Nature of the ferromagnetic-antiferromagnetic transition in Y$_{1-x}$La$_{x}$TiO$_{3}$
S. Hameed,
S. El-Khatib,
K. P. Olson
et al.
Abstract:We explore the magnetically-ordered ground state of the isovalently-substituted Mott-insulator Y1−xLaxTiO3 for x ≤ 0.3 via single crystal growth, magnetometry, neutron diffraction, x-ray magnetic circular dichroism (XMCD), muon spin rotation (µSR) and small-angle neutron scattering (SANS). We find that the decrease in the magnetic transition temperature on approaching the ferromagnetic (FM) -antiferromagnetic (AFM) phase boundary at the La concentration xc ≈ 0.3 is accompanied by a strong suppression of both b… Show more
“…For the growth of Y 1−x La x TiO 3 single crystals, we fixed the value of δ at 0.04, i.e., the same value as for YTiO 3 in order to avoid property changes due to differences in oxygen off-stoichiometry in the starting material composition 8 . Intriguingly, however, we found that, at large x, the changes in T C along the growth axis can be particularly severe.…”
Section: B Characterization Of Y1−xlaxtio3 Single Crystalsmentioning
confidence: 99%
“…For our own inelastic neutron measurements of the spin-wave spectra at large La-substitution levels, we used samples from the latter parts of the growths that exhibit a nearly constant T C . Given the strong suppression of the ordered moments exhibited by these samples with La substitution 8 , it was necessary to co-mount samples from many different growths, in order to obtain a sufficiently large signal-to-noise ratio (see Fig. 6) 21 .…”
Section: B Characterization Of Y1−xlaxtio3 Single Crystalsmentioning
confidence: 99%
“…display a ferromagnetic ground state 1,3,4 . The phase-transition/cross-over can also be induced in solidsolution systems formed by isovalent substitution, e.g., Y 1−x La x TiO 3 [5][6][7][8] and Sm 1−x Gd x TiO 3 9 . It is also possible to tune RTiO 3 from a Mott insulator to a metallic state via hole doping, which can be achieved by substituting the trivalent R 3+ ion with a divalent A 2+ ion such as Ca 2+ or Sr 2+ to form R 1−y A y TiO 3 .…”
Section: Introductionmentioning
confidence: 99%
“…Here we describe our efforts to grow large single crystals of La-substituted and Ca-doped YTiO 3 with the traveling solvent floating zone (TSFZ) technique, to enable neutron scattering and muon spin rotation studies of the magnetic ground state 8 . We carefully character-ized the changes in properties that can appear across large single crystals using chemical composition analysis, magnetometry, charge transport, elastic and inelastic neutron scattering, x-ray diffraction, x-ray absorption spectroscopy and x-ray magnetic circular dichroism.…”
Section: Introductionmentioning
confidence: 99%
“…Our goal here is to provide a comprehensive report on the growth of large single crystals of Y 1−x La x TiO 3 and Y 1−y Ca y TiO 3 , so as to aid future studies of this important class of quantum materials. Some of these crystals were used in recent studies of the ferromagnetantiferromagnet transition in Y 1−x La x TiO 3 8 , the Mott insulator-metal transition in Y 1−y Ca y TiO 3 12 , and the effect of uniaxial strain on the magnetic ground state in these systems 22 .…”
The Mott-insulating rare-earth titanates (RTiO3, R being a rare-earth ion) are an important class of materials that encompasses interesting spin-orbital phases as well as ferromagnet-antiferromagnet and insulator-metal transitions. The growth of these materials has been plagued by difficulties related to overoxidation, which arises from a strong tendency of Ti 3+ to oxidize to Ti 4+ . We describe our efforts to grow sizable single crystals of YTiO3 and its La-substituted and Ca-doped variants with the optical travelling-solvent floating-zone technique. We present sample characterization via chemical composition analysis, magnetometry, charge transport, neutron scattering, x-ray absorption spectroscopy and x-ray magnetic circular dichroism to understand macroscopic physical property variations associated with overoxidation. Furthermore, we demonstrate a good signal-to-noise ratio in inelastic magnetic neutron scattering measurements of spin-wave excitations. A superconducting impurity phase, found to appear in Ca-doped samples at high doping levels, is identified as TiO.
“…For the growth of Y 1−x La x TiO 3 single crystals, we fixed the value of δ at 0.04, i.e., the same value as for YTiO 3 in order to avoid property changes due to differences in oxygen off-stoichiometry in the starting material composition 8 . Intriguingly, however, we found that, at large x, the changes in T C along the growth axis can be particularly severe.…”
Section: B Characterization Of Y1−xlaxtio3 Single Crystalsmentioning
confidence: 99%
“…For our own inelastic neutron measurements of the spin-wave spectra at large La-substitution levels, we used samples from the latter parts of the growths that exhibit a nearly constant T C . Given the strong suppression of the ordered moments exhibited by these samples with La substitution 8 , it was necessary to co-mount samples from many different growths, in order to obtain a sufficiently large signal-to-noise ratio (see Fig. 6) 21 .…”
Section: B Characterization Of Y1−xlaxtio3 Single Crystalsmentioning
confidence: 99%
“…display a ferromagnetic ground state 1,3,4 . The phase-transition/cross-over can also be induced in solidsolution systems formed by isovalent substitution, e.g., Y 1−x La x TiO 3 [5][6][7][8] and Sm 1−x Gd x TiO 3 9 . It is also possible to tune RTiO 3 from a Mott insulator to a metallic state via hole doping, which can be achieved by substituting the trivalent R 3+ ion with a divalent A 2+ ion such as Ca 2+ or Sr 2+ to form R 1−y A y TiO 3 .…”
Section: Introductionmentioning
confidence: 99%
“…Here we describe our efforts to grow large single crystals of La-substituted and Ca-doped YTiO 3 with the traveling solvent floating zone (TSFZ) technique, to enable neutron scattering and muon spin rotation studies of the magnetic ground state 8 . We carefully character-ized the changes in properties that can appear across large single crystals using chemical composition analysis, magnetometry, charge transport, elastic and inelastic neutron scattering, x-ray diffraction, x-ray absorption spectroscopy and x-ray magnetic circular dichroism.…”
Section: Introductionmentioning
confidence: 99%
“…Our goal here is to provide a comprehensive report on the growth of large single crystals of Y 1−x La x TiO 3 and Y 1−y Ca y TiO 3 , so as to aid future studies of this important class of quantum materials. Some of these crystals were used in recent studies of the ferromagnetantiferromagnet transition in Y 1−x La x TiO 3 8 , the Mott insulator-metal transition in Y 1−y Ca y TiO 3 12 , and the effect of uniaxial strain on the magnetic ground state in these systems 22 .…”
The Mott-insulating rare-earth titanates (RTiO3, R being a rare-earth ion) are an important class of materials that encompasses interesting spin-orbital phases as well as ferromagnet-antiferromagnet and insulator-metal transitions. The growth of these materials has been plagued by difficulties related to overoxidation, which arises from a strong tendency of Ti 3+ to oxidize to Ti 4+ . We describe our efforts to grow sizable single crystals of YTiO3 and its La-substituted and Ca-doped variants with the optical travelling-solvent floating-zone technique. We present sample characterization via chemical composition analysis, magnetometry, charge transport, neutron scattering, x-ray absorption spectroscopy and x-ray magnetic circular dichroism to understand macroscopic physical property variations associated with overoxidation. Furthermore, we demonstrate a good signal-to-noise ratio in inelastic magnetic neutron scattering measurements of spin-wave excitations. A superconducting impurity phase, found to appear in Ca-doped samples at high doping levels, is identified as TiO.
Rare-earth titanates are Mott insulators whose magnetic ground state -antiferromagnetic (AFM) or ferromagnetic (FM) -can be tuned by the radius of the rare-earth element. Here, we combine phenomenology and first-principles calculations to shed light on the generic magnetic phase diagram of a chemically-substituted titanate on the rare-earth site that interpolates between an AFM and a FM state. Octahedral rotations present in these perovskites cause the AFM order to acquire a small FM component -and vice-versa -removing any multi-critical point from the phase diagram. However, for a wide parameter range, a first-order metamagnetic transition line terminating at a critical end-point survives inside the magnetically ordered phase. Similarly to the liquid-gas transition, a Widom line emerges from the end-point, characterized by enhanced fluctuations. In contrast to metallic ferromagnets, this metamagnetic transition involves two symmetry-equivalent and insulating canted spin states. Moreover, instead of a magnetic field, we show that uniaxial strain can be used to tune this transition to zero-temperature, inducing a quantum critical end-point.
The perovskite rare-earth titanates are model Mott insulators with magnetic ground states that are sensitive to structural distortions. These distortions couple strongly to the orbital degrees of freedom and, in principle, it should be possible to tune the superexchange and to manipulate the Curie temperature (TC ) with strain. We investigate the representative system (Y,La,Ca)TiO3, which exhibits low crystallographic symmetry and no structural instabilities. From magnetic susceptibility measurements of TC , we demonstrate direct, reversible and continuous control of ferromagnetism by influencing the TiO6 octahedral tilts and rotations with uniaxial strain. The relative change in TC as a function of strain is well described by ab initio calculations, which provides detailed understanding of the complex interactions among structural, orbital and magnetic properties in these compounds. The demonstrated manipulation of octahedral distortions opens up far-reaching possibilities for investigations of electron-lattice coupling, competing ground states and magnetic quantum phase transitions in a wide range of quantum materials.
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