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1.
Rev Sci Instrum ; 93(6): 065109, 2022 Jun 01.
Article in English | MEDLINE | ID: mdl-35778024

ABSTRACT

CHESS, chopper spectrometer examining small samples, is a planned direct geometry neutron chopper spectrometer designed to detect and analyze weak signals intrinsic to small cross sections (e.g., small mass, small magnetic moments, or neutron absorbing materials) in powders, liquids, and crystals. CHESS is optimized to enable transformative investigations of quantum materials, spin liquids, thermoelectrics, battery materials, and liquids. The broad dynamic range of the instrument is also well suited to study relaxation processes and excitations in soft and biological matter. The 15 Hz repetition rate of the Second Target Station at the Spallation Neutron Source enables the use of multiple incident energies within a single source pulse, greatly expanding the information gained in a single measurement. Furthermore, the high flux grants an enhanced capability for polarization analysis. This enables the separation of nuclear from magnetic scattering or coherent from incoherent scattering in hydrogenous materials over a large range of energy and momentum transfer. This paper presents optimizations and technical solutions to address the key requirements envisioned in the science case and the anticipated uses of this instrument.

2.
Phys Rev Lett ; 125(4): 046403, 2020 Jul 24.
Article in English | MEDLINE | ID: mdl-32794786

ABSTRACT

For materials near the phase boundary between weak and strong topological insulators (TIs), their band topology depends on the band alignment, with the inverted (normal) band corresponding to the strong (weak) TI phase. Here, taking the anisotropic transition-metal pentatelluride ZrTe_{5} as an example, we show that the band inversion manifests itself as a second extremum (band gap) in the layer stacking direction, which can be probed experimentally via magnetoinfrared spectroscopy. Specifically, we find that the band anisotropy of ZrTe_{5} features a slow dispersion in the layer stacking direction, along with an additional set of optical transitions from a band gap next to the Brillouin zone center. Our work identifies ZrTe_{5} as a strong TI at liquid helium temperature and provides a new perspective in determining band inversion in layered topological materials.

3.
J Phys Condens Matter ; 32(37): 374007, 2020 Feb 12.
Article in English | MEDLINE | ID: mdl-32050188

ABSTRACT

It is well established that in the low-temperature limit, the two-dimensional quantum Heisenberg antiferromagnet on a square lattice (2DQHAFSL) exhibits an anomaly in its spectrum at short-wavelengths on the zone-boundary. In the vicinity of the [Formula: see text] point the pole in the one-magnon response exhibits a downward dispersion, is heavily damped and attenuated, giving way to an isotropic continuum of excitations extending to high energies. The origin of the anomaly and the presence of the continuum are of current theoretical interest, with suggestions focused around the idea that the latter evidences the existence of spinons in a two-dimensional system. Here we present the results of neutron inelastic scattering experiments and Quantum Monte Carlo calculations on the metallo-organic compound Cu(DCOO)[Formula: see text]D2O (CFTD), an excellent physical realisation of the 2DQHAFSL, designed to investigate how the anomaly at [Formula: see text] evolves up to finite temperatures [Formula: see text]. Our data reveal that on warming the anomaly survives the loss of long-range, three-dimensional order, and that it is thus a robust feature of the two-dimensional system. With further increase of temperature the zone-boundary response gradually softens and broadens, washing out the [Formula: see text] anomaly. This is confirmed by a comparison of our data with the results of finite-temperature Quantum Monte Carlo simulations where the two are found to be in good accord. In the vicinity of the antiferromagnetic zone centre, there was no significant softening of the magnetic excitations over the range of temperatures investigated.

4.
Phys Rev Lett ; 122(9): 097201, 2019 Mar 08.
Article in English | MEDLINE | ID: mdl-30932548

ABSTRACT

We report a comprehensive inelastic neutron-scattering study of the frustrated pyrochlore antiferromagnet MgCr_{2}O_{4} in its cooperative paramagnetic regime. Theoretical modeling yields a microscopic Heisenberg model with exchange interactions up to third-nearest neighbors, which quantitatively explains all of the details of the dynamic magnetic response. Our work demonstrates that the magnetic excitations in paramagnetic MgCr_{2}O_{4} are faithfully represented in the entire Brillouin zone by a theory of magnons propagating in a highly correlated paramagnetic background. Our results also suggest that MgCr_{2}O_{4} is proximate to a spiral spin-liquid phase distinct from the Coulomb phase, which has implications for the magnetostructural phase transition in MgCr_{2}O_{4}.

5.
Nat Commun ; 9(1): 5394, 2018 12 19.
Article in English | MEDLINE | ID: mdl-30568161

ABSTRACT

One-dimensional (1D) magnetic insulators have attracted significant interest as a platform for studying quasiparticle fractionalization, quantum criticality, and emergent phenomena. The spin-1/2 Heisenberg chain with antiferromagnetic nearest neighbour interactions is an important reference system; its elementary magnetic excitations are spin-1/2 quasiparticles called spinons that are created in even numbers. However, while the excitation continuum associated with two-spinon states is routinely observed, the study of four-spinon and higher multi-spinon states is an open area of research. Here we show that four-spinon excitations can be accessed directly in Sr2CuO3 using resonant inelastic x-ray scattering (RIXS) in a region of phase space clearly separated from the two-spinon continuum. Our finding is made possible by the fundamental differences in the correlation function probed by RIXS in comparison to other probes. This advance holds promise as a tool in the search for novel quantum states and quantum spin liquids.

6.
Nat Commun ; 9(1): 3110, 2018 08 01.
Article in English | MEDLINE | ID: mdl-30068947

ABSTRACT

The original version of this Article omitted the following from the Acknowledgements: 'J. Ma's primary affiliation is Shanghai Jiao Tong University.' This has been corrected in both the PDF and HTML versions of the Article.

7.
Nat Commun ; 9(1): 2666, 2018 07 10.
Article in English | MEDLINE | ID: mdl-29991805

ABSTRACT

Magnetization plateaus in quantum magnets-where bosonic quasiparticles crystallize into emergent spin superlattices-are spectacular yet simple examples of collective quantum phenomena escaping classical description. While magnetization plateaus have been observed in a number of spin-1/2 antiferromagnets, the description of their magnetic excitations remains an open theoretical and experimental challenge. Here, we investigate the dynamical properties of the triangular-lattice spin-1/2 antiferromagnet Ba3CoSb2O9 in its one-third magnetization plateau phase using a combination of nonlinear spin-wave theory and neutron scattering measurements. The agreement between our theoretical treatment and the experimental data demonstrates that magnons behave semiclassically in the plateau in spite of the purely quantum origin of the underlying magnetic structure. This allows for a quantitative determination of Ba3CoSb2O9 exchange parameters. We discuss the implication of our results to the deviations from semiclassical behavior observed in zero-field spin dynamics of the same material and conclude they must have an intrinsic origin.

8.
J Chem Phys ; 143(12): 124201, 2015 Sep 28.
Article in English | MEDLINE | ID: mdl-26429001

ABSTRACT

For over a century, vibrational spectroscopy has enhanced the study of materials. Yet, assignment of particular molecular motions to vibrational excitations has relied on indirect methods. Here, we demonstrate that applying group theoretical methods to the dynamic pair distribution function analysis of neutron scattering data provides direct access to the individual atomic displacements responsible for these excitations. Applied to the molecule-based frustrated magnet with a potential magnetic valence-bond state, LiZn2Mo3O8, this approach allows direct assignment of the constrained rotational mode of Mo3O13 clusters and internal modes of MoO6 polyhedra. We anticipate that coupling this well known data analysis technique with dynamic pair distribution function analysis will have broad application in connecting structural dynamics to physical properties in a wide range of molecular and solid state systems.

9.
Phys Rev Lett ; 115(4): 047401, 2015 Jul 24.
Article in English | MEDLINE | ID: mdl-26252707

ABSTRACT

Iron pnictides and selenides display a variety of unusual magnetic phases originating from the interplay between electronic, orbital, and lattice degrees of freedom. Using powder inelastic neutron scattering on the two-leg ladder BaFe_{2}Se_{3}, we fully characterize the static and dynamic spin correlations associated with the Fe_{4} block state, an exotic magnetic ground state observed in this low-dimensional magnet and in Rb_{0.89}Fe_{1.58}Se_{2}. All the magnetic excitations of the Fe_{4} block state predicted by an effective Heisenberg model with localized spins are observed below 300 meV and quantitatively reproduced. However, the data only account for 16(3)µ_{B}^{2} per Fe^{2+}, approximatively 2/3 of the total spectral weight expected for localized S=2 moments. Our results highlight how orbital degrees of freedom in iron-based magnets can conspire to stabilize an exotic magnetic state.

10.
Nat Phys ; 11(1): 62-68, 2015 Jan 01.
Article in English | MEDLINE | ID: mdl-25729400

ABSTRACT

Quantum magnets have occupied the fertile ground between many-body theory and low-temperature experiments on real materials since the early days of quantum mechanics. However, our understanding of even deceptively simple systems of interacting spins-1/2 is far from complete. The quantum square-lattice Heisenberg antiferromagnet (QSLHAF), for example, exhibits a striking anomaly of hitherto unknown origin in its magnetic excitation spectrum. This quantum effect manifests itself for excitations propagating with the specific wave vector (π, 0). We use polarized neutron spectroscopy to fully characterize the magnetic fluctuations in the metal-organic compound CFTD, a known realization of the QSLHAF model. Our experiments reveal an isotropic excitation continuum at the anomaly, which we analyse theoretically using Gutzwiller-projected trial wavefunctions. The excitation continuum is accounted for by the existence of spatially-extended pairs of fractional S=1/2 quasiparticles, 2D analogues of 1D spinons. Away from the anomalous wave vector, these fractional excitations are bound and form conventional magnons. Our results establish the existence of fractional quasiparticles in the high-energy spectrum of a quasi-two-dimensional antiferromagnet, even in the absence of frustration.

11.
Phys Rev Lett ; 112(2): 027202, 2014 Jan 17.
Article in English | MEDLINE | ID: mdl-24484043

ABSTRACT

Inelastic neutron scattering at low temperatures T≤30 K from a powder of LiZn2Mo3O8 demonstrates this triangular-lattice antiferromagnet hosts collective magnetic excitations from spin-1/2 Mo3O13 molecules. Apparently gapless (Δ<0.2 meV) and extending at least up to 2.5 meV, the low-energy magnetic scattering cross section is surprisingly broad in momentum space and involves one-third of the spins present above 100 K. The data are compatible with the presence of valence bonds involving nearest-neighbor and next-nearest-neighbor spins forming a disordered or dynamic state.

12.
Phys Rev Lett ; 109(2): 027203, 2012 Jul 13.
Article in English | MEDLINE | ID: mdl-23030203

ABSTRACT

Polarized and unpolarized neutron scattering experiments on the frustrated ferromagnetic spin-1/2 chain LiCuVO4 show that the phase transition at H(Q) of 8 T is driven by quadrupolar fluctuations and that dipolar correlations are short range with moments parallel to the applied magnetic field in the high-field phase. Heat-capacity measurements evidence a phase transition into this high-field phase, with an anomaly clearly different from that at low magnetic fields. Our experimental data are consistent with a picture where the ground state above H(Q) has a next-nearest neighbor bond-nematic order along the chains with a fluidlike coherence between weakly coupled chains.

13.
Phys Rev Lett ; 108(18): 187206, 2012 May 04.
Article in English | MEDLINE | ID: mdl-22681114

ABSTRACT

A quantum magnet, LiCuSbO4, with chains of edge-sharing spin-1/2 CuO6 octahedra is reported. While short-range order is observed for T<10 K, no zero-field phase transition or spin freezing occurs down to 100 mK. Specific heat indicates a distinct high-field phase near the 12 T saturation field. Neutron scattering shows incommensurate spin correlations with q=(0.47±0.01)π/a and places an upper limit of 70 µeV on any spin gap. Exact diagonalization of 16-spin easy-plane spin-1/2 chains with competing ferro- and antiferromagnetic interactions (J1=-75 K, J2=34 K) accounts for the T>2 K data.

14.
Nature ; 485(7396): 82-5, 2012 May 03.
Article in English | MEDLINE | ID: mdl-22522933

ABSTRACT

When viewed as an elementary particle, the electron has spin and charge. When binding to the atomic nucleus, it also acquires an angular momentum quantum number corresponding to the quantized atomic orbital it occupies. Even if electrons in solids form bands and delocalize from the nuclei, in Mott insulators they retain their three fundamental quantum numbers: spin, charge and orbital. The hallmark of one-dimensional physics is a breaking up of the elementary electron into its separate degrees of freedom. The separation of the electron into independent quasi-particles that carry either spin (spinons) or charge (holons) was first observed fifteen years ago. Here we report observation of the separation of the orbital degree of freedom (orbiton) using resonant inelastic X-ray scattering on the one-dimensional Mott insulator Sr2CuO3. We resolve an orbiton separating itself from spinons and propagating through the lattice as a distinct quasi-particle with a substantial dispersion in energy over momentum, of about 0.2 electronvolts, over nearly one Brillouin zone.

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