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Gapless spin-liquid state in the structurally disorder-free triangular antiferromagnet NaYbO$_2$

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 Added by Lei Ding
 Publication date 2019
  fields Physics
and research's language is English




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We present the structural characterization and low-temperature magnetism of the triangular-lattice delafossite NaYbO$_2$. Synchrotron x-ray diffraction and neutron scattering exclude both structural disorder and crystal-electric-field randomness, whereas heat-capacity measurements and muon spectroscopy reveal the absence of magnetic order and persistent spin dynamics down to at least 70,mK. Continuous magnetic excitations with the low-energy spectral weight accumulating at the $K$-point of the Brillouin zone indicate the formation of a novel spin-liquid phase in a triangular antiferromagnet. This phase is gapless and shows a non-trivial evolution of the low-temperature specific heat. Our work demonstrates that NaYbO$_2$ practically gives the most direct experimental access to the spin-liquid physics of triangular antiferromagnets.



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Quantum spin liquid (QSL) is a novel state of matter which refuses the conventional spin freezing even at 0 K. Experimentally searching for the structurally perfect candidates is a big challenge in condensed matter physics. Here we report the successful synthesis of a new spin-1/2 triangular antiferromagnet YbMgGaO$_4$ with R$bar{3}$m symmetry. The compound with an ideal two-dimensional and spatial isotropic magnetic triangular-lattice has no site-mixing magnetic defects and no antisymmetric Dzyaloshinsky-Moriya (DM) interactions. No spin freezing down to 60 mK (despite $Theta$$_w$ $sim$ -4 K), the low-T power-law temperature dependence of heat capacity and nonzero susceptibility suggest that YbMgGaO$_4$ is a promising gapless ($leq$ $|$$Theta$$_w$$|$/100) QSL candidate. The residual spin entropy, which is accurately determined with a non-magnetic reference LuMgGaO$_4$, approaches zero ($<$ 0.6 %). This indicates that the possible QSL ground state (GS) of the frustrated spin system has been experimentally achieved at the lowest measurement temperatures.
Here we present a neutron scattering-based study of magnetic excitations and magnetic order in NaYbO$_2$ under the application of an external magnetic field. The crystal electric field-split $J = 7/2$ multiplet structure is determined, revealing a mixed $|m_z>$ ground state doublet and is consistent with a recent report Ding et al. [1]. Our measurements further suggest signatures of exchange effects in the crystal field spectrum, manifested by a small splitting in energy of the transition into the first excited doublet. The field-dependence of the low-energy magnetic excitations across the transition from the quantum disordered ground state into the fluctuation-driven ordered regime is analyzed. Signs of a first-order phase transition into a noncollinear ordered state are revealed at the upper-field phase boundary of the ordered regime, and higher order magnon scattering, suggestive of strong magnon-magnon interactions, is resolved within the previously reported $up-up-down$ phase. Our results reveal a complex phase diagram of field-induced order and spin excitations within NaYbO$_2$ and demonstrate the dominant role of quantum fluctuations cross a broad range of fields within its interlayer frustrated triangular lattice.
We report a comprehensive investigation of the magnetism of the $S$ = 3/2 triangular-lattice antiferromagnet, $alpha$-CrOOH(D) (delafossites green-grey powder). The nearly Heisenberg antiferromagnetic Hamiltonian ($J_1$ $sim$ 23.5 K) with a weak single-ion anisotropy of $|D|$/$J_1$ $sim$ 4.6% is quantitatively determined by fitting to the electron spin resonance (ESR) linewidth and susceptibility measured at high temperatures. The weak single-ion anisotropy interactions, possibly along with other perturbations, e.g. next-nearest-neighbor interactions, suppress the long-range magnetic order and render the system disordered, as evidenced by both the absence of any clear magnetic reflections in neutron diffraction and the presence of the dominant paramagnetic ESR signal down to 2 K ($sim$ 0.04$J_1$$S^2$), where the magnetic entropy is almost zero. The power-law behavior of specific heat ($C_m$ $sim$ $T^{2.2}$) observed below the freezing temperature of $T_f$ = 25 K in $alpha$-CrOOH or below $T_f$ = 22 K in $alpha$-CrOOD is insensitive to the external magnetic field, and thus is consistent with the theoretical prediction of a gapless U(1) Dirac quantum spin liquid (QSL) ground state. At low temperatures, the spectral weight of the low-energy continuous spin excitations accumulates at the K points of the Brillouin zone, e.g. $|mathbf{Q}|$ = 4$pi$/(3$a$), and the putative Dirac cones are clearly visible. Our work is a first step towards the understanding of the possible Dirac QSL ground state in this triangular-lattice magnet with $S$ = 3/2.
Rare-earth delafossites were recently proposed as promising candidates for the realization of an effective $S$=1/2 quantum spin liquid (QSL) on the triangular lattice. In contrast to the most actively studied triangular-lattice antiferromagnet YbMgGaO$_4$, which is known for considerable structural disorder due to site intermixing, NaYbS$_2$ delafossite realizes structurally ideal triangular layers. We present detailed $mu$SR studies on this regular (undistorted) triangular Yb sublattice based system with effective spin $J_{mathrm{eff}}=1/2$ in the temperature range 0.05 - 40 K. Zero-field (ZF) and longitudinal field (LF) $mu$SR studies confirm the absence of any long range magnetic order state down to 0.05K ($sim J$/80). Current $mu$SR results together with the so far available bulk characterization data suggest that NaYbS$_2$ is an ideal candidate to identify QSL ground state.
Polycrystalline samples of NaYbO$_2$ are investigated by bulk magnetization and specific-heat measurements, as well as by nuclear magnetic resonance (NMR) and electron spin resonance (ESR) as local probes. No signatures of long-range magnetic order are found down to 0.3~K, evidencing a highly frustrated spin-liquid-like ground state in zero field. Above 2,T, signatures of magnetic order are observed in thermodynamic measurements, suggesting the possibility of a field-induced quantum phase transition. The $^{23}$Na NMR relaxation rates reveal the absence of magnetic order and persistent fluctuations down to 0.3~K at very low fields and confirm the bulk magnetic order above 2~T. The $H$-$T$ phase diagram is obtained and discussed along with the existing theoretical concepts for layered spin-$frac{1}{2}$ triangular-lattice antiferromagnets
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