Quenched crystal-field disorder and magnetic liquid ground states in Tb2Sn2-xTixO7 [Crystal field disorder in the quantum spin ice ground state of Tb2Sn2-xTixO7]

Gaulin, B. D.; Kermarrec, E.; Dahlberg, M. L.; Matthews, M. J.; Bert, F.; Zhang, J.; Mendels, P.; Fritsch, K.; Granroth, G. E.; Jiramongkolchai, P.; Amato, A.; Baines, C.; Cava, R. J.; Schiffer, P.

doi:10.1103/PhysRevB.91.245141

Title: Quenched crystal-field disorder and magnetic liquid ground states in ${Tb}_{2} {Sn}_{2 - x} {Ti}_{x} O_{7}$ [Crystal field disorder in the quantum spin ice ground state of Tb2Sn2-xTixO7]

Journal Article · Mon Jun 01 00:00:00 EDT 2015 · Physical Review. B, Condensed Matter and Materials Physics

DOI:https://doi.org/10.1103/PhysRevB.91.245141· OSTI ID:1185348

Gaulin, B. D. ^[1]; Kermarrec, E. ^[2]; Dahlberg, M. L. ^[3]; Matthews, M. J. ^[3]; Bert, F. ^[2]; Zhang, J. ^[1]; Mendels, P. ^[4]; Fritsch, K. ^[5]; Granroth, G. E. ^[6]; Jiramongkolchai, P. ^[7]; Amato, A. ^[8]; Baines, C. ^[8]; Cava, R. J. ^[7]; Schiffer, P. ^[3]

McMaster Univ., Hamilton, ON (Canada)
Univ. Paris Sud XI, Orsay, (France)
Pennsylvania State Univ., University Park, PA (United States)
Univ. Paris Sud XI, Orsay, (France); Institut Universitaire de France, Paris (France)
McMaster Univ., Hamilton, ON (Canada); Helmholtz-Zentrum Berlin (HZB), (Germany). German Research Centre for Materials and Energy
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Princeton Univ., NJ (United States)
Paul Scherrer Inst. (PSI), Villigen (Switzerland)

Solid-solutions of the "soft" quantum spin ice pyrochlore magnets Tb₂B₂O₇ with B=Ti and Sn display a novel magnetic ground state in the presence of strong B-site disorder, characterized by a low susceptibility and strong spin fluctuations to temperatures below 0.1 K. These materials have been studied using ac-susceptibility and muSR techniques to very low temperatures, and time-of-flight inelastic neutron scattering techniques to 1.5 K. Remarkably, neutron spectroscopy of the Tb³⁺ crystal field levels appropriate to at high B-site mixing (0.5 < x < 1.5 in Tb₂Sn_2-xTi_xO₇) reveal that the doublet ground and first excited states present as continua in energy, while transitions to singlet excited states at higher energies simply interpolate between those of the end members of the solid solution. The resulting ground state suggests an extreme version of a random-anisotropy magnet, with many local moments and anisotropies, depending on the precise local configuration of the six B sites neighboring each magnetic Tb³⁺ ion.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; DG-FG02-08ER46544

OSTI ID:: 1185348

Alternate ID(s):: OSTI ID: 1186723

Journal Information:: Physical Review. B, Condensed Matter and Materials Physics, Vol. 91, Issue 24; ISSN 1098-0121

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 9 works

Citation information provided by
Web of Science

References (40)

Magnetic pyrochlore oxides Gardner, Jason S.; Gingras, Michel J. P.; Greedan, John E. Reviews of Modern Physics, Vol. 82, Issue 1 https://doi.org/10.1103/RevModPhys.82.53	journal	January 2010
Introduction to Frustrated Magnetism Lacroix, Claudine; Mendels, Philippe; Mila, Frédéric Springer Series in Solid-State Sciences https://doi.org/10.1007/978-3-642-10589-0	book	January 2011
Geometrical Frustration in the Ferromagnetic Pyrochlore ${Ho}_{2} {Ti}_{2} O_{7}$ Harris, M. J.; Bramwell, S. T.; McMorrow, D. F. Physical Review Letters, Vol. 79, Issue 13 https://doi.org/10.1103/PhysRevLett.79.2554	journal	September 1997
Magnetic Coulomb Phase in the Spin Ice Ho2Ti2O7 Fennell, T.; Deen, P. P.; Wildes, A. R. Science, Vol. 326, Issue 5951 https://doi.org/10.1126/science.1177582	journal	September 2009
Revisiting static and dynamic spin-ice correlations in ${Ho}_{2} {Ti}_{2} O_{7}$ with neutron scattering Clancy, J. P.; Ruff, J. P. C.; Dunsiger, S. R. Physical Review B, Vol. 79, Issue 1 https://doi.org/10.1103/PhysRevB.79.014408	journal	January 2009
Zero-point entropy in ‘spin ice’ Ramirez, A. P.; Hayashi, A.; Cava, R. J. Nature, Vol. 399, Issue 6734 https://doi.org/10.1038/20619	journal	May 1999
Spin Ice State in Frustrated Magnetic Pyrochlore Materials Bramwell, S. T. Science, Vol. 294, Issue 5546 https://doi.org/10.1126/science.1064761	journal	November 2001
Spin liquids in frustrated magnets Balents, Leon Nature, Vol. 464, Issue 7286 https://doi.org/10.1038/nature08917	journal	March 2010
Magnetic monopoles in spin ice Castelnovo, C.; Moessner, R.; Sondhi, S. L. Nature, Vol. 451, Issue 7174 https://doi.org/10.1038/nature06433	journal	January 2008
Signature of magnetic monopole and Dirac string dynamics in spin ice Jaubert, L. D. C.; Holdsworth, P. C. W. Nature Physics, Vol. 5, Issue 4 https://doi.org/10.1038/nphys1227	journal	March 2009
Dirac Strings and Magnetic Monopoles in the Spin Ice Dy2Ti2O7 Morris, D. J. P.; Tennant, D. A.; Grigera, S. A. Science, Vol. 326, Issue 5951 https://doi.org/10.1126/science.1178868	journal	September 2009
Quantum Excitations in Quantum Spin Ice Ross, Kate A.; Savary, Lucile; Gaulin, Bruce D. Physical Review X, Vol. 1, Issue 2 https://doi.org/10.1103/PhysRevX.1.021002	journal	October 2011
Neutron spectroscopic study of crystal field excitations in ${Tb}_{2} {Ti}_{2} O_{7}$ and ${Tb}_{2} {Sn}_{2} O_{7}$ Zhang, J.; Fritsch, K.; Hao, Z. Physical Review B, Vol. 89, Issue 13 https://doi.org/10.1103/PhysRevB.89.134410	journal	April 2014
Thermodynamic and single-ion properties of Tb3+ within the collective paramagnetic-spin liquid state of the frustrated pyrochlore antiferromagnet Tb2Ti2O7 Gingras, M.; den Hertog, B.; Faucher, M. Physical Review B, Vol. 62, Issue 10 https://doi.org/10.1103/PhysRevB.62.6496	journal	September 2000
Magnetic excitations in ${Tb}_{2} {Sn}_{2} O_{7}$ and ${Tb}_{2} {Ti}_{2} O_{7}$ as measured by inelastic neutron scattering Mirebeau, I.; Bonville, P.; Hennion, M. Physical Review B, Vol. 76, Issue 18 https://doi.org/10.1103/PhysRevB.76.184436	journal	November 2007
Cooperative Paramagnetism in the Geometrically Frustrated Pyrochlore Antiferromagnet ${Tb}_{2} {Ti}_{2} O_{7}$ Gardner, J. S.; Dunsiger, S. R.; Gaulin, B. D. Physical Review Letters, Vol. 82, Issue 5 https://doi.org/10.1103/PhysRevLett.82.1012	journal	February 1999
Neutron scattering studies of the cooperative paramagnet pyrochlore ${Tb}_{2} {Ti}_{2} O_{7}$ Gardner, J. S.; Gaulin, B. D.; Berlinsky, A. J. Physical Review B, Vol. 64, Issue 22 https://doi.org/10.1103/PhysRevB.64.224416	journal	November 2001
Dipolar Interactions and Origin of Spin Ice in Ising Pyrochlore Magnets den Hertog, Byron C.; Gingras, Michel J. P. Physical Review Letters, Vol. 84, Issue 15 https://doi.org/10.1103/PhysRevLett.84.3430	journal	April 2000
Understanding paramagnetic spin correlations in the spin-liquid pyrochlore ${Tb}_{2} {Ti}_{2} O_{7}$ Kao, Ying-Jer; Enjalran, Matthew; Del Maestro, Adrian Physical Review B, Vol. 68, Issue 17 https://doi.org/10.1103/PhysRevB.68.172407	journal	November 2003
Power-Law Spin Correlations in the Pyrochlore Antiferromagnet ${Tb}_{2} {Ti}_{2} O_{7}$ Fennell, T.; Kenzelmann, M.; Roessli, B. Physical Review Letters, Vol. 109, Issue 1 https://doi.org/10.1103/PhysRevLett.109.017201	journal	July 2012
Antiferromagnetic spin ice correlations at ( $\frac{1}{2}$ , $\frac{1}{2}$ , $\frac{1}{2}$ ) in the ground state of the pyrochlore magnet Tb $_{2}$ Ti $_{2}$ O $_{7}$ Fritsch, K.; Ross, K. A.; Qiu, Y. Physical Review B, Vol. 87, Issue 9 https://doi.org/10.1103/PhysRevB.87.094410	journal	March 2013
Temperature and magnetic field dependence of spin-ice correlations in the pyrochlore magnet ${Tb}_{2} {Ti}_{2} O_{7}$ Fritsch, K.; Kermarrec, E.; Ross, K. A. Physical Review B, Vol. 90, Issue 1 https://doi.org/10.1103/PhysRevB.90.014429	journal	July 2014
Spin liquid correlations, anisotropic exchange, and symmetry breaking in Tb $_{2}$ Ti $_{2}$ O $_{7}$ Petit, Sylvain; Bonville, Pierre; Robert, Julien Physical Review B, Vol. 86, Issue 17 https://doi.org/10.1103/PhysRevB.86.174403	journal	November 2012
Magnetoelastic Excitations in the Pyrochlore Spin Liquid ${Tb}_{2} {Ti}_{2} O_{7}$ Fennell, T.; Kenzelmann, M.; Roessli, B. Physical Review Letters, Vol. 112, Issue 1 https://doi.org/10.1103/PhysRevLett.112.017203	journal	January 2014
Anisotropic Propagating Excitations and Quadrupolar Effects in ${Tb}_{2} {Ti}_{2} O_{7}$ Guitteny, Solène; Robert, Julien; Bonville, Pierre Physical Review Letters, Vol. 111, Issue 8 https://doi.org/10.1103/PhysRevLett.111.087201	journal	August 2013
Tetragonal distortion yielding a two-singlet spin liquid in pyrochlore Tb $_{2}$ Ti $_{2}$ O $_{7}$ Bonville, Pierre; Mirebeau, Isabelle; Gukasov, Arsène Physical Review B, Vol. 84, Issue 18 https://doi.org/10.1103/PhysRevB.84.184409	journal	November 2011
Dynamically Induced Frustration as a Route to a Quantum Spin Ice State in ${Tb}_{2} {Ti}_{2} O_{7}$ via Virtual Crystal Field Excitations and Quantum Many-Body Effects Molavian, Hamid R.; Gingras, Michel J. P.; Canals, Benjamin Physical Review Letters, Vol. 98, Issue 15 https://doi.org/10.1103/PhysRevLett.98.157204	journal	April 2007
Ordered Spin Ice State and Magnetic Fluctuations in ${Tb}_{2} {Sn}_{2} O_{7}$ Mirebeau, I.; Apetrei, A.; Rodríguez-Carvajal, J. Physical Review Letters, Vol. 94, Issue 24 https://doi.org/10.1103/PhysRevLett.94.246402	journal	June 2005
Crystal field and magnetoelastic interactions in Tb2Ti2O7 Klekovkina, V. V.; Malkin, B. Z. Optics and Spectroscopy, Vol. 116, Issue 6 https://doi.org/10.1134/S0030400X14060137	journal	June 2014
Low-temperature dynamic freezing and the fragility of ordering in Tb $_{2} {Sn}_{2} O_{7}$ Dahlberg, M. L.; Matthews, M. J.; Jiramongkolchai, P. Physical Review B, Vol. 83, Issue 14 https://doi.org/10.1103/PhysRevB.83.140410	journal	April 2011
SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS Granroth, G. E.; Kolesnikov, A. I.; Sherline, T. E. Journal of Physics: Conference Series, Vol. 251 https://doi.org/10.1088/1742-6596/251/1/012058	journal	November 2010
SEQUOIA: A fine resolution chopper spectrometer at the SNS Granroth, G. E.; Vandergriff, D. H.; Nagler, S. E. Physica B: Condensed Matter, Vol. 385-386 https://doi.org/10.1016/j.physb.2006.05.379	journal	November 2006
Low temperature magnetic properties of the geometrically frustrated pyrochlores Tb2Ti2O7, Gd2Ti2O7, and Gd2Sn2O7 Luo, Gang; Hess, Steven T.; Corruccini, L. R. Physics Letters A, Vol. 291, Issue 4-5 https://doi.org/10.1016/S0375-9601(01)00734-4	journal	December 2001
Low-temperature phases of the pyrochlore compound ${Tb}_{2} {Ti}_{2} O_{7}$ Hamaguchi, Nobuko; Matsushita, Taku; Wada, Nobuo Physical Review B, Vol. 69, Issue 13 https://doi.org/10.1103/PhysRevB.69.132413	journal	April 2004
Static Correlation and Dynamical Properties of Tb ³⁺ -moments in Tb ₂ Ti ₂ O ₇ –Neutron Scattering Study– Yasui, Yukio; Kanada, Masaki; Ito, Masafumi Journal of the Physical Society of Japan, Vol. 71, Issue 2 https://doi.org/10.1143/JPSJ.71.599	journal	February 2002
Dynamic frustrated magnetism in ${Tb}_{2} {Ti}_{2} O_{7}$ at 50 mK Gardner, J. S.; Keren, A.; Ehlers, G. Physical Review B, Vol. 68, Issue 18 https://doi.org/10.1103/PhysRevB.68.180401	journal	November 2003
Low-temperature magnetization in geometrically frustrated Tb $_{2}$ Ti $_{2}$ O $_{7}$ Lhotel, E.; Paulsen, C.; de Réotier, P. Dalmas Physical Review B, Vol. 86, Issue 2 https://doi.org/10.1103/PhysRevB.86.020410	journal	July 2012
Spin Dynamics and Magnetic Order in Magnetically Frustrated ${Tb}_{2} {Sn}_{2} O_{7}$ Dalmas de Réotier, P.; Yaouanc, A.; Keller, L. Physical Review Letters, Vol. 96, Issue 12 https://doi.org/10.1103/PhysRevLett.96.127202	journal	March 2006
Direct Evidence for a Dynamical Ground State in the Highly Frustrated ${Tb}_{2} {Sn}_{2} O_{7}$ Pyrochlore Bert, F.; Mendels, P.; Olariu, A. Physical Review Letters, Vol. 97, Issue 11 https://doi.org/10.1103/PhysRevLett.97.117203	journal	September 2006
Inhomogeneous Level Splitting in $\Pr_{2 - x} {Bi}_{x} {Ru}_{2} O_{7}$ van Duijn, J.; Kim, K. H.; Hur, N. Physical Review Letters, Vol. 94, Issue 17 https://doi.org/10.1103/PhysRevLett.94.177201	journal	May 2005

Similar Records

Crystal field excitations from

{Yb}^{3 +}

ions at defective sites in highly stuffed

{Yb}_{2} {Ti}_{2} O_{7}

Journal Article · Mon Jun 11 00:00:00 EDT 2018 · Physical Review B · OSTI ID:1185348

Sala, Gabriele; Maharaj, Dalini D.; Stone, Matthew B.; +2 more

XY antiferromagnetic ground state in the effective

S = \frac{1}{2}

pyrochlore

{Yb}_{2} {Ge}_{2} O_{7}

Journal Article · Tue Mar 01 00:00:00 EST 2016 · Physical Review B · OSTI ID:1185348

Hallas, Alannah M.; Gaudet, J.; Wilson, Murray N.; +10 more

Non-Fermi-liquid types of behavior associated with a magnetic quantum critical point in

Sr {({Co}_{1 - x} {Ni}_{x})}_{2} {As}_{2}

single crystals

Journal Article · Mon Sep 30 00:00:00 EDT 2019 · Physical Review B · OSTI ID:1185348

Sangeetha, N. S.; Wang, L. -L.; Smirnov, A. V.; +6 more

Related Subjects

36 MATERIALS SCIENCE

Title: Quenched crystal-field disorder and magnetic liquid ground states in Tb 2 Sn 2 - x Ti x O 7 [Crystal field disorder in the quantum spin ice ground state of Tb2Sn2-xTixO7]

Citation Formats

References (40)

Similar Records

Related Subjects

Title: Quenched crystal-field disorder and magnetic liquid ground states in ${Tb}_{2} {Sn}_{2 - x} {Ti}_{x} O_{7}$ [Crystal field disorder in the quantum spin ice ground state of Tb2Sn2-xTixO7]