Erratum: Long-range order and spin-liquid states of polycrystalline<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:msub><mml:mi>Tb</mml:mi><mml:mrow><mml:mn>2</mml:mn><mml:mo>+</mml:mo><mml:mi>x</mml:mi></mml:mrow></mml:msub><mml:msub><mml:mi>Ti</mml:mi><mml:mrow><mml:mn>2</mml:mn><mml:mo>−</mml:mo><mml:mi>x</mml:mi></mml:mrow></mml:msub><mml:msub><mml:mi mathvariant="normal">O</mml:mi><mml:mrow><mml:mn>7</mml:mn><mml:mo>+</mml:mo><mml:mi>y</mml:mi></mml:mrow></mml:msub></mml:mrow><

Taniguchi, Tadatsugu; Kadowaki, Hiroko; Takatsu, Hiroshi; Fåk, B.; Ollivier, Jacques; Yamazaki, T.; Sato, T.; Yoshizawa, H.; Shimura, Yosuke; Sakakibara, T.; Hong, Tao; Goto, Kenji; Yaraskavitch, L. R.; Kycia, J. B.

doi:10.1103/physrevb.92.019903

Cited by 42 publications

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“…(1)] and the perturbation through first excited crystal-field (CF) states [14,32], and by taking another assumption of Jahn-Teller (JT) distortion [28,33]. Under the present postulation, two ground states of off-stoichiometric Tb 2+x Ti 2−x O 7+y samples [34] will possibly be accounted for by the U(1) QSL (x < x c ) and electric quadrupolar (x > x c ) states of Ref. [9].…”

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Quadrupole Order in the Frustrated PyrochloreTb2+xTi2−xO
Takatsu
¹
,
Onoda
²
,
Kittaka
³

et al. 2016
Phys. Rev. Lett.
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A hidden order that emerges in the frustrated pyrochlore Tb 2+x Ti 2−x O 7+y with T c = 0.53 K is studied using specific heat, magnetization, and neutron scattering experiments on a high-quality single crystal. Semi-quantitative analyses based on a pseudospin-1/2 Hamiltonian for ionic non-Kramers magnetic doublets demonstrate that it is an ordered state of electric quadrupole moments. The elusive spin liquid state of the nominal Tb 2 Ti 2 O 7 is most likely a U(1) quantum spin-liquid state. PACS numbers: 75.40.Cx, 78.70.Nx, 75.10.Kt, 75.30.Ds Geometrically frustrated magnets have been actively investigated in condensed matter physics [1]. In particular, spin ice (SI), e.g. R 2 Ti 2 O 7 (R = Dy or Ho) [2,3], provides prototypical frustrated Ising magnets with the pyrochlore lattice structure [4], consisting of a three-dimensional network of cornersharing tetrahedra [ Fig. 1(b)]. It displays fascinating features such as a finite zero-point entropy [5] and thermally excited emergent magnetic or SI monopoles [6,7]. An intriguing theoretical proposal for a U(1) quantum spin liquid (QSL) state [8] has been made for variants of SI endowed with quantum spin fluctuations [9][10][11][12][13][14]. The U(1) QSL state [8-10] is characterized by an emergent U(1) gauge field producing gapless fictitious photons and by gapped bosonic spinon excitations carrying the SI magnetic monopole charge [8,9,13,15]. By increasing the transverse interaction, the system can undergo a phase transition from the U(1) QSL to a long range ordered (LRO) state of transverse spins or pseudospins representing electric-quadrupole moments for non-Kramers ions [9][10][11]. This state can be described as a Higgs phase [16][17][18][19][20].In a quest to QSL states in frustrated magnetic systems from both theoretical [21][22][23] and experimental [24,25] viewpoints, an Ising-like pyrochlore Tb 2 Ti 2 O 7 (TTO) is a potential candidate for a U(1) QSL: it has been reported to remain in a fluctuating spin state down to 50 mK without magnetic LRO [26,27]. However, the origin of this spin liquid state of TTO has been elusive for more than a decade despite many investigations (see Refs. [4,13,28] and references therein, and recent Refs. [29-31]), and is still under hot debate [13,28]. To solve this challenging problem of TTO, we start this investigation by postulating that the theoretically-proposed interaction between electric quadrupole moments of non-Kramers ions including Tb 3+ [the fourth term of Eq. interactions between magnetic dipole moments [the first three terms of Eq. (1)] and the perturbation through first excited crystal-field (CF) states [14,32], and by taking another assumption of Jahn-Teller (JT) distortion [28,33]. Under the present postulation, two ground states of off-stoichiometric Tb 2+x Ti 2−x O 7+y samples [34] will possibly be accounted for by the U(1) QSL (x < x c ) and electric quadrupolar (x > x c ) states of Ref. [9].In this Letter, we investigate the hidden order of Tb 2+x Ti 2−x O 7+y (x = 0.005 > x c ), because the electric qua...

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“…Polycrystalline and single-crystalline Tb 2+x Ti 2−x O 7+y samples were prepared by a standard solid-state reaction [34] and by a floating zone method [35]. Specific heat was measured by a quasi-adiabatic method down to 0.1 K using a plate-shape crystal with a size of 0.7 × 0.9 × 0.1 mm 3 whose shortest dimension is along a [110] axis.…”

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confidence: 99%

Quadrupole Order in the Frustrated PyrochloreTb2+xTi2−xO
Takatsu
¹
,
Onoda
²
,
Kittaka
³

et al. 2016
Phys. Rev. Lett.
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“…31. The value of x was adjusted by changing the mass of the starting constituents, Tb 4 O 7 and TiO 2 , which were heated in air at 1350 • C for several days with periodic grindings to ensure complete reactions.…”

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confidence: 99%

“…The detailed nature of this k= ( 1 2 , 1 2 , 1 2 ) order was not determined in Ref. 31, but it seemed to extend over mesoscopic length scales, rather than the infinite length scale associated with symmetry breaking and Bragg scattering.…”

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confidence: 99%

“…This intensity vanishes under a small magnetic field of about 0.1 T and shows some sample dependence, suggesting the influence of a minute amount of defects. In powders, a systematic study of Tb 2+x Ti 2−x O 7+y samples 31 showed that the system could be tuned by minute changes of the Tb content around a critical concentration x c =-0.005 from a purely spin liquid state for x ≤ x c to a state with partial antiferromagnetic order with k= ( 1 2 , 1 2 , 1 2 ) propagation vector for x > x c . The detailed nature of this k= ( 1 2 , 1 2 , 1 2 ) order was not determined in Ref.…”

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Mesoscopic correlations inTb2Ti2O7spin liquid

et al. 2015

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We have studied the spin correlations with k= ( 1 2 , 1 2 , 1 2 ) propagation vector which appear below 0.4 K in Tb2Ti2O7 spin liquid by combining powder neutron diffraction and specific heat on Tb2+xTi2−xO7+y samples with x=0, 0.01, -0.01. The k= ( 1 2 , 1 2 , 1 2 ) order clearly appears on all neutron patterns by subtracting a pattern at 1.2(1) K. Refining the subtracted patterns at 0.07 K yields two possible spin structures, with spin-ice-like and monopole-like correlations respectively. Mesoscopic correlations involve Tb moments of 1 to 2 µB ordered on a length scale of about 20Å. In addition, long range order involving a small spin component of 0.1 to 0.2 µB is detected for the x= 0 and 0.01 samples showing a peak in the specific heat. Comparison with previous single crystals data suggests that the ( 1 2 , 1 2 , 1 2 ) order settles in through nanometric spin textures with dominant spin ice character and correlated orientations, analogous to nanomagnetic twins.Rare earth pyrochlores with geometrical magnetic frustration are model compounds to investigate classical spin ice as well as quantum spin ice physics. The short range ordered ground states with large degeneracy give rise to a large variety of interesting phenomena such as magnetic monopoles 1,2 , first order transition 3 , or unconventional magnetoelastic excitations 4,5 . These frustrated ground states are highly sensitive to small perturbations and to the presence of defects. Already in the 80s, Villain 6 predicted that for an arbitrary small concentration of defects the spinel lattice with pyrochlore structure could switch its ground state from spin liquid to spin glass. More recently many studies focus on the role of a minute amount of defects in pyrochlores. The crystal structure of R 2 Ti 2 O 7 pyrochlores (where R 3+ is a rare earth ion, Ti 4+ is non magnetic) accommodates oxygen vacancies, small off-stoechiometries in the R 3+ or Ti 4+ lattice, "stuffing" or site inversion. Oxygen vacancies introduce Ti 3+ defects instead of Ti 4+ ions, modifying the R 3+ crystal field and inducing local distortions, with various consequences on the low temperature magnetic properties and spin ice physics. In classical spin ice Dy 2 Ti 2 O 7 , oxygen depletion or a low level Dy stuffing in the Ti sites strongly slows down the monopole dynamics at very low temperature 7,8 and affects the nonequilibrium macroscopic properties 9,10 . In the quantum spin ice Yb 2 Ti 2 O 7 , small off-stoechiometry clearly affects the magnetic ground state 11 . It appears that precise studies of the magnetic defects are needed to resolve controversies concerning these unconventional ground states.Among the pyrochlores, Tb 2 Ti 2 O 7 is one of the most complex, the subject of numerous investigations since the discovery of its spin liquid character in 1999. The Tb 3+ short range correlated moments fluctuate 12 down to 20 mK at the time scale of the muon probe (10 −6 s). The origin of these fluctuations has been highly debated [13][14][15][16][17][18] . Several mechanisms have been pr...

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High temperature spin-freezing transition in pyrochlore Eu2Ti2O7: A new observation from ac-susceptibility

Pal

Singh

Ghosh

et al. 2018

Journal of Magnetism and Magnetic Materials

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The magnetization (both dc and ac) of pyrochlore Eu 2 Ti 2 O 7 have been investigated. Ac susceptibility (χ / &χ // ) measurements reveal a new unusual spin freezing below 35K for pure Eu 2 Ti 2 O 7 . Frequency dependence of these ac χ // peak positions indicate slow spin relaxation near this temperature and it follows the Arrhenius formulasuggesting a thermally activated relaxation process. The origin of this spin freezing has been attributed essentially to a single ion process which is associated to Eu 3+ spin relaxation. Non-magnetic dilution by Y 3+ ions also confirms the single ion freezing.

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Erratum: Long-range order and spin-liquid states of polycrystallineTb2+xTi2−xO7+y<

Cited by 42 publications

References 0 publications

Quadrupole Order in the Frustrated PyrochloreTb2+xTi2−xO
Takatsu
¹
,
Onoda
²
,
Kittaka
³

et al. 2016
Phys. Rev. Lett.
Self Cite
57
15
89
0
1
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Quadrupole Order in the Frustrated PyrochloreTb2+xTi2−xO
Takatsu
¹
,
Onoda
²
,
Kittaka
³

et al. 2016
Phys. Rev. Lett.
Self Cite
57
15
89
0
1
View full text Add to dashboard Cite

Mesoscopic correlations inTb2Ti2O7spin liquid

High temperature spin-freezing transition in pyrochlore Eu2Ti2O7: A new observation from ac-susceptibility

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Erratum: Long-range order and spin-liquid states of polycrystallineTb2+xTi2−xO7+y<

Cited by 42 publications

References 0 publications

Quadrupole Order in the Frustrated PyrochloreTb2+xTi2−xOTakatsu1, Onoda2, Kittaka3 et al. 2016Phys. Rev. Lett.Self Cite57158901View full textAdd to dashboardCite

Quadrupole Order in the Frustrated PyrochloreTb2+xTi2−xOTakatsu1, Onoda2, Kittaka3 et al. 2016Phys. Rev. Lett.Self Cite57158901View full textAdd to dashboardCite

Mesoscopic correlations inTb2Ti2O7spin liquid

High temperature spin-freezing transition in pyrochlore Eu2Ti2O7: A new observation from ac-susceptibility

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Quadrupole Order in the Frustrated PyrochloreTb2+xTi2−xO
Takatsu
¹
,
Onoda
²
,
Kittaka
³

et al. 2016
Phys. Rev. Lett.
Self Cite
57
15
89
0
1
View full text Add to dashboard Cite

Quadrupole Order in the Frustrated PyrochloreTb2+xTi2−xO
Takatsu
¹
,
Onoda
²
,
Kittaka
³

et al. 2016
Phys. Rev. Lett.
Self Cite
57
15
89
0
1
View full text Add to dashboard Cite