Emergence of long-range order in sheets of magnetic dimers.

Quantum spins placed on the corners of a square lattice can dimerize and form singlets, which then can be transformed into a magnetic state as the interactions between dimers increase beyond threshold. This is a strictly 2D transition in theory, but real-world materials often need the third dimension to stabilize long-range order. We use high pressures to convert sheets of Cu(2+) spin 1/2 dimers from local singlets to global antiferromagnet in the model system SrCu2(BO3)2. Single-crystal neutron diffraction measurements at pressures above 5 GPa provide a direct signature of the antiferromagnetic ordered state, whereas high-resolution neutron powder and X-ray diffraction at commensurate pressures reveal a tilting of the Cu spins out of the plane with a critical exponent characteristic of 3D transitions. The addition of anisotropic, interplane, spin-orbit terms in the venerable Shastry-Sutherland Hamiltonian accounts for the influence of the third dimension.

Continuous and discontinuous quantum phase transitions in a model two-dimensional magnet.

The Shasty-Sutherland model, which consists of a set of spin 1/2 dimers on a 2D 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, SrCu(2)(BO(3))(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.

Order parameter fluctuations at a buried quantum critical point.

Quantum criticality is a central concept in condensed matter physics, but the direct observation of quantum critical fluctuations has remained elusive. Here we present an X-ray diffraction study of the charge density wave (CDW) in 2H-NbSe(2) at high pressure and low temperature, where we observe a broad regime of order parameter fluctuations that are controlled by proximity to a quantum critical point. X-rays can track the CDW despite the fact that the quantum critical regime is shrouded inside a superconducting phase; and in contrast to transport probes, allow direct measurement of the critical fluctuations of the charge order. Concurrent measurements of the crystal lattice point to a critical transition that is continuous in nature. Our results confirm the long-standing expectations of enhanced quantum fluctuations in low-dimensional systems, and may help to constrain theories of the quantum critical Fermi surface.

Crystallization of spin superlattices with pressure and field in the layered magnet SrCu2(BO3)2.

An exact mapping between quantum spins and boson gases provides fresh approaches to the creation of quantum condensates and crystals. Here we report on magnetization measurements on the dimerized quantum magnet SrCu2(BO3)2 at cryogenic temperatures and through a quantum-phase transition that demonstrate the emergence of fractionally filled bosonic crystals in mesoscopic patterns, specified by a sequence of magnetization plateaus. We apply tens of Teslas of magnetic field to tune the density of bosons and gigapascals of hydrostatic pressure to regulate the underlying interactions. Simulations help parse the balance between energy and geometry in the emergent spin superlattices. The magnetic crystallites are the end result of a progression from a direct product of singlet states in each short dimer at zero field to preferred filling fractions of spin-triplet bosons in each dimer at large magnetic field, enriching the known possibilities for collective states in both quantum spin and atomic systems.

In-gap spin excitations and finite triplet lifetimes in the dilute singlet ground state system SrCu(2-x)Mgx(BO3)2.

High resolution neutron scattering measurements on a single crystal of SrCu(2-x)Mgx(BO3)2 with x approximately 0.05 reveal the presence of new spin excitations within the gap of this quasi-two-dimensional, singlet ground state system. The application of a magnetic field induces Zeeman-split states associated with S=1/2 unpaired spins which are antiferromagnetically correlated with the bulk singlet. Substantial broadening of both the one- and two-triplet excitations in the doped single crystal is observed, as compared with pure SrCu2(BO3)2. Theoretical calculations using a variational algorithm and a single quenched magnetic vacancy on an infinite lattice are shown to qualitatively account for these effects.

High-resolution study of spin excitations in the singlet ground state of SrCu2(BO3)2.

High-resolution, inelastic neutron scattering measurements on SrCu2(BO3)2, a realization of the Shastry-Sutherland model for two-dimensional Heisenberg antiferromagnets, reveal the dispersion of the three single triplet excitations continuously across the (H,0) direction within its tetragonal basal plane. These measurements also show distinct Q dependencies for the single and multiple triplet excitations, and that these excitations are largely dispersionless perpendicular to this plane. The temperature dependence of the intensities of these excitations is well described as the complement of the dc susceptibility of SrCu2(BO3)2.