The degree of contact between a system and the external environment can alter dramatically its proclivity to quantum mechanical modes of relaxation. We show that controlling the thermal coupling of cubic centimeter-sized crystals of the Ising magnet
$LiHo_xY_{1-x}F_4$ to a heat bath can be used to tune the system between a glassy state dominated by thermal excitations over energy barriers and a state with the hallmarks of a quantum spin liquid. Application of a magnetic field transverse to the Ising axis introduces both random magnetic fields and quantum fluctuations, which can retard and speed the annealing process, respectively, thereby providing a mechanism for continuous tuning between the destination states. The non-linear response of the system explicitly demonstrates quantum interference between internal and external relaxation pathways.
The Shastry-Sutherland model, which consists of a set of spin 1/2 dimers on a 2-dimensional square lattice, is simple and soluble, but captures a central theme of condensed matter physics by sitting precariously on the quantum edge between isolated,
gapped excitations and collective, ordered ground states. We compress the model Shastry-Sutherland material, SrCu2(BO3)2, in a diamond anvil cell at cryogenic temperatures to continuously tune the coupling energies and induce changes in state. High-resolution x-ray measurements exploit what emerges as a remarkably strong spin-lattice coupling to both monitor the magnetic behavior and the absence or presence of structural discontinuities. In the low-pressure spin-singlet regime, the onset of magnetism results in an expansion of the lattice with decreasing temperature, which permits a determination of the pressure dependent energy gap and the almost isotropic spin-lattice coupling energies. The singlet-triplet gap energy is suppressed continuously with increasing pressure, vanishing completely by 2 GPa. This continuous quantum phase transition is followed by a structural distortion at higher pressure.
When performed in the proper low field, low frequency limits, measurements of the dynamics and the nonlinear susceptibility in the model Ising magnet in transverse field, $text{LiHo}_xtext{Y}_{1-x}text{F}_4$, prove the existence of a spin glass trans
ition for $x$ = 0.167 and 0.198. The classical behavior tracks for the two concentrations, but the behavior in the quantum regime at large transverse fields differs because of the competing effects of quantum entanglement and random fields.
A transverse magnetic field is used to scan the diagonal and off-diagonal susceptibility of the uniaxial quantum magnet, $text{LiHo}_{0.045}text{Y}_{0.955}text{F}_4$. Clusters of strongly-coupled spins act as the primary source for the response funct
ions, which result from a field-induced quantum projection of the system into a classically forbidden (meaning non-Ising) regime. Calculations based on spin pairs reproduce only some features of the data and fail to predict the measured off-diagonal response, providing evidence of a multi-spin collective state.
