Shaoyan Chu

Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet.

The experimental realization of quantum spin liquids is a long-sought goal in physics, as they represent new states of matter. Quantum spin liquids cannot be described by the broken symmetries associated with conventional ground states. In fact, the interacting magnetic moments in these systems do not order, but are highly entangled with one another over long ranges. Spin liquids have a prominent role in theories describing high-transition-temperature superconductors, and the topological properties of these states may have applications in quantum information. A key feature of spin liquids is that they support exotic spin excitations carrying fractional quantum numbers. However, detailed measurements of these ‘fractionalized excitations’ have been lacking. Here we report neutron scattering measurements on single-crystal samples of the spin-1/2 kagome-lattice antiferromagnet ZnCu3(OD)6Cl2 (also called herbertsmithite), which provide striking evidence for this characteristic feature of spin liquids. At low temperatures, we find that the spin excitations form a continuum, in contrast to the conventional spin waves expected in ordered antiferromagnets. The observation of such a continuum is noteworthy because, so far, this signature of fractional spin excitations has been observed only in one-dimensional systems. The results also serve as a hallmark of the quantum spin-liquid state in herbertsmithite.

Electronic Structure of the Topological Insulator Bi2Se3 Using Angle-Resolved Photoemission Spectroscopy: Evidence for a Nearly Full Surface Spin Polarization

We performed high-resolution spin- and angle-resolved photoemission spectroscopy studies of the electronic structure and the spin texture on the surface of Bi2Se3, a model TI. By tuning the photon energy, we found that the topological surface state is well separated from the bulk states in the vicinity of kz = Z plane of the bulk Brillouin zone. The spin-resolved measurements in that region indicate a very high degree of spin polarization of the surface state, ~0.75, much higher than previously reported. Our results demonstrate that the topological surface state on Bi2Se3 is highly spin polarized and that the dominant factors limiting the polarization are mainly extrinsic.

Photoemission spectroscopy of magnetic and nonmagnetic impurities on the surface of the Bi2Se3 topological insulator.

Dirac-like surface states on surfaces of topological insulators have a chiral spin structure that suppresses backscattering and protects the coherence of these states in the presence of nonmagnetic scatterers. In contrast, magnetic scatterers should open the backscattering channel via the spin-flip processes and degrade the states coherence. We present angle-resolved photoemission spectroscopy studies of the electronic structure and the scattering rates upon the adsorption of various magnetic and nonmagnetic impurities on the surface of Bi2Se3, a model topological insulator. We reveal a remarkable insensitivity of the topological surface state to both nonmagnetic and magnetic impurities in the low impurity concentration regime. Scattering channels open up with the emergence of hexagonal warping in the high-doping regime, irrespective of the impuritys magnetic moment.

Measurement of an exceptionally weak electron-phonon coupling on the surface of the topological insulator Bi2Se3 using angle-resolved photoemission spectroscopy.

Gapless surface states on topological insulators are protected from elastic scattering on nonmagnetic impurities which makes them promising candidates for low-power electronic applications. However, for widespread applications, these states should have to remain coherent at ambient temperatures. Here, we studied temperature dependence of the electronic structure and the scattering rates on the surface of a model topological insulator, Bi2Se3, by high-resolution angle-resolved photoemission spectroscopy. We found an extremely weak broadening of the topological surface state with temperature and no anomalies in the states dispersion, indicating exceptionally weak electron-phonon coupling. Our results demonstrate that the topological surface state is protected not only from elastic scattering on impurities, but also from scattering on low-energy phonons, suggesting that topological insulators could serve as a basis for room-temperature electronic devices.

Searching for stable Na-ordered phases in single-crystal samples of γ-NaxCOO2

We report on the preparation and characterization of single-crystal {gamma} phase Na{sub x}CoO{sub 2} with 0.25{<=}x{<=}0.84 using a nonaqueous electrochemical chronoamperemetry technique. By carefully mapping the overpotential versus x (for x<0.84), we find six distinct stable phases with Na levels corresponding to x{approx} 0.75, 0.71, 0.50, 0.43, 0.33, and 0.25. The composition with x{approx_equal}0.55 appears to have a critical Na concentration which separates samples with different magnetic behavior as well as different Na ion diffusion mechanisms. Chemical analysis of an aged crystal reveals different Na ion diffusion mechanisms above and below x{sub c}{approx}0.53, where the diffusion process above x{sub c} has a diffusion coefficient about five times larger than that below x{sub c}. The series of crystals were studied with x-ray diffraction, susceptibility, and transport measurements. The crystal with x=0.5 shows a weak ferromagnetic transition below T=27 K in addition to the usual transitions at T=51 and 88 K. The resistivity of the Curie-Weiss metallic Na{sub 0.71}CoO{sub 2} composition has a very low residual resistivity, which attests to the high homogeneity of the crystals prepared by this improved electrochemical method. Our results on the various stable crystal compositions point to the importance of Na ion ordering across the phase diagram.

A Cu2+(S = 1/2) Kagomé Antiferromagnet: MgxCu4−x(OH)6Cl2

Spin-frustrated systems are one avenue for inducing macroscopic quantum states in materials. However, experimental realization of this goal has been difficult because of the lack of simple materials and, if available, the separation of the unusual magnetic properties arising from exotic magnetic states from behavior associated with chemical disorder, such as site mixing. Here we report the synthesis and magnetic properties of a new series of magnetically frustrated materials, Mg(x)Cu(4-x)(OH)(6)Cl(2). Because of the substantially different ligand-field chemistry of Mg(2+) and Cu(2+), site disorder within the kagomé layers is minimized, as directly measured by X-ray diffraction. Our results reveal that many of the properties of these materials and related systems are not due to disorder of the magnetic lattice but rather reflect an unusual ground state.

Refining the Spin Hamiltonian in the Spin-1/2 Kagome Lattice Antiferromagnet ZnCu3(OH)6Cl2 Using Single Crystals

We report thermodynamic measurements of the S=1/2 kagome lattice antiferromagnet ZnCu3(OH)6Cl2, a promising candidate system with a spin-liquid ground state. Using single crystal samples, the magnetic susceptibility both perpendicular and parallel to the kagome plane has been measured. A small, temperature-dependent anisotropy has been observed, where χ(z)/χ(p)>1 at high temperatures and χ(z)/χ(p)<1 at low temperatures. Fits of the high-temperature data to a Curie-Weiss model also reveal an anisotropy. By comparing with theoretical calculations, the presence of a small easy-axis exchange anisotropy can be deduced as the primary perturbation to the dominant Heisenberg nearest neighbor interaction. These results have great bearing on the interpretation of theoretical calculations based on the kagome Heisenberg antiferromagnet model to the experiments on ZnCu3(OH)6Cl2.

Interplay of thermal and quantum spin fluctuations in the kagome lattice compound herbertsmithite

We present a Raman spectroscopic investigation of the Herbertsmithite ZnCu3(OH)6Cl2, the first realization of a Heisenberg s=1/2 antiferromagnet on a perfect kagome lattice. The magnetic excitation spectrum of this compound is dominated by two components, a high temperature quasi elastic signal and a low temperature, broad maximum. The latter has a linear low energy slope and extends to high energy. We have investigated the temperature dependence and symmetry properties of both signals. Our data agree with previous calculations and point to a spin liquid ground state.

Hydrothermal growth of single crystals of the quantum magnets: Clinoatacamite, paratacamite, and herbertsmithite

We present a hydrothermal method for growing millimeter-sized crystals of the quantum magnets with formula Cu4−xZnx(OH)6Cl2: clinoatacamite (x=0), paratacamite (0.33<x<1) and herbertsmithite (x=1). These highly pure single crystals have been characterized by x-ray diffraction, chemical analysis, Raman spectroscopy, and magnetic susceptibility measurements. This synthesis success opens the door for detailed investigations of the magnetic ground-state properties of these compounds.

Spin correlations in the geometrically frustrated pyrochlore Tb 2 Mo 2 O 7

We report neutron scattering studies of the spin correlations of the geometrically frustrated pyrochlore Tb2Mo2O7 using single crystal samples. This material undergoes a spin-freezing transition below Tg~24 K, similar to Y2Mo2O7, and has little apparent chemical disorder. Diffuse elastic peaks are observed at low temperatures, indicating short-range ordering of the Tb moments in an arrangement where the Tb moments are slightly rotated from the preferred directions of the spin ice structure. In addition, a Q-independent signal is observed which likely originates from frozen, but completely uncorrelated, Tb moments. Inelastic measurements show the absence of sharp peaks due to crystal field excitations. These data show how the physics of the Tb sublattice responds to the glassy behavior of the Mo sublattice with the associated effects of lattice disorder.