Critical X-ray Scattering Studies of Jahn-Teller Phase Transitions in TbV1−x_{1-x}Asx_{x}O4_{4}

The critical behaviour associated with cooperative Jahn-Teller phase transitions in TbV$_{1-x}$As$_{x}$O$_{4}$ (where \textit{x} = 0, 0.17, 1) single crystals have been studied using high resolution x-ray scattering. These materials undergo continuous tetragonal $\to$ orthorhombic structural phase transitions driven by Jahn-Teller physics at T$_C$ = 33.26(2) K, 30.32(2) K and 27.30(2) K for \textit{x} = 0, 0.17 and 1 respectively. The orthorhombic strain was measured close to the phase transition and is shown to display mean field behavior in all three samples. Pronounced fluctuation effects are manifest in the longitudinal width of the Bragg scattering, which diverges as a power law, with an exponent given by $x=0.45 \pm 0.04$, on approaching the transition from either above or below. All samples exhibited twinning; however the disordered x = 0.17 sample showed a broad distribution of twins which were stable to relatively low temperatures, well below T$_C$. This indicates that while the orthorhombic strain continues to develop in a conventional mean field manner in the presence of disorder, twin domains are easily pinned by the quenched impurities and their associated random strains.Comment: 8 pages, 6 figure

Neutron spectroscopic study of crystal field excitations in Tb2Ti2O7 and Tb2Sn2O7

We present time-of-flight inelastic neutron scattering measurements at low temperature on powder samples of the magnetic pyrochlore oxides Tb2Ti2O7 and Tb2Sn2O7. These two materials possess related, but different ground states, with Tb2Sn2O7 displaying "soft" spin ice order below Tn~0.87 K, while Tb2Ti2O7 enters a hybrid, glassy spin ice state below Tg~0.2 K. Our neutron measurements, performed at T=1.5 K and 30 K, probe the crystal field states associated with the J=6 states of Tb3+ within the appropriate Fd\bar{3}m pyrochlore environment. These crystal field states determine the size and anisotropy of the Tb3+ magnetic moment in each material's ground state, information that is an essential starting point for any description of the low-temperature phase behavior and spin dynamics in Tb2Ti2O7 and Tb2Sn2O7. While these two materials have much in common, the cubic stanate lattice is expanded compared to the cubic titanate lattice. As our measurements show, this translates into a factor of ~2 increase in the crystal field bandwidth of the 2J+1=13 states in Tb2Ti2O7 compared with Tb2Sn2O7. Our results are consistent with previous measurements on crystal field states in Tb2Sn2O7, wherein the ground state doublet corresponds primarily to m_J=|\pm 5> and the first excited state doublet to mJ=|\pm 4>. In contrast, our results on Tb2Ti2O7 differ markedly from earlier studies, showing that the ground state doublet corresponds to a significant mixture of mJ=|\pm 5>, |\mp 4>, and |\pm 2>, while the first excited state doublet corresponds to a mixture of mJ=|\pm 4>, |\mp 5>, and |\pm 1>. We discuss these results in the context of proposed mechanisms for the failure of Tb2Ti2O7 to develop conventional long-range order down to 50 mK.Comment: 12 pages, 6 figures. Version is the same as the published one, except for figure placement on page

Spin Waves in the Ferromagnetic Ground State of the Kagome Staircase System Co3V2O8

Inelastic neutron scattering measurements were performed on single crystal Co3V2O8 wherein magnetic cobalt ions reside on distinct spine and cross-tie sites within kagome staircase planes. This system displays a rich magnetic phase diagram which culminates in a ferromagnetic ground state below Tc~6 K. We have studied the low-lying magnetic excitations in this phase within the kagome plane. Despite the complexity of the system at higher temperatures, linear spin-wave theory describes most of the quantitative detail of the inelastic neutron measurements. Our results show two spin-wave branches, the higher energy of which displays finite spin-wave lifetimes well below Tc, and negligible magnetic exchange coupling between Co moments on the spine sites.Comment: 4 pages and 4 figure

High resolution X-ray scattering studies of structural phase transitions in underdoped La2−x_{2-x}Bax_xCuO4_4

We have studied structural phase transitions in high quality underdoped La$_{2-x}$Ba$_x$CuO$_4$ single crystals using high resolution x-ray scattering techniques. Critical properties associated with the continuous High Temperature Tetragonal (HTT, $I4/mmm$) to Middle Temperature Orthorhombic (MTO, $Cmca$) phase transition were investigated in single crystal samples with x=0.125, 0.095, and 0.08 and we find that all behavior is consistent with three dimensional XY criticality, as expected from theory. Power law behavior in the orthorhombic strain, 2(a-b)/(a+b), is observed over a remarkably wide temperature range, spanning most of the MTO regime in the phase diagram. Low temperature measurements investigating the Low Temperature Tetragonal (LTT, $P4_{2}/ncm$) phase, below the strongly discontinuous MTO$\to$LTT phase transition, in x=0.125 and x=0.095 samples show that the LTT phase is characterized by relatively broad Bragg scattering, compared with that observed at related wavevectors in the HTT phase. This shows that the LTT phase is either an admixture of tetragonal and orthorhombic phases, or that it is orthorhombic with very small orthorhombic strain, consistent with the ``less orthorhombic" low temperature structure previously reported in mixed La$_{2-x}$Sr$_{x-y}$Ba$_y$CuO$_4$ single crystals. We compare the complex temperature-composition phase diagram for the location of structural and superconducting phase transitions in underdoped La$_{2-x}$Ba$_x$CuO$_4$ and find good agreement with results obtained on polycrystalline samples.Comment: 8 pages, 7 figures, 1 tabl

Quenched crystal field disorder and magnetic liquid ground states in Tb2Sn2-xTixO7

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 Tb2Sn2-xTixO7) 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.Comment: 6 pages, 6 figure

Lack of Evidence for a Singlet Crystal Field Ground State in the Tb2Ti2O7 Magnetic Pyrochlore

We present new high resolution inelastic neutron scattering data on the candidate spin liquid Tb2Ti2O7. We find that there is no evidence for a zero field splitting of the ground state doublet within the 0.2 K resolution of the instrument. This result contrasts with a pair of recent works on Tb2Ti2O7 claiming that the spin liquid behavior can be attributed to a 2 K split singlet-singlet single-ion spectrum at low energies. We also reconsider the entropy argument presented in Chapuis {\it et al.} as further evidence of a singlet-singlet crystal field spectrum. We arrive at the conclusion that estimates of the low temperature residual entropy drawn from heat capacity measurements are a poor guide to the single ion spectrum without understanding the nature of the correlations.Comment: 4 pages, 3 figure. Submitted to Physical Review