Pressure-Induced Quantum Phase Transition in the Spin-Liquid TlCuCl3

Ch. Regg1, A. Furrer1, D. Sheptyakov1, Th. Strssle2, K. Krmer3, H.-U. Gdel3 and L. Mlsi4 1 Laboratory for Neutron Scattering, ETHZ & PSI, CH-5232 Villigen PSI, Switzerland 2 Physique des Milieux Condenss, Universit Pierre et Marie Curie, F-75252 Paris, France 3 Department for Chemistry and Biochemistry, University of Berne, Freiestrasse 3, CH-3000 Bern 9, Switzerland 4 Institut Laue-Langevin, BP 156, F-38042 Grenoble Cedex 9, France The novel pressure-induced quantum phase transition in the dimer spin-liquid TlCuCl3 has been investigated by means of elastic and inelastic neutron scattering. The latter demonstrates the softening of the relevant triplet excitations at the critical pressure pc . The former provides the pressure-temperature phase diagram with long-range antiferromagnetic order above pc . The condensation of magnetic quasi-particles (triplet excitations with total spin S=1) into the non-magnetic ground state (singlet with S=0) has been used to explain novel magnetic ordering phenomena observed in quantum spin systems [1,2]. The neutron scattering results across the pressure-induced quantum phase transition and for the novel ordered phase of the magnetic insulator TlCuCl3 are consistent with the theoretically predicted two degenerate "gapless" Goldstone modes, similar to the low-energy spin excitations in the field-induced case. These experimental findings complete the field-induced Bose-Einstein condensate picture and supports the recently proposed fieldpressure phase diagram common for quantum spin systems with an energy gap of singlet-triplet nature, see Fig. 1.
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6 5 Energy [meV]

Magnetic field [T]

c
8 6 4 2

4 3 2 1 0

e
-0.5 0.0 0.5 Momentum (0 qk 0) [r.l.u]

AF SL
0.50

pressure-cell (aluminum/TiZr, p=7.3(5) kbar) and a tunable 4 He-gas pressure-cell (p<5 kbar). The pressure-dependence of the singlet-triplet spin energy gap (p) has been measured up to p=2.0 kbar. The results are summarized in Fig. 2. We observe a softening of the gap for increasing 0<p<pc . The INS spectra at pc <p<2 kbar are consistent, within instrumental resolution, with a gapless excitation spectrum and the spin waves at p=7.3 kbar show an increased stiffness. Neutron diffraction experiments have been performed to observe long-range magnetic order above pc . The Nel temperature as a function of pressure TN(p) is extracted from the characteristic temperature-dependence of magnetic Bragg peaks. A combined fit to (p) and T N(p) yields pc =1.07(1) kbar, see Fig. 1. These results clearly demonstrate that dimer quantum spin systems with a spin energy gap of singlet-triplet nature can be driven to an ordered phase by external pressure. The driving mechanism for the quantum phase transition is hereby the change in the exchange interactions closing the spin gap at p c . A detailed discussion of the present study can be found in Ref. [3].
1 0.8

pc=1.07(1) kbar

10 8

a
0 0.00

d
[meV]
1.00 1.50 8.00

0.6

TN [K]

Pressure [kbar]
Figure 1: Magnetic field versus pressure phase diagram for the dimer compound TlCuCl 3 at T=0 K. A square root phase boundary separates the spin-liquid phase (SL) from the antiferromagnetic phase (AF). Insets: Spin dynamics around the AF zone center [1], Q=q+=(0 qk 0)+(0 4 0) in reciprocal lattice units [r.l.u.]. Common scale for (a)-(e), possible anisotropy gaps are not considered. (a) Degenerate triplet modes. (b) Zeeman split triplet modes at Hc . (c) Spin dynamics in the field-induced ordered phase [2]. (d) Degenerate and linear triplet modes close the spin energy gap at the critical pressure pc . (e) Spin dynamics in the pressure-induced ordered phase [3]. Two degenerate transverse Goldstone modes (solid line) and a longitudinal amplitude mode (dashed line) are expected [1]. Elastic and inelastic neutron scattering experiments have been performed on the triple-axis spectrometer TASP (SINQ, PSI) to investigate the novel pressure-induced quantum phase transition in TlCuCl3. Single crystals (sample masses 0.5 g and 2.0 g) were mounted in a clamp

0.4

TN(p) (p), T=1.85 K

6 4 2 0

0.2

SL
0 1 2

AF
3 4 5

Pressure [kbar]

Figure 2: Pressure-induced quantum phase transition in TlCuCl3 between spin-liquid (SL) and antiferromagnetic (AF) phase. Singlet-triplet gap (p) and Nel temperature TN(p) measured at Q=(0 0 1) r.l.u. [1] [2] [3] M. Matsumoto et al., Phys. Rev. B 69, 054423 (2004). Ch. Regg et al., Nature 423, 62 (2003). Ch. Regg et al., Phys. Rev. Lett. 93, 257201 (2004). Work fully performed at SINQ Proposal-number: II/04-S100, II/03-S59 Instruments: TASP