Browsing by Author "Adroja, DT"

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    Competing exchange interactions on the verge of a metal-insulator transition in the two-dimensional spiral magnet Sr3Fe2O7
    (Americal Physical Society, 2014-10-03) Kim, JH; Jain, A; Reehuis, M; Khaliullin, G; Peets, DC; Ulrich, C; Park, JT; Faulhaber, E; Hoser, A; Walker, HC; Adroja, DT; Walters, AC; Inosov, DS; Maljuk, A; Keimer, B
    We report a neutron scattering study of the magnetic order and dynamics of the bilayer perovskite Sr 3 Fe 2 O 7 , which exhibits a temperature-driven metal-insulator transition at 340 K. We show that the Fe 4+ moments adopt incommensurate spiral order below T N =115  K and provide a comprehensive description of the corresponding spin-wave excitations. The observed magnetic order and excitation spectra can be well understood in terms of an effective spin Hamiltonian with interactions ranging up to third-nearest-neighbor pairs. The results indicate that the helical magnetism in Sr 3 Fe 2 O 7 results from competition between ferromagnetic double-exchange and antiferromagnetic superexchange interactions whose strengths become comparable near the metal-insulator transition. They thus confirm a decades-old theoretical prediction and provide a firm experimental basis for models of magnetic correlations in strongly correlated metals. © 2014, American Physical Society.
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    Complex magnetic properties associated with competing local and itinerant magnetism in Pr2Co0.86Si2.88
    (Springer Nature, 2021-06-24) Kundu, M; Pakhira, S; Choudhary, R; Paudyal, D; Lakshminarasimhan, N; Avdeev, M; Cottrell, SP; Adroja, DT; Ranganathan, R; Mazumdar, C
    Ternary intermetallic compound Pr2Co0.86Si2.88 has been synthesized in single phase and characterized by x-ray diffraction, scanning electron microscopy with energy dispersive x-ray spectroscopy (SEM-EDX) analysis, magnetization, heat capacity, neutron diffraction and muon spin rotation/relaxation (μSR) measurements. The polycrystalline compound was synthesized in single phase by introducing necessary vacancies in Co/Si sites. Magnetic, heat capacity, and zero-field neutron diffraction studies reveal that the system undergoes magnetic transition below ∼4 K. Neutron diffraction measurement further reveals that the magnetic ordering is antiferromagnetic in nature with an weak ordered moment. The high temperature magnetic phase has been attributed to glassy in nature consisting of ferromagnetic clusters of itinerant (3d) Co moments as evident by the development of internal field in zero-field μSR below 50 K. The density-functional theory (DFT) calculations suggest that the low temperature magnetic transition is associated with antiferromagnetic coupling between Pr 4f and Co 3d spins. Pr moments show spin fluctuation along with unconventional orbital moment quenching due to crystal field. The evolution of the symmetry and the crystalline electric field environment of Pr-ions are also studied and compared theoretically between the elemental Pr and when it is coupled with other elements such as Co. The localized moment of Pr 4f and itinerant moment of Co 3d compete with each other below ∼20 K resulting in an unusual temperature dependence of magnetic coercivity in the system. This article is licensed under a Creative Commons Attribution 4.0 International License.
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    Crystal field excitations of YbMn2Si2
    (Elsevier Science BV, 2013-12-01) Mole, RA; Hofmann, M; Adroja, DT; Moze, O; Campbell, SJ
    The crystal field excitations of the rare earth intermetallic compound YbMn2Si2 have been measured by inelastic neutron scattering over the temperature range 2.5-50 K. The YbMn2Si2 spectra exhibit three low energy excitations (similar to 3-7 meV) in the antiferromagnetic AFil region above the magnetic phase transition at T-N2 = 30(5) K. The crystal field parameters have been determined for YbMn2Si2 in the antiferromagnetic AFil region. A further two inelastic excitations (similar to 9 meV, 17 meV) are observed below T-N2=30(5) K, the temperature at which the high temperature antiferromagnetic structure is reported to exhibit doubling of the magnetic cell. Energy level diagrams have been determined for Yb3+ ions in the different sites above (single site) and below the magnetic transition temperature (two sites). The excitation energies for both sites are shown to be temperature independent with the temperature dependences of the transition intensities for the two sites described well by a simple Boltzmann model. The spectra below T-N2 cannot be described fully in terms of molecular field models based on either a single Yb3+ site or two Yb3+ sites. This indicates that the magnetic behaviour of YbMn(2)Si2 is more complicated than previously considered. The inability to account fully for excitations below the magnetic phase transition may be due to an, as yet, unresolved structural transition associated with the magnetic transition. © 2013, Elsevier Ltd.
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    Electron doping effects on the spin spectroscopy of BaFe2-xNixAs2 superconductors
    (International Conference on Neutron Scattering, 2017-07-12) Luo, HQ; Gong, DL; Xie, T; Lu, XY; Kamazawa, K; Iida, K; Kajimoto, R; Ivanov, AS; Adroja, DT; Kulda, J; Danilkin, SA; Deng, GC; Li, SL; Dai, PC
    High-temperature superconductivity in iron pnictides emerges from electron or hole doped parent compounds with antiferromagnetic order, which is argued to be associated with both the presence of high-energy spin excitations and a coupling between low-energy spin excitations and itinerant electrons. With more than 6 years\' efforts, we have used time-of-flight neutron spectroscopy to extensively map out the spin excitations in the electron-doped BaFe2-xNixAs2 especially around the overdoped zone boundary of superconductivity. We have found that the high energy spin fluctuations survive in the extremely high doping x=0.6 far beyond the superconducting dome, but the low energy spin excitations including the spin resonance mode is very sensitive to the electron dopings, by finally forming a large spin gap just after the disappearance of superconductivity in the overdoped regime. Further polarized neutron analysis indicate that the spin gap actually is anisotropic, and the longitudinal mode of spin fluctuations, as a hallmark of the itinerant magnetism from Fermi surface nesting, is totally eliminated together with the hole pockets near the electron-overdoped zone boundary of superconductivity.Our results suggest that the strong fluctuations from local moments give framework for magnetic interaction, while itinerant spin excitations originated from Fermi surface nesting are crucial to the superconductivity in iron pnictides.
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    Electron doping evolution of the anisotropic spin excitations in BaFe(2-x)NixAs2
    (Americal Physical Society, 2012-07-10) Luo, HQ; Yamani, Z; Chen, YC; Lu, XY; Wang, M; Li, SL; Maier, TA; Danilkin, SA; Adroja, DT; Dai, PC
    We use inelastic neutron scattering to systematically investigate the Ni-doping evolution of the low-energy spin excitations in BaFe(2-x)NixAs2 spanning from underdoped antiferromagnet to overdoped superconductor (0.03 <= x <= 0.18). In the undoped state, BaFe2As2 changes from paramagnetic tetragonal phase to orthorhombic antiferromagnetic (AF) phase below about 138 K, where the low-energy (<=similar to 80 meV) spin waves form transversely elongated ellipses in the [H, K] plane of the reciprocal space. Upon Ni doping to suppress the static AF order and induce superconductivity, the c-axis magnetic exchange coupling is rapidly suppressed and the momentum distribution of spin excitations in the [H, K] plane is enlarged in both the transverse and longitudinal directions with respect to the in-plane AF ordering wave vector of the parent compound. As a function of increasing Ni-doping x, the spin excitation widths increase linearly but with a larger rate along the transverse direction. These results are in general agreement with calculations of dynamic susceptibility based on the random phase approximation (RPA) in an itinerant electron picture. For samples near optimal superconductivity at x approximate to 0.1, a neutron spin resonance appears in the superconducting state. Upon further increasing the electron doping to decrease the superconducting transition temperature T-c, the intensity of the low-energy magnetic scattering decreases and vanishes concurrently with vanishing superconductivity in the overdoped side of the superconducting dome. Comparing with the low-energy spin excitations centered at commensurate AF positions for underdoped and optimally doped materials (x <= 0.1), spin excitations in the overdoped side (x = 0.15) form transversely incommensurate spin excitations, consistent with the RPA calculation. Therefore, the itinerant electron approach provides a reasonable description to the low-energy AF spin excitations in BaFe(2-x)NixAs2. © 2012, American Physical Society.
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    Electron doping evolution of the magnetic excitations in BaFe(2-x)NixAs2
    (American Physical Society., 2013-10-25) Luo, HQ; Lu, XY; Zhang, R; Wang, M; Goremychkin, EA; Adroja, DT; Danilkin, SA; Deng, GC; Yamani, Z; Dai, PC
    We use inelastic neutron scattering (INS) spectroscopy to study the magnetic excitations spectra throughout the Brillouin zone in electron-doped iron pnictide superconductors BaFe2-xNixAs2 with x = 0.096,0.15,0.18. While the x = 0.096 sample is near optimal superconductivity with T-c = 20 K and has coexisting static incommensurate magnetic order, the x = 0.15,0.18 samples are electron overdoped with reduced T-c of 14 and 8 K, respectively, and have no static antiferromagnetic (AF) order. In previous INS work on undoped (x = 0) and electron optimally doped (x = 0.1) samples, the effect of electron doping was found to modify spin waves in the parent compound BaFe2As2 below similar to 100 meV and induce a neutron spin resonance at the commensurate AF ordering wave vector that couples with superconductivity. While the new data collected on the x = 0.096 sample confirm the overall features of the earlier work, our careful temperature dependent study of the resonance reveals that the resonance suddenly changes its Q width below T-c similar to that of the optimally hole-doped iron pnictides Ba0.67K0.33Fe2As2. In addition, we establish the dispersion of the resonance and find it to change from commensurate to transversely incommensurate with increasing energy. Upon further electron doping to overdoped iron pnictides with x = 0.15 and 0.18, the resonance becomes weaker and transversely incommensurate at all energies, while spin excitations above similar to 100 meV are still not much affected. Our absolute spin excitation intensity measurements throughout the Brillouin zone for x = 0.096,0.15,0.18 confirm the notion that the low-energy spin excitation coupling with itinerant electron is important for superconductivity in these materials, even though the high-energy spin excitations are weakly doping dependent. © 2013, American Physical Society.
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    Experimental observation and computational study of the spin-gap excitation in Ba3BiRu2O9
    (American Physical Society, 2016-11-01) Ling, CD; Huang, Z; Kennedy, BJ; Rols, S; Johnson, MR; Zbiri, M; Kimber, SAJ; Hudspeth, J; Adroja, DT; Rule, KC; Avdeev, M; Blanchard, PER
    Ba3BiRu2O9 is a 6H-type perovskite compound containing face-sharing octahedral M2O9 (M=Ir, Ru) dimers, which are magnetically frustrated at low temperatures. On cooling through T∗=176 K, it undergoes a pronounced magnetostructural transition, which is not accompanied by any change in space group symmetry, long-range magnetic ordering, or charge ordering. Here, we report the first direct evidence from inelastic neutron scattering that this transition is due to an opening of a gap in the excitation spectra of dimers of low-spin Ru4+ (S=1) ions. X-ray absorption spectroscopy reveals a change in Ru-Ru orbital overlap at T∗, linking the emergence of this spin-gap excitation to the magnetostructural transition. Ab initio calculations point to a geometrically frustrated magnetic ground state due to antiferromagnetic interdimer exchange on a triangular Ru2O9 dimer lattice. X-ray total-scattering data rule out long-range magnetic ordering at low temperatures, consistent with this geometrically frustrated model. ©2016 American Physical Society