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.

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.

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.

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.

Breakdown of the Bardeen-Cooper-Schrieffer ground state at a quantum phase transition.

Advances in solid-state and atomic physics are exposing the hidden relationships between conventional and exotic states of quantum matter. Prominent examples include the discovery of exotic superconductivity proximate to conventional spin and charge order, and the crossover from long-range phase order to preformed pairs achieved in gases of cold fermions and inferred for copper oxide superconductors. The unifying theme is that incompatible ground states can be connected by quantum phase transitions. Quantum fluctuations about the transition are manifestations of the competition between qualitatively distinct organizing principles, such as a long-wavelength density wave and a short-coherence-length condensate. They may even give rise to 'protected' phases, like fluctuation-mediated superconductivity that survives only in the vicinity of an antiferromagnetic quantum critical point. However, few model systems that demonstrate continuous quantum phase transitions have been identified, and the complex nature of many systems of interest hinders efforts to more fully understand correlations and fluctuations near a zero-temperature instability. Here we report the suppression of magnetism by hydrostatic pressure in elemental chromium, a simple cubic metal that demonstrates a subtle form of itinerant antiferromagnetism formally equivalent to the Bardeen-Cooper-Schrieffer (BCS) state in conventional superconductors. By directly measuring the associated charge order in a diamond anvil cell at low temperatures, we find a phase transition at pressures of approximately 10 GPa driven by fluctuations that destroy the BCS-like state but preserve the strong magnetic interaction between itinerant electrons and holes. Chromium is unique among stoichiometric magnetic metals studied so far in that the quantum phase transition is continuous, allowing experimental access to the quantum singularity and a direct probe of the competition between conventional and exotic order in a theoretically tractable material.

Magnetic structure of RuSr2GdCu2O8 determined by resonant x-ray diffraction.

X-ray diffraction with photon energies near the Ru L2-absorption edge was used to detect resonant reflections characteristic of a G-type superstructure in RuSr2GdCu2O8 single crystals. A polarization analysis confirms that these reflections are due to magnetic order of Ru moments, and the azimuthal-angle dependence of the scattering amplitude reveals that the moments lie along a low-symmetry axis with substantial components parallel and perpendicular to the RuO2 layers. Complemented by susceptibility data and a symmetry analysis of the magnetic structure, these results reconcile many of the apparently contradictory findings reported in the literature.

Pressure-tuned spin and charge ordering in an itinerant antiferromagnet.

Elemental chromium orders antiferromagnetically near room temperature, but the ordering temperature can be driven to zero by applying large pressures. We combine diamond anvil cell and synchrotron x-ray diffraction techniques to measure directly the spin and charge order in the pure metal at the approach to its quantum critical point. Both spin and charge order are suppressed exponentially with pressure, well beyond the region where disorder cuts off such a simple evolution, and they maintain a harmonic scaling relationship over decades in scattering intensity. By comparing the development of the order parameter with that of the magnetic wave vector, it is possible to ascribe the destruction of antiferromagnetism to the growth in electron kinetic energy relative to the underlying magnetic exchange interaction.

Role of Ge in bridging ferromagnetism in the giant magnetocaloric Gd5(Ge1-xSix)4 alloys.

X-ray magnetic circular dichroism (XMCD) measurements and density functional theory (DFT) are used to study the electronic conduction states in Gd5(Ge(1-x)Si(x))4 materials through the first-order bond-breaking magnetostructural transition responsible for their giant magnetocaloric effect. Spin-dependent hybridization between Ge 4p and Gd 5d conduction states, which XMCD senses through the induced magnetic polarization in Ge ions, enables long-range Ruderman-Kittel-Kasuya-Yosida ferromagnetic interactions between Gd 4f moments in adjacent Gd slabs connected by Ge(Si) bonds. These interactions are strong below but weaken above the Ge(Si) bond-breaking transition that destroys 3D ferromagnetic order.

Ferrimagnetism in EuFe4Sb12 due to the interplay of f-electron moments and a nearly ferromagnetic host.

We combine x-ray magnetic circular dichroism spectroscopy at Fe L2,3 edges, at Eu M4,5 edges, x-ray absorption spectroscopy (XAS) investigation of Eu valence, and local spin density calculations, to show that the filled skutterudite Eu0.95Fe4Sb12 is a ferrimagnet in which the Fe 3d moment and the Eu2+ 4f moment are magnetically ordered with dominant antiferromagnetic coupling. From Eu L3 edge XAS, we find that about 13% of the Eu have a formal valence of 3+. We ascribe the origin of ferrimagnetism at a relatively high transition temperature TC of 85 K in Eu0.95Fe4Sb12 to f-electron interaction with the nearly ferromagnetic [Fe4Sb12]2.2- host lattice.

Non-resonant and resonant x-ray scattering studies on multiferroic TbMn2O5.

Comprehensive x-ray scattering studies, including resonant scattering at Mn L, Tb L, and M edges, were performed on single crystals of TbMn2O5 for crystallographic data to elucidate the nature of its commensurate and incommensurate phases. The scattering results provide direct evidence of symmetry lowering to the ferroelectric phase driven by magnetically induced lattice modulations and show the presence of multiple magnetic orders. The competing orders under spin-frustrated geometry are believed to cause discommensuration and result in the commensurate-to-incommensurate phase transition around 24 K. It is proposed that the low temperature incommensurate phase consists of commensurate domains separated by antiphase domain walls which change both signs of spontaneous polarizations and x-ray scattering amplitudes for forbidden reflections.

Atomic origin of magnetocrystalline anisotropy in Nd(2)Fe(14)B.

The magnetic moment reversal at each of the two inequivalent Nd sites in a single crystal of ferromagnetic Nd(2)Fe(14)B is probed by dichroic resonant diffraction of circularly polarized x rays. The results, supported by theory, show that the c-axis intrinsic magnetic stability of this superior permanent magnetic material arises predominantly at one of the Nd sites (g). The other site (f) undermines magnetic stability by favoring a magnetic moment orientation in the basal plane.

Orbital ordering transition in Ca2RuO4 observed with resonant X-ray diffraction.

Resonant x-ray diffraction performed at the L(II) and L(III) absorption edges of Ru has been used to investigate the magnetic and orbital ordering in Ca2RuO4 single crystals. A large resonant enhancement due to electric dipole 2p-->4d transitions is observed at the wave-vector characteristic of antiferromagnetic ordering. Besides the previously known antiferromagnetic phase transition at T(N)=110 K, an additional phase transition, between two paramagnetic phases, is observed around 260 K. Based on the polarization and azimuthal angle dependence of the diffraction signal, this transition can be attributed to orbital ordering of the Ru t(2g) electrons. The propagation vector of the orbital order is inconsistent with some theoretical predictions for the orbital state of Ca2RuO4.

Four-unit-cell superstructure in the optimally doped YBa2Cu3O6.92 superconductor.

Diffuse x-ray scattering measurements reveal that the optimally doped YBa2Cu3O6.92 superconductor is intrinsically modulated due to the formation of a kinetically limited 4-unit-cell superlattice, q(0)=(1/4, 0, 0), along the shorter Cu-Cu bonds. The superlattice consists of large anisotropic displacements of Cu, Ba, and O atoms, respectively, which are correlated over approximately 3-6 unit cells in the ab plane, and appears to be consistent with the presence of an O-ordered "ortho-IV" phase. Long-range strains emanating from these modulated regions generate an inhomogeneous lattice which may play a fundamentally important role in the electronic properties of yttrium-barium-copper-oxides.

Interlayer structures of the chiral smectic liquid crystal phases revealed by resonant X-ray scattering.

The structures of the liquid crystalline chiral subphases exhibited by several materials containing either a selenium or sulphur atom have been investigated using a resonant x-ray scattering technique. This technique provides a unique structural probe for the ferroelectric, ferrielectric, antiferroelectric, and SmC(*)(alpha) phases. An analysis of the scattering features allows the structural models of the different subphases to be distinguished, in addition to providing a measurement of the helical pitch. This paper reports resonant scattering features in the antiferroelectric hexatic phase, the three- and four-layer intermediate phases, the antiferroelectric and ferroelectric phases and the SmC(*)(alpha) phase. The helicoidal pitch has been measured from the scattering peaks in the four-layer intermediate phase as well as in the antiferroelectric and ferroelectric phases. In the SmC(*)(alpha) phase, an investigation into the helical structure has revealed a pitch ranging from 5 to 54 layers in different materials. Further, a strong resonant scattering signal has been observed in mixtures of a selenium containing material with as much as 90% nonresonant material.

Enhanced interfacial magnetic coupling of Gd /Fe multilayers.

The spatial extent zeta(AFM) and strength J(AFM) of the antiferromagnetic (AFM) exchange coupling at buried Gd /Fe interfaces in ferrimagnetic [Gd(50 A)Fe(15,35 A)](15) sputtered multilayers is obtained from combined x-ray resonance magnetic reflectivity and magnetic circular dichroism measurements. zeta(AFM) is 4.1(7) A or approximately 1-2 interatomic distances in bulk Gd and Fe; J(AFM) is 1050(90) K, comparable to the ferromagnetic exchange in bulk Fe.

Resonant x-ray scattering study of the antiferroelectric and ferrielectric phases in liquid crystal devices.

Resonant x-ray scattering has been used to investigate the interlayer ordering of the antiferroelectric and ferrielectric smectic C* subphases in a device geometry. The liquid crystalline materials studied contain a selenium atom and the experiments were carried out at the selenium K edge allowing x-ray transmission through glass. The resonant scattering peaks associated with the antiferroelectric phase were observed in two devices containing different materials. It was observed that the electric-field-induced antiferroelectric to ferroelectric transition coincides with the chevron to bookshelf transition in one of the devices. Observation of the splitting of the antiferroelectric resonant peaks as a function of applied field also confirmed that no helical unwinding occurs at fields lower than the chevron to bookshelf threshold. Resonant features associated with the four-layer ferrielectric liquid crystal phase were observed in a device geometry. Monitoring the electric field dependence of these ferrielectric resonant peaks showed that the chevron to bookshelf transition occurs at a lower applied field than the ferrielectric to ferroelectric switching transition.

Regulation of human PLD1 and PLD2 by calcium and protein kinase C.

Numerous studies show that PLD is activated in cells by calcium and by protein kinase C (PKC). We found that human PLD1 and PLD2 expressed in Sf9 cells can be activated by calcium-mobilizing agonists and by co-expression with PKCalpha. The calcium-mobilizing agonists A23187 and CryIC toxin triggered large increases in phosphatidylethanol (PtdEth) production in Sf9 cells over-expressing PLD1 and PLD2, but not in vector controls. PLD activation by these agonists was largely dependent on extracellular calcium. Membrane assays demonstrated significant PLD1 and PLD2 activity in the absence of divalent cations, which could be enhanced by low levels of calcium either in the presence or absence of magnesium. PLD1 but not PLD2 activity was slightly enhanced by magnesium. Treatment of Sf9 cells expressing PLD1 and PLD2 with PMA resulted in little PtdEth production. However, a significant and comparable formation of PtdEth occurred when PLD1 or PLD2 were co-expressed with PKCalpha, but not PKCdelta, and was further augmented by PMA. In contrast to PLD1, co-expressing PLD2 with PKCalpha or PKCdelta further enhanced A23187-induced PtdEth production. Immunoprecipitation experiments demonstrated that PLD1 and PLD2 associated with the PKC isoforms in Sf9 cells. Furthermore, in membrane reconstitution assays, both PLD1 and PLD2 could be stimulated by calmodulin and PKCalpha-enriched cytosol. The results indicate that PLD2 as well as PLD1 is subject to agonist-induced activation in intact cells and can be regulated by calcium and PKC.

In situ surface monitoring system for synchrotron mirrors under high heat load.

A portable electro-optical system capable of real-time measurements of surface slope distortions down to 0.5 murad is described; the system is limited primarily by its short-term stability. The system employs an angle measurement technique that, in combination with the least-squares signal extraction method, reduces system fluctuations. In addition, a multireflection technique is used to enhance the detectable resolution. Although designed for use with mirrors for synchrotron radiation sources, this system has the flexibility to be applied to other optical components. The prototype system has been tested on a sample mirror piece, and preliminary results are presented. A brief discussion about the extension of this metrology unit to adaptive optics is also given.