MAGNETIC EXCITATIONS IN A QUANTUM SPIN LIQUID ACROSS Hc PART 1

N. Cavadini 1, Ch. Regg1, A. Furrer1, K. Krmer2, H.U. Gdel2, K. Habicht3, P. Vorderwisch3 Laboratory for Neutron Scattering, ETH Zurich & Paul Scherrer Institute, CH-5232 Villigen PSI 2 Department for Chemistry and Biochemistry, University of Berne, CH-3000 Bern 9 3 BENSC, Hahn-Meitner-Institut, D-14109 Berlin Wannsee

Field-driven magnetic ordering occurs in three-dimensional quantum spin liquids when the Zeeman energy g BH overcomes the singlet-triplet energy gap of the elementary excitations. Virtually nothing is known about the excitations in this novel state. The dynamic framework of the field-driven magnetic ordering in S=1/2 spin liquid TlCuCl3 is illustrated for the first time by means of inelastic neutron scattering. Increasing interest is devoted to the occurrence of quantum phase transitions in solid state physics. Quantum magnetism is the ideal testing ground for novel predictions, but appropriate scientific cases in neutron scattering often suffers from intrinsic sample limitations. S=1/2 spin liquid TlCuCl3 is an exception of recent interest [1-3]. The modest energy gap /gB=6T allows in TlCuCl 3 experimental access to a quantum phase transition, which at T=0 separates quantum disorder from field-driven order. By means of neutron diffraction the value of the staggered magnetization M(H)=0.26B per Cu 2 + at H=12T was recently determined [2]. Extending the above investigations to the excited states, a study of the magnetic spectrum in the field range 0<H<12T is presented in the following [3]. Measurements were performed on the cold neutron spectrometer FLEX (HMI, Berlin), operated at fixed final energy Ef =4.7meV with a Be filter in front of the analyzer. A large TlCuCl3 single crystal oriented in the scattering plane spanned by the (0,2,0) and (1,0,4) Bragg reflections was mounted in the VM-1 cryomagnet and kept at T=1.5K. Above Hc=6T, the field dependent profiles observed at the excitation minimum Q=(0,4,0) r.l.u. consist of two sharp transitions, corresponding to the renormalized |1-1 and |10 Zeeman states (Figure 1). A simple picture based on dimer states in an effective internal field captures the experimental observations, under consideration of
3.5 3 2.5 2 1.5 1 0.5 0

Energy [meV]

10

12

Field strength [T]

Fig 1: Energies of the Zeeman transitions observed in TlCuCl 3 at fixed T=1.5K, from [3]. The hatched area denotes the additional intensity evidenced at H=12T.

H=6 T

Norm. intensity [a. u.]

H=9 T

H = H D + HZ + HMF

(1)
H=12 T

where H D denotes the zero-field dimer interaction term, HZ the external Zeeman term, HMF the staggered internal mean-field term [3]. The latter accounts for the field-induced transverse antiferromagnetic order and is responsible for the mixing of the elementary dimer states, justifying the observed spectral transitions. From Eq. (1), an additional low-lying transition corresponding to the renormalized |11 Zeeman state is expected. The flank of the incoherent line prevented the complete investigation of this issue due to the finite energy resolution. Nevertheless, evidence for additional low-lying intensity is reported from the measurements performed at H=12T (Figure 2, arrow). The broad nature of the additional intensity casts doubts on the validity of the Zeeman description for the soft mode. Further experimental efforts conclusively elucidate its nature as presented in Part 2.

0.0

0.5

1.0

1.5

2.0

2.5

3.0

3.5

4.0

Energy [meV]

Fig 2: Representative neutron spectra observed in TlCuCl 3 at fixed T=1.5K, from [3]. Instrumental set-up and experimental outcomes are commented in the text.

[1] N. Cavadini et al., Phys. Rev. B 63, 172414 (2001). [2] H. Tanaka et al., J. Phys. Soc. Jpn. 70, 939 (2001). [3] Ch. Regg et al., Appl. Phys. A (at press).