Pressure Induced Magnetic Order in the Spin Liquid Tb2 Ti2 O7 , as Studied by SR

I. Mirebeau 1 , D. Andreica 2 , A. Amato 3 , G. Dhalenne 4 , A. Revcolevschi 4 1 Laboratoire Lon Brillouin, CEA-Saclay, 91191 Gif-sur-Yvette, France e 2 Babe-Bolyai University, Faculty of Physics, 3400 Cluj-Napoca, Romania s 3 Laboratory for Muon-Spin Spectroscopy, CH-5232 Villigen PSI, Switzerland 4 Laboratoire de Physico-Chimie de lEtat Solide UMR C8648, Universit Paris XI, 91405 Orsay Cedex, France e Tb2 Ti2 O7 is a geometrically frustrated system, spin liquid, where the Tb3+ spins uctuate down to 70 mK [1]. By neutron diraction, we observed a magnetic long range order induced by pressure below T N =2 K [2,3]. A stress along [110] axis is the key feature to induce order. Above TN , the correlations between the uctuating spins change under pressure. We have investigated, by SR under pressure (up to 13 kbar), the eect of the pressure on the spin uctuations above TN , and the coexistence of the ordered and liquid phase below TN . Our rst muons experiments SR on oriented single crystals are not fully conclusive, since the pressure was limited to 13 kbars and hydrostatic conditions. In Tb2 Ti2 O7 , the Tb3+ ions occupy a pyrochlore lattice of corner sharing tetrahedra. This lattice is fully frustrated for antiferromagnetic rst neighbor interaction, leading to a large degeneracy of the magnetic ground state, without magnetic long-range order. Low energy local excitations exist down to the lowest temperature, involving short range correlations between the uctuating spins. This correspond to the spin liquid state predicted both by classical and quantum models. The spin liquid state in Tb2 Ti2 O7 which persists down to unusually low temperatures (about 300 times lower than the typical temperature for exchange interactions) is a real challenge to theory. SR in a LF of 0.005 T [1] showed large rapidly uctuating elds, evidenced by a single exponential muon spin relaxation at all temperatures. A plateau of the relaxation rate was observed at low temperatures, with a uctuation rate of 0.04 THz. By high pressure powder neutron diraction, we observed the onset of antiferromagnetic long range order [2,3] in Tb2 Ti2 O7 below a TN value of 2 K. TN and the ordered magnetic moment can be tuned by the uniaxial pressure component of the applied pressure. Above TN , a high hydrostatic pressure increases the antiferromagnetic exchange, enhancing the amplitude of the spin uctuations in the spin liquid phase. During 2004, we have performed a rst set of SR measurements on Tb2 Ti2 O7 . The LTF and GPS spectrometers were used to check the SR results of Gardner et al. [1], while temperature scans at selected pressures (ambient pressure, 3 kbar, 6.5 kbar, 13.6 kbar) on GPD were performed with the aim of investigating the pressure effect on the uctuation rates of the magnetic moment of the Tb ion. Contrarily to the results of Gardner et al. [1], who have tted the SR spectra recorded at low temperatures using a simple exponential depolarization function, for our Tb2 Ti2 O7 sample a stretched exponential (with 1 < < 1.2) tted better the SR spectra. This might arise from fact that our sample (a single crystal) was not heat-treated. A change from a stretched exponential depolarization to a simple exponential, following a heat treatment, was already observed in a similar sample [4]. The sample used for the SR experiment under pressure was a heat-treated cylindrical single crystal (5 mm diam. 18 mm length). The sample was measured in a Cu-Be pressure cell [5] at ambient pressure, 3 kbar, 6.5 kbar and 13.6 kbar. The SR spectra were tted using a simple exponential depolarization function for the sample and a Kubo-Toyabe depolarization function for the Cu-Be pressure cell. Within the limits of the experimental errors, we have found no eect of the pressure on the uctuation rates of the Tb magnetic moments and no sign of induced magnetic ordering. These results are fully consistent with the neutron scattering results: hydrostatic pressure does not induces the magnetic transition (an uniaxial component of the applied pressure is needed to induce it). A preliminary calculation of the expected pressure eect on the uctuation rate of the Tb3+ magnetic moments (taking into account the neutron data) indicates that lower temperatures or higher pressures are needed. Therefore a new set of pressure cells (made of MP35N to be used in 2005) is under construction. A rst trial to obtain an axial component of the pressure, was unsuccessful. For this trial, at the end of our GPD beam time, Tb2 Ti2 O7 powder was used as pressure transmitting media but the obtained pressure at low T (after applying 16 kbar at room temperature) was only 3 kbar, due perhaps to the air enclosed in the p-cell together with the powder. We are still searching for the best method to apply an uniaxial pressure component on top of the hydrostatic pressure. [1] [2] [3] [4] [5] J. Gardner et al., PRL 82,1012, (1999). I. Mirebeau et al., Nature 420, 54, (2002). I. Mirebeau et al., PRL 93, 187204, (2004). P. Dalmas de Rotier, private communication. e D. Andreica, Ph.D. Thesis, ETH-Zurich, 2001

Work fully performed at SS Proposal-number: RA-04-06 Instruments: GPD, GPS, LTF