn_5 has been determined by means of inelastic neutron scattering (INS). Peaks observed in the INS spectra at 8 meV and 27 meV with incident neutron energies between E_i=30-60 meV and at a temperature T = 10 K correspond to transitions from the ground state to the two excited states, respectively. The wavevector and temperature dependence of these peaks are consistent with CEF excitations. Fits of the data to a CEF model yield the CEF parameters B^0_2=-0.80 meV, B^0_4=0.059 meV, and |B^4_4|= 0.137 meV corresponding to an energy level scheme: Gamma_7^(1) (0)[=0.487|+/-5/2> - 0.873|-/+3/2>], Gamma_7^(2) (8.6 meV, 100 K), and Gamma_6 (24.4 meV, 283 K).
The electrodynamic response of organic spin liquids with highly-frustrated triangular lattices has been measured in a wide energy range. While the overall optical spectra of these Mott insulators are governed by transitions between the Hubbard bands, distinct in-gap excitations can be identified at low temperatures and frequencies which we attribute to the quantum spin liquid state. For the strongly correlated $beta^{prime}$-EtMe$_3$-Sb-[Pd(dmit)$_2$]$_2$, we discover enhanced conductivity below $175~{rm cm}^{-1}$, comparable to the energy of the magnetic coupling $Japprox 250$ K. For $omegarightarrow 0$ these low-frequency excitations vanish faster than the charge-carrier response subject to Mott-Hubbard correlations, resulting in a dome-shape band peaked at 100~cm. Possible relations to spinons, magnons and disorder are discussed.
We apply moderate-high-energy inelastic neutron scattering (INS) measurements to investigate Yb$^{3+}$ crystalline electric field (CEF) levels in the triangular spin-liquid candidate YbMgGaO$_4$. Three CEF excitations from the ground-state Kramers doublet are centered at the energies $hbar omega$ = 39, 61, and 97,meV in agreement with the effective mbox{spin-1/2} $g$-factors and experimental heat capacity, but reveal sizable broadening. We argue that this broadening originates from the site mixing between Mg$^{2+}$ and Ga$^{3+}$ giving rise to a distribution of Yb--O distances and orientations and, thus, of CEF parameters that account for the peculiar energy profile of the CEF excitations. The CEF randomness gives rise to a distribution of the effective spin-1/2 $g$-factors and explains the unprecedented broadening of low-energy magnetic excitations in the fully polarized ferromagnetic phase of YbMgGaO$_4$, although a distribution of magnetic couplings due to the Mg/Ga disorder may be important as well.
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