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At least 865 records · Page 48
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Temporal and spatial valley dynamics in two-dimensional semiconductors probed via Kerr rotation

Monolayer transition metal dichalcogenides (TMDCs) offer a tantalizing platform for control of both spin and valley degrees of freedom, which may enable future optoelectronic devices with enhanced and novel functionalities. In this work, we investigate the valley dynamics of two prototypical members of TMDCs, namely Mo S 2 and WS e 2 , using time-resolved Kerr rotation (TRKR) at temperatures from 10 K to 300 K. This pump-probe technique enables sub-picosecond temporal resolution, providing insight into ultrafast valley dynamics, which is inaccessible by polarized and time-resolved photoluminescence spectroscopy. Bi-exponential decay dynamics were observed for both materials at low temperatures, and the fast decay component indicated a rapid exciton valley depolarization time (< 10 ps) due to strong Coulomb exchange interactions between the K valleys. However, the slow decay components (several tens of picoseconds) were attributed to different origins in the two materials, which were further elucidated by temperature-dependent TRKR measurements. Moreover, the spatial dependence of the TRKR intensity across Mo S 2 monolayer flakes indicated a weaker valley polarization near the edges, which is likely associated with quenched excitons near the grain boundaries or a disordered edge region in chemical vapor deposition–grown monolayers. These temporal and spatial TRKR measurements reveal insight into the complex dynamics of valley excitonic states, which will be critical for valleytronic applications of monolayer TMDCs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Combining microscopic and macroscopic probes to untangle the single-ion anisotropy and exchange energies in an S = 1 quantum antiferromagnet [Combining micro- and macroscopic probes to untangle single-ion and spatial exchange anisotropies in a S = 1 quantum antiferromagnet]

The magnetic ground state of the quasi-one-dimensional spin-1 antiferromagnetic chain is sensitive to the relative sizes of the single-ion anisotropy (D) and the intrachain (J) and interchain (J') exchange interactions. The ratios D/J and J' /J dictate the material's placement in one of three competing phases: a Haldane gapped phase, a quantum paramagnet, and an XY-ordered state, with a quantum critical point at their junction. We have identified [Ni(HF 2 )(pyz) 2 ] SbF 6 , where pyz = pyrazine, as a rare candidate in which this behavior can be explored in detail. Combining neutron scattering (elastic and inelastic) in applied magnetic fields of up to 10 tesla and magnetization measurements in fields of up to 60 tesla with numerical modeling of experimental observables, we are able to obtain accurate values of all of the parameters of the Hamiltonian [D = 13.3(1) K, J = 10.4(3) K, and J' = 1.4(2) K], despite the polycrystalline nature of the sample. Density-functional theory calculations result in similar couplings (J = 9.2 K, J' = 1.8 K) and predict that the majority of the total spin population resides on the Ni(II) ion, while the remaining spin density is delocalized over both ligand types. Finally, the general procedures outlined in this paper permit phase boundaries and quantum-critical points to be explored in anisotropic systems for which single crystals are as yet unavailable.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Lattice spin models for non-Abelian chiral spin liquids

Here, we suggest a class of two-dimensional lattice spin Hamiltonians describing non-Abelian SU(2) chiral spin liquids—spin analogs of fractional non-Abelian quantum Hall states—with gapped bulk and gapless chiral edge excitations described by the SU(2) n Wess-Zumino-Novikov-Witten conformal field theory. The models are constructed from an array of generalized spin-n/2 ladders with multi-spin-exchange interactions which are coupled by isolated spins. Such models allow a controllable analytic treatment starting from the one-dimensional limit and are characterized by a bulk gap and non-Abelian SU(2) n gapless edge excitations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Spin order and dynamics in the diamond-lattice Heisenberg antiferromagnets CuRh 2 O 4 and CoRh 2 O 4

Here, antiferromagnetic insulators on a diamond lattice are candidate materials to host exotic magnetic phenomena ranging from spin-orbital entanglement to degenerate spiral ground states and topological paramagnetism. Compared to other three-dimensional networks of magnetic ions, such as the geometrically frustrated pyrochlore lattice, the investigation of diamond-lattice magnetism in real materials is less mature. In this work, we characterize the magnetic properties of model A-site spinels CoRh 2 O 4 (cobalt rhodite) and CuRh 2 O 4 (copper rhodite) by means of thermomagnetic and neutron-scattering measurements, and we perform group theory analysis, Rietveld refinement, mean-field theory, and spin-wave theory calculations to analyze the experimental results. Our investigation reveals that cubic CoRh 2 O 4 is a canonical S = 3/2 diamond-lattice Heisenberg antiferromagnet with a nearest-neighbor exchange J = 0.63 meV and a Néel ordered ground state below a temperature of 25 K. In tetragonally distorted CuRh 2 O 4 , competing exchange interactions between up to third-nearest-neighbor spins lead to the development of an incommensurate spin helix at 24 K with a magnetic propagation vector k m = (0,0,0.79). Strong reduction of the ordered moment is observed for the S = 1/2 spins in CuRh 2 O 4 and captured by our 1/ S corrections to the staggered magnetization. Our work identifies CoRh 2 O 4 and CuRh 2 O 4 as reference materials to guide future work searching for exotic quantum behavior in diamond-lattice antiferromagnets.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Ordering mechanism and quantum anomalous Hall effect of magnetically doped topological insulators

We investigate magnetic ordering and the quantum anomalous Hall effect (QAHE) in Cr-doped topological insulators using systematic first-principles calculations, explaining the mechanism responsible for ferromagnetic order and the reason why Sb 2 Te 3 is a better QAHE host than Bi 2 Se 3 or Bi 2 Te 3 . In this work, we conclude that these magnetic topological insulators have relatively long-range exchange interactions within quintuple layers and weak interactions between quintuple layers. Our analyses for the spin splitting of the topological surface states suggest that the temperature at which the QAHE occurs in these materials can be enhanced significantly by Mo-Cr co-doping.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Neutron diffraction and μ SR studies of two polymorphs of nickel niobate NiNb 2 O 6

Neutron diffraction and muon spin relaxation (μSR) studies are presented in this paper for the newly characterized polymorph of NiNb 2 O 6 (β-NiNb 2 O 6 ) with space group P4 2 /n and μSR data only for the previously known columbite structure polymorph with space group Pbcn. The magnetic structure of the P4 2 /n form was determined from neutron diffraction using both powder and single-crystal data. Powder neutron diffraction determined an ordering wave vector → k=( 1 / 2 , 1 / 2 , 1 / 2 ). Single-crystal data confirmed the same → k vector and showed that the correct magnetic structure consists of antiferromagnetically coupled chains running along the a or b axis in adjacent Ni 2+ layers perpendicular to the c axis, which is consistent with the expected exchange interaction hierarchy in this system. The refined magnetic structure is compared with the known magnetic structures of the closely related trirutile phases, NiSb 2 O 6 and NiTa 2 O 6 . μSR data finds a transition temperature of T N ~15K for this system, while the columbite polymorph exhibits a lower T N =5.7(3) K. Our μSR measurements also allowed us to estimate the critical exponent of the order parameter β for each polymorph. We found β =0.25(3) and 0.16(2) for the β and columbite polymorphs, respectively. The single-crystal neutron scattering data give a value for the critical exponent β =0.28(3) for β-NiNb 2 O 6 , in agreement with the μSR value. While both systems have β values less than 0.3, which is indicative of reduced dimensionality, this effect appears to be much stronger for the columbite system. Finally, in other words, although both systems appear to be well described by S=1 spin chains, the interchain interactions in the β polymorph are likely much larger.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Tuning interfacial ferromagnetism in LaNiO 3 / CaMnO 3 superlattices by stabilizing nonequilibrium crystal symmetry

Perovskite oxide heterostructures offer an important path forward for stabilizing and controlling low-dimensional magnetism. One of the guiding design principles for these materials systems is octahedral connectivity. In superlattices composed of perovskites with different crystal symmetries, variation of the relative ratio of the constituent layers and the individual layer thicknesses gives rise to nonequilibrium crystal symmetries that, in turn, lead to unprecedented control of interfacial ferromagnetism. We have found that in superlattices of CaMnO 3 (CMO) and LaNiO 3 (LNO), interfacial ferromagnetism can be modulated by a factor of 3 depending on LNO and CMO layer thicknesses as well as their relative ratio. Such an effect is only possible due to the nonequilibrium crystal symmetries at the interfaces and can be understood in terms of the anisotropy of the exchange interactions and modifications in the interfacial Ni-O-Mn and Mn-O-Mn bond angles and lengths with increasing LNO layer thickness. Here, these results demonstrate the potential of engineering nonequilibrium crystal symmetries in designing ferromagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Influence of magnetism and correlation on the spectral properties of doped Mott insulators

Unraveling the nature of the doping-induced transition between a Mott insulator and a weakly correlated metal is crucial to understanding novel emergent phases in strongly correlated materials. Here, for this purpose, we study the evolution of spectral properties upon doping Mott insulating states by utilizing the cluster perturbation theory on the Hubbard and t – J -like models. Specifically, a quasifree dispersion crossing the Fermi level develops with small doping, and it eventually evolves into the most dominant feature at high doping levels. Although this dispersion is related to the free-electron hopping, our study shows that this spectral feature is, in fact, influenced inherently by both electron-electron correlation and spin-exchange interaction: the correlation destroys coherence, while the coupling between spin and mobile charge restores it in the photoemission spectrum. Due to the persistent impact of correlations and spin physics, the onset of gaps or the high-energy anomaly in the spectral functions can be expected in doped Mott insulators.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Enhanced moments of Eu in single crystals of the metallic helical antiferromagnet EuCo 2 - y As 2

EuCo 2 - y As 2 with the tetragonal ThCr 2 Si 2 structure is known to contain Eu +2 ions with spin S=$\frac{7}{2}$that order below a temperature T N ≈ 47 K into an antiferromagnetic (AFM) proper helical structure with the ordered moments aligned in the tetragonal ab plane, perpendicular to the helix axis along the c axis, with no contribution from the Co atoms. Here we carry out a detailed investigation of the properties of single crystals. We consistently find about 5% vacancies on the Co site from energy-dispersive x-ray analysis and x-ray diffraction refinements. Enhanced ordered and effective moments of the Eu spins are found in most of our crystals. Electronic structure calculations indicate that the enhanced moments arise from polarization of the d bands, as occurs in ferromagnetic Gd metal. Electrical resistivity measurements indicate metallic behavior. The low-field in-plane magnetic susceptibilities $\chi_{ab}$ (T < T N ) for several crystals are reported that are fitted well by unified molecular field theory (MFT), and the Eu–Eu exchange interactions J ij are extracted from the fits. High-field magnetization M data for magnetic fields H ∥ ab reveal what appears to be a first-order spin-flop transition followed at higher field by a second-order metamagnetic transition of unknown origin, and then by another second-order transition to the paramagnetic (PM) state. For H ∥ c , the magnetization shows only a second-order transition from the canted AFM to the PM state, as expected. The critical fields for the AFM to PM transition are in approximate agreement with the predictions of MFT. Heat capacity C p measurements in zero and high H are reported. Phase diagrams for H ∥ c and H ∥ ab versus T are constructed from the high-field M (H ,T) and C p (H,T) measurements. Lastly, the magnetic part C mag (T,H = 0) of C p (T,H= 0) is extracted and is fitted rather well below T N by MFT, although dynamic short-range AFM order is apparent in C mag (T) up to about 70 K, where the molar entropy attains its high- T limit of R ln 8.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Local quantum criticality of a one-dimensional Kondo insulator model

Here, the continuous quantum phase transition and the nature of the quantum critical point (QCP) in a modified Kondo lattice model with Ising anisotropic exchange interactions are studied within the density-matrix renormalization group algorithm. We investigate the effect of quantum fluctuations on critical Kondo destruction QCP by probing static and dynamic properties of the magnetic order and the Kondo effect. In particular, we identify that local Kondo physics itself becomes critical at the magnetic phase transition point, providing unbiased evidences for local quantum criticality between two insulators without involving the Fermi surface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Spin freezing into a disordered state in CaFeT i 2 O 6 synthesized under high pressure

Double perovskites exhibit a variety of interesting phenomena due to numerous combinations of cation orderings and distortions. CaMnTi 2 O 6 and CaFeTi 2 O 6 are the only two discovered double perovskites that have the columnar type A-site ordering associated with the a + a + c – titling system. The former perovskite, synthesized recently, has a polar structure below T c and shows an unusual ferroelectricity. The latter, while synthesized decades ago, received less investigation. Here, we have synthesized CaFeTi 2 O 6 under high pressure and carried out thorough characterizations through measurements of x-ray powder diffraction (XRD), second harmonic generation (SHG), dc and ac magnetization, Mössbauer spectra, resistivity, thermoelectric power, and specific heat. Although the structural refinement of the XRD pattern cannot distinguish two possible tetragonal phases, SHG measurements help to rule out the possibility of a polar structure observed in CaMnTi 2 O 6 . Fitting the paramagnetic susceptibility to a Curie-Weiss law gives a negligible Weiss constant. The weak exchange interaction gives way to a dipole-dipole interaction and single-ion anisotropy. An anomaly at 1.2 K in the specific heat is too broad for a magnetic transition, but suggestive of a spin-ice-like state as in the pyrochlores. Mössbauer spectroscopy shows two distinct iron sites, as expected for the crystal structure. Both sites are occupied by high-spin Fe 2+ as indicated by the isomer shift. The sharply different temperature dependence of the quadrupole splitting at the two iron sites can be well explained based on the local structural distortions from the refinement of XRD patterns. In conclusion, the line broadening associated with long spin-relaxation times is observed at 6 K as the spin freezing transition is approached from high temperatures.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Unified phase diagram of antiferromagnetic SU( N ) spin ladders

Motivated by near-term experiments with ultracold alkaline-earth atoms confined to optical lattices, we establish numerically and analytically the phase diagram of two-leg SU ( N ) spin ladders. Two-leg ladders provide a rich and highly nontrivial extension of the single chain case on the way towards the relatively little explored two-dimensional situation. Focusing on the experimentally relevant limit of one fermion per site, antiferromagnetic exchange interactions, and 2 ≤ N ≤ 6, we show that the phase diagrams as a function of the interchain (rung) to intrachain (leg) coupling ratio, J ⊥ /J ∥ , strongly differ for even versus odd N. For even N = 4 and 6, we demonstrate that the phase diagram consists of a single valence bond crystal (VBC) with a spatial period of N/2 rungs. For odd N = 3 and 5, we find surprisingly rich phase diagrams exhibiting three distinct phases. For weak rung coupling, we obtain a VBC with a spatial period of N rungs, whereas for strong coupling we obtain a critical phase related to the case of a single chain. In addition, we encounter intermediate phases for odd N, albeit of a different nature for N = 3 as compared to N = 5. For N = 3, we find a novel gapless intermediate phase with J ⊥ -dependent incommensurate spatial fluctuations in a sizeable region of the phase diagram. For N = 5 , there are strong indications for a narrow potentially gapped intermediate phase, whose nature is not entirely clear. Lastly, our results are based on (i) field theoretical techniques, (ii) qualitative symmetry considerations, and (iii) large-scale density matrix renormalization group (DMRG) simulations keeping beyond a million of states by fully exploiting and thus preserving the SU (N) symmetry.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Spin gaps in the ordered states of La 2 Li X O 6 ( X = Ru , Os ) and their relation to the distortion of the cubic double perovskite structure in 4 d 3 and 5 d 3 magnets

Time-of-flight inelastic neutron scattering measurements have been carried out on polycrystalline samples of the 4d 3 and 5d 3 double pervoskite antiferromagnets La 2 LiRuO 6 and La 2 LiOsO 6 . These reveal the development of an inelastic spin gap in La 2 LiRuO 6 and La 2 LiOsO 6 of ~1.8(8) and 6(1) meV, below their respective ordering temperatures TN, ~23.8 and 30 K. The bandwidths of the spin excitations are shown to be ~5.7(9)and12(1)meV, respectively, at low temperatures. Spin gaps are surprising in such magnets as the t 2g levels of Ru 5+ or Os 5+ are expected to be half-filled, resulting in an anticipated orbital singlet for both materials. We compare these results in monoclinic double perovskites La 2 LiRuO 6 and La 2 LiOsO 6 with those in cubic Ba 2 YRuO 6 and Ba 2 YOsO 6 as well as with those in other monoclinic La 2 NaRuO 6 ,La 2 NaOsO 6 , and Sr 2 ScOsO 6 and model the inelastic magnetic scattering with linear spin-wave theory using minimal anisotropic exchange interactions. We discuss the possible role of the distortion of the face-centered-cubic double perovskite structure on the spin gap formation and geometric frustration in these materials and show that T N scales with the top of the spin-wave band in all members of these families that display long-range order.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Collapse of the Kondo state and ferromagnetic quantum phase transition in YbFe 2 Zn 20

Here, we present the electrical resistivity data under application of pressures up to ~26 GPa and down to 50 mK on YbFe 2 Zn 20 . We find a pressure induced magnetic phase transition with an onset at p c = 18.2±0.8 GPa. At ambient pressure, YbFe 2 Zn 20 manifests a heavy fermion, nonmagnetic ground state and the Fermi liquid behavior at low temperatures. As pressure is increased, the power law exponent in resistivity, n, deviates significantly from Fermi liquid behavior and tends to saturate with n = 1 near p c . A pronounced resistivity maximum T max , which scales with the Kondo temperature, is observed. T max decreases with increasing pressure and flattened out near pc indicating the suppression of Kondo exchange interaction. For p > p c , T max shows a sudden upward shift, most likely becoming associated with crystal electric field scattering. Application of magnetic field for p > p c broadens the transition and shifts it toward the higher temperature, which is a typical behavior of a transition towards a ferromagnetic state, or a state with a significant ferromagnetic component. The magnetic transition appears to abruptly develop above pc, suggesting probable first-order (with changing pressure) nature of the transition; once stabilized, the ordering temperature does not depend on pressure up to ~26 GPa. Taken as a whole, these data suggest that YbFe 2 Zn 20 has a quantum phase transition at p c = 18.2 GPa associated with the avoided quantum criticality in metallic ferromagnets.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Bandwidth controlled insulator-metal transition in BaFe 2 S 3 : A Mössbauer study under pressure

BaFe 2 S 3 is a quasi one-dimensional Mott insulator that orders antiferromagnetically below 125 K. The application of pressure induces a transition to a metallic state, and superconductivity emerges.The evolution of the magnetic behavior on increasing pressure has up to now been either studied indirectly by means of transport measurements, or by using local magnetic probes only in the low pressure region. Here, we investigate the magnetic properties of BaFe 2 S 3 up to 9.9GPa by means of synchrotron 57 Fe Mossbauer spectroscopy experiments, providing the First local magnetic phase diagram. The magnetic ordering temperature increases up to 185(5) K at 7.5GPa, and is fully suppressed at 9.9GPa. The low-temperature magnetic hyperne field is continuously reduced from 12.9 to 10.3T between 1.4 and 9.1GPa, followed by a sudden drop to zero at 9.9GPa indicating a First-order phase transition. The pressure dependence of the magnetic order in BaFe2S3 can be qualitatively explained by a combination of a bandwidth-controlled insulator-metal transition as well as a pressure enhanced exchange interaction between Fe-atoms and Fe 3d-S 3p hybridization.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Relaxing Kondo-screened Kramers doublets in CeRhSi 3

${\mathrm{CeRhSi}}_{3}$ is a superconductor under pressure coexisting with a weakly antiferromagnetic phase characterized by a Bragg peak at q → 0 = (~ 0.2,0,0.5) [N. Aso et al., J. Magn. Magn. Mater. 310, 602 (2007)]. The compound is also a heavy-fermion material with a large specific heat coefficient ${\gamma}=110$ mJ ${\mathrm{mol}}^{{-}1}{\mathrm{K}}^{{-}2}$ and a high Kondo temperature of ${T}_{K}=50$ K, indicating ${\mathrm{CeRhSi}}_{3}$ is in a strongly Kondo screened state. We apply high-resolution neutron spectroscopy to investigate the magnetic fluctuations in the normal phase, at ambient pressures, and at low temperatures. We measure a commensurate dynamic response centered around the Q → = (0,0,2) position that gradually evolves to $H{\sim}0.2$ with decreasing temperature and/or energy transfers. The response is broadened both in momentum and energy and is not reminiscent of sharp spin wave excitations found in insulating magnets where the electrons are localized. We parametrize the excitation spectrum and temperature dependence using a heuristic model utilizing the random-phase approximation to couple relaxing ${\mathrm{Ce}}^{3+}$ ground-state Kramers doublets with a Kondo-like dynamic response. With a Ruderman-Kittel-Kasuya-Yosida exchange interaction within the $ab$ plane and an increasing single-site susceptibility, we can qualitatively reproduce the neutron spectroscopic results in ${\mathrm{CeRhSi}}_{3}$ and, namely, the trade-off between scattering at commensurate and incommensurate positions. We suggest that the antiferromagnetic phase in ${\mathrm{CeRhSi}}_{3}$ is driven by weakly correlated relaxing localized Kramers doublets and that ${\mathrm{CeRhSi}}_{3}$ at ambient pressures is on the border between a Rudderman-Kittel-Yosida antiferromagnetic state and a Kondo-screened phase where static magnetism is predominately absent.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Comprehensive magnetic phase diagrams of the polar metal Ca 3 (Ru 0.95 Fe 0.05 ) 2 O 7

Polar metals exist as a rather unique class of materials as they combine two seemingly mutually exclusive properties (polar order and metallicity) in one system. So far only a few polar metals have been unambiguously identified; the magnetic ones are exceptionally rare. Here we investigate a 5% Fe-doped polar metal Ca 3 Ru 2 O 7 , via electrical transport, magnetization, microstrain, and optical second-harmonic generation measurements. We report the full magnetic phase diagrams (in the field-temperature space) for magnetic field H∥a and H∥b, which exhibit distinct field-dependent magnetizations behavior. In particular, for H∥a we found a ferromagnetic incommensurate spin structure, which is absent in the pure Ca 3 Ru 2 O 7 . Furthermore, we propose a microscopic spin model to understand this behavior, highlighting the role of Fe doping in tipping the delicate balance of the underlying exchange-interaction energy in this system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Light mesons within the basis light-front quantization framework

In this work, we study the light-unflavored mesons as relativistic bound states in the nonperturbative Hamiltonian formalism of the basis light-front quantization approach. The dynamics for the valence quarks of these mesons is specified by an effective Hamiltonian containing the one-gluon exchange interaction and the confining potentials both introduced in our previous work on heavy quarkonia, supplemented additionally by a pseudoscalar contact interaction. We diagonalize this Hamiltonian in our basis function representation to obtain the mass spectrum and the light-front wave functions (LFWFs). Based on these LFWFs, we then study the structure of these mesons by computing the electromagnetic form factors, the decay constants, the parton distribution amplitudes, and the parton distribution functions. Our results are comparable to those from experiments and other theoretical models.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗