H. D. Zhou

Chinese Academy of Sciences, Peping, Beijing, China

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Publications (132)402.17 Total impact

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    ABSTRACT: The magnetic phases of the ideal spin-1/2 triangular-lattice antiferromagnet Ba3CoSb2O9 are identified and studied using Ba nuclear magnetic resonance (NMR) spectroscopy in magnetic fields ranging to 30T, oriented parallel and near perpendicular to the crystallographic ab-plane. For both directions, the saturation field is approximately 33T. Notably, the NMR spectra provide microscopic evidence for the stabilization of an up-up-down spin configuration for in-plane fields, giving rise to an one-third magnetization plateau (Msat/3), as well as for a higher field phase transition near to ∼(3/5)Msat for both field orientations. Phase transitions are signaled by the evolution of the NMR spectra, and in some cases through spin-lattice relaxation measurements. The results are compared with expectations obtained from a semi-classical energy density modeling, in which quantum effects are incorporated by effective interactions extracted from the spin-wave analysis of the two-dimensional model. The interlayer coupling also plays a significant role in the outcome. Good agreement between the model and the experimental results is achieved, except for the case of fields approaching the saturation value applied along the c-axis.
    Physical Review B 01/2015; 91(2):024410. · 3.66 Impact Factor
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    ABSTRACT: The origin of the spin liquid state in Tb$_2$Ti$_2$O$_7$ has challenged experimentalists and theorists alike for nearly 20 years. To improve our understanding of the exotic magnetism in Tb$_2$Ti$_2$O$_7$, we have synthesized a chemical pressure analog, Tb$_2$Ge$_2$O$_7$. Germanium substitution results in a lattice contraction and enhanced exchange interactions. We have characterized the magnetic ground state of Tb$_2$Ge$_2$O$_7$ with specific heat, ac and dc magnetic susceptibility, and polarized neutron scattering measurements. Akin to Tb$_2$Ti$_2$O$_7$, there is no long-range order in Tb$_2$Ge$_2$O$_7$ down to 20 mK. The Curie-Weiss temperature of $-19.2(1)$ K, which is more negative than that of Tb$_2$Ti$_2$O$_7$, supports the picture of stronger antiferromagnetic exchange. Polarized neutron scattering of Tb$_2$Ge$_2$O$_7$ reveals that at 3.5 K liquid-like correlations dominate in this system. However, below 1 K, the liquid-like correlations give way to intense short-range ferromagnetic correlations with a length scale related to the Tb-Tb distance. Despite stronger antiferromagnetic exchange, the ground state of Tb$_2$Ge$_2$O$_7$ has ferromagnetic character, in stark contrast to the pressure-induced antiferromagnetic order observed in Tb$_2$Ti$_2$O$_7$.
    Physical Review Letters 12/2014; 113:267205. · 7.73 Impact Factor
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    ABSTRACT: After nearly 20 years of study, the origin of the spin-liquid state in Tb_{2}Ti_{2}O_{7} remains a challenge for experimentalists and theorists alike. To improve our understanding of the exotic magnetism in Tb_{2}Ti_{2}O_{7}, we synthesize a chemical pressure analog: Tb_{2}Ge_{2}O_{7}. Substitution of titanium by germanium results in a lattice contraction and enhanced exchange interactions. We characterize the magnetic ground state of Tb_{2}Ge_{2}O_{7} with specific heat, ac and dc magnetic susceptibility, and polarized neutron scattering measurements. Akin to Tb_{2}Ti_{2}O_{7}, there is no long-range order in Tb_{2}Ge_{2}O_{7} down to 20 mK. The Weiss temperature of -19.2(1) K, which is more negative than that of Tb_{2}Ti_{2}O_{7}, supports the picture of stronger antiferromagnetic exchange. Polarized neutron scattering of Tb_{2}Ge_{2}O_{7} reveals that liquidlike correlations dominate in this system at 3.5 K. However, below 1 K, the liquidlike correlations give way to intense short-range ferromagnetic correlations with a length scale similar to the Tb-Tb nearest neighbor distance. Despite stronger antiferromagnetic exchange, the ground state of Tb_{2}Ge_{2}O_{7} has ferromagnetic character, in stark contrast to the pressure-induced antiferromagnetic order observed in Tb_{2}Ti_{2}O_{7}.
    Physical Review Letters 12/2014; 113(26):267205. · 7.73 Impact Factor
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    ABSTRACT: We have performed magnetic, electric, thermal, and neutron powder diffraction (NPD) experiments as well as density functional theory (DFT) calculations on Ba3MnNb2O9. All results suggest that Ba3MnNb2O9 is a spin-5/2 triangular lattice antiferromagnet (TLAF) with weak easy-axis anisotropy. At zero field, we observed a narrow two-step transition at TN1 = 3.4 K and TN2 = 3.0 K. The neutron diffraction measurement and the DFT calculation indicate a 120◦ spin structure in the ab plane with out-of-plane canting at low temperatures. With increasing magnetic field, the 120◦ spin structure evolves into up-up-down (uud) and oblique phases showing successive magnetic phase transitions, which fits well to the theoretical prediction for the 2D Heisenberg TLAF with classical spins. Multiferroicity is observed when the spins are not collinear but suppressed in the uud and oblique phases.
    Physical Review B 12/2014; 90(22):224402. · 3.66 Impact Factor
  • Phys. Rev. B. 11/2014; 90(18):184408.
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    ABSTRACT: A flop of electric polarization from $P$$\parallel$$c$ ($P_c$) to $P$$\parallel$$a$ ($P_a$) is observed in MnTiO$_3$ as a spin flop transition is triggered by a $c$-axis magnetic field, $H_{\|c}$=7 T. The critical magnetic field $H_{\|c}$ for $P_a$ is significantly reduced in Mn$_{1-x}$Ni$_x$TiO$_3$ (x=0.33). $P_a$ and $P_c$ have been observed with both $H_{\|c}$ and $H_{\|a}$. Neutron diffraction measurements revealed similar magnetic arrangements for the two compositions where the ordered spins couple antiferromagnetically with their nearest intra- and inter-planar neighbors. In the x=0.33 system, the uniaxial and planar anisotropies of Mn$^{2+}$ and Ni$^{2+}$ compete and give rise to a spin reorientation transition at $T_R$. A magnetic field, $H_{\|c}$, aligns the spins along $c$ for $T_R$$<$$T$$<$$T_N$. The rotation of the collinear spins away from the $c$-axis for $T$$<$$T_R$ alters the magnetic point symmetry and gives rise to a new ME susceptibility tensor form. Such linear ME response provides satisfactory explanation for the behavior of the field-induced electric polarization in both compositions. As the Ni content increases to x=0.5 and 0.68, the ME effect disappears as a new magnetic phase emerges.
    Physical Review B 09/2014; 90:144429. · 3.66 Impact Factor
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    ABSTRACT: We report the complex magnetic phase diagram and electronic structure of Cr2(Te1-xWx)O6 systems. While compounds with different x values possess the same crystal structure, they display different magnetic structures below and above xc = 0.7, where both the transition temperature TN and sublattice magnetization (Ms) reach a minimum. Unlike many known cases where magnetic interactions are controlled either by injection of charge carriers or by structural distortion induced via chemical doping, in the present case it is achieved by tuning the orbital hybridization between Cr 3d and O 2p orbitals through W 5d states. The result is supported by ab-initio electronic structure calculations. Through this concept, we introduce a new approach to tune magnetic and electronic properties via chemical doping.
    09/2014;
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    ABSTRACT: We report the complex magnetic phase diagram and electronic structure of Cr_{2}(Te_{1-x}W_{x})O_{6} systems. While compounds with different x values possess the same crystal structure, they display different magnetic structures below and above x_{c}=0.7, where both the transition temperature T_{N} and sublattice magnetization (M_{s}) reach a minimum. Unlike many known cases where magnetic interactions are controlled either by injection of charge carriers or by structural distortion induced via chemical doping, in the present case it is achieved by tuning the orbital hybridization between Cr 3d and O 2p orbitals through W 5d states. The result is supported by ab initio electronic structure calculations. Through this concept, we introduce a new approach to tune magnetic and electronic properties via chemical doping.
    Physical Review Letters 08/2014; 113(7):076406. · 7.73 Impact Factor
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    ABSTRACT: The crossover from localized- to itinerant-electron behavior is associated with many intriguing phenomena in condensed-matter physics. In this paper, we investigate the crossover from localized to itinerant regimes in the spinel system Mn$_{1-x}$Co$_x$V$_2$O$_4$. At low Co doping, orbital order (OO) of the localized electrons on the V3+ ions suppresses magnetic frustration by triggering a tetragonal distortion. With Co doping, electronic itinerancy melts the OO and suppresses the structural phase transition while the reduced spin-lattice coupling produces magnetic frustration. Neutron scattering measurements and first-principles-guided spin models reveal that the non-collinear state at high Co doping is produced by weakened local anisotropy and enhanced Co-V spin interactions.
    07/2014;
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    ABSTRACT: Low-temperature thermal conductivity (\kappa), as well as magnetization (M) and electric polarization (P), of multiferroic orthoferrite DyFeO_3 single crystals are studied with H \parallel c. When the crystal is cooled in zero field, M, P, and \kappa all consistently exhibit irreversible magnetic-field dependencies. In particular, with 500 mK < T \le 2 K, all these properties show two transitions at the first run of increasing field but only the higher-field transition is present in the subsequent field sweepings. Moreover, the ultra-low-T (T < 500 mK) \kappa(H) shows a different irreversibility and there is only one transition when the field is swept both up and down. All the results indicate a complex low-T H-T phase diagram involving successive magnetic phase transitions of the Fe^{3+} spins. In particular, the ground state, obtained with cooling to subKelvin temperatures in zero field, is found to be an unexplored phase.
    06/2014;
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    ABSTRACT: We present specific-heat and neutron-scattering results for the S = 1/2 quantum antiferromagnet (dimethylammonium)(3,5-dimethylpyridinium)CuBr4. The material orders magnetically at TN = 1.99(2) K, and magnetic excitations are accompanied by an energy gap of 0.30(2) meV due to spin anisotropy. The system is best described as coupled two-leg spin-1/2 ladders with the leg exchange Jleg = 0.60(2) meV, rung exchange Jrung = 0.64(9) meV, interladder exchange Jint = 0.19(2) meV, and an interaction-anisotropy parameter λ = 0.93(2), according to inelastic neutron-scattering measurements. In contrast to most spin ladders reported to date, the material is a rare example in which the interladder coupling is very near the critical value required to drive the system to a Neel-ordered phase without the assistance of a magnetic field.
    Physical Review B 05/2014; 89:174432. · 3.66 Impact Factor
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    ABSTRACT: We have carried out 63,65Cu NMR spectra measurements in magnetic field up to about 15.5 T on single crystal of a multiferroic triangular-lattice antiferromagnet CuCrO2. The measurements were performed for perpendicular and parallel orientation of the magnetic field with respect to the c-axis of the crystal, and the detailed angle dependence of the spectra on the magnetic field direction within ab-plane was studied. The shape of the spectra can be well described in the model of spiral spin structure proposed by recent neutron diffraction experiments. When field is rotated perpendicular to crystal c-axis, we observed, directly for the first time, a remarkable reorientation of spin plane simultaneous with rotation of the incommensurate wavevector by quantitatively deducing the conversion of less energetically favorable domain to a more favorable one. At high enough fields parallel to c-axis, the data are consistent with either a field-induced commensurate spiral magnetic structure or an incommensurate spiral magnetic structure with a disorder in the c direction, suggesting that high fields may have influence on interplanar ordering.
    05/2014;
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    ABSTRACT: Neutron and X-ray diffraction, magnetic susceptibility, and specific heat measurements have been used to investigate the magnetic and structural phase transitions of the spinel system Fe1+xCr2-xO4(0.0<=x<=1.0). The temperature versus Fe concentration (x) phase diagram features two magnetically ordered states and four structural states below 420 K. The complexity of the phase diagram is closely related to the change in the spin and orbital degrees of freedom induced by substitution of Fe ions for Cr ions. The systematic change in the crystal structure is explained by the combined effects of Jahn-Teller distortion, spin-lattice interaction, Fe2+-Fe3+ hopping, and disorder among Fe2+, Fe3+, and Cr3+ ions.
    04/2014; 89(13).
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    ABSTRACT: We present a detailed local probe study of the magnetic order in the oxychalcogenide La2O2Fe2OSe2 utilizing 57Fe Moessbauer, 139La NMR, and muon spin relaxation spectroscopy. This system can be regarded as an insulating reference system of the Fe arsenide and chalcogenide superconductors. From the combination of the local probe techniques we identify a non-collinear magnetic structure similar to Sr2F2Fe2OS2. The analysis of the magnetic order parameter yields an ordering temperature TN = 90.1 K and a critical exponent of beta = 0.133, which is close to the 2D Ising universality class as reported in the related oxychalcogenide family.
    04/2014;
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    ABSTRACT: The ferrimagnetic spinels MnB2O4 (B=Mn,V) exhibit a similar series of closely spaced magnetic and structural phase transitions at low temperatures, reflecting both magnetic frustration and a strong coupling between the spin and lattice degrees of freedom. Careful studies of excitations in MnB2O4 (B=Mn,V), and the evolution of these excitations with temperature, are important for obtaining a microscopic description of the role that magnetic excitations and spin-lattice coupling play in the low-temperature phase transitions of these materials. We report an inelastic light (Raman) scattering study of the temperature and magnetic-field dependences of one- and two-magnon excitations in MnV2O4 and Mn3O4. We observe a pair of q =0 one-magnon modes at 74 and 81 cm-1 in MnV2O4, which is in contrast with the single 80-cm-1 q =0 magnon that has been reported for MnV2O4 based on previous neutron-scattering measurements and spin-wave calculations. Additionally, we find that the two-magnon energy of MnV2O4 decreases ("softens") with decreasing temperature below TN, which we attribute to strong coupling between magnetic and vibrational excitations near the zone boundary.
    Physical Review B 03/2014; 89(13). · 3.66 Impact Factor
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    ABSTRACT: The spinel vanadates have become a model family for exploring orbital order on the frustrated pyrochlore lattice, and recent debate has focused on the symmetry of local crystal fields at the cation sites. Here, we present neutron scattering measurements of the magnetic excitation spectrum in $\mathrm{FeV_2O_4}$, a recent example of a ferrimagnetic spinel vanadate which is available in single crystal form. We report the existence of two emergent magnon modes at low temperatures, which draw strong parallels with the closely related material, $\mathrm{MnV_2O_4}$. We were able to reproduce the essential elements of both the magnetic ordering pattern and the dispersion of the inelastic modes with semi- classical spin wave calculations, using a minimal model that implies a sizeable single-ion anisotropy on the vanadium sublattice. Taking into account the direction of ordered spins, we associate this anisotropy with the large trigonal distortion of $\mathrm{VO_6}$ octahedra, previously observed via neutron powder diffraction measurements. We further report on the spin gap, which is an order-of-magnitude larger than that observed in $\mathrm{MnV_2O_4}$. By looking at the overall temperature dependence, we were able to show that the gap magnitude is largely associated with the ferro-orbital order known to exist on the iron sublattice, but the contribution to the gap from the vanadium sublattice is in fact comparable to what is reported in the Mn compound. This reinforces the conclusion that the spin canting transition is associated with the ordering of vanadium orbitals in this system, and closer analysis indicates closely related physics underlying orbital transitions in $\mathrm{FeV_2O_4}$ and $\mathrm{MnV_2O_4}$.
    03/2014;
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    ABSTRACT: We have investigated the magnetic and electric ground states of a quasi-two-dimensional triangular lattice antiferromagnet (TLAF), Ba3CoNb2O9, in which the effective spin of Co2+ is 1/2. At zero field, the system undergoes a two-step transition upon cooling at TN2=1.36 K and TN1=1.10 K and enters a 120∘ ordered state. By applying magnetic fields, a series of spin states with fractions of the saturation magnetization Ms are observed. They are spin states with 1/3, 1/2, 2/3 (or √3 /3) Ms. The ferroelectricity emerges in all spin states, either with collinear or noncollinear spin structure, which makes Ba3CoNb2O9 another unique TLAF exhibiting both a series of magnetic phase transitions and multiferroicity. We discuss the role of quantum fluctuations and magnetic anisotropy in contributing more complex phase diagram compared to its sister multiferroic TLAF compound Ba3NiNb2O9 [J. Hwang et al., Phys. Rev. Lett. 109, 257205 (2012), 10.1103/PhysRevLett.109.257205].
    02/2014; 89(10).
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    ABSTRACT: The linear and nonlinear ac susceptibility measurements of Yb-pyrochlores, Yb2X2O7 (X =Sn, Ti, and Ge), show transitions with a ferromagnetic nature at 0.13 and 0.25 K for Yb2Sn2O7 and Yb2Ti2O7, respectively, and an antiferromagnetic ordering at 0.62 K for Yb2Ge2O7. These systematical results (i) provided information about the nature of the unconventional magnetic ground state in Yb2Ti2O7; (ii) realized a distinct antiferromagnetic ordering state in Yb2Ge2O7; and (iii) demonstrated that the application of chemical pressure through the series of Yb-pyrochlores can efficiently perturb the fragile quantum spin fluctuations of the Yb3+ ions and lead to very different magnetic ground states.
    Physical Review B 02/2014; 89(6):064401. · 3.66 Impact Factor
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    ABSTRACT: A cubic Er2Ge2O7 pyrochlore was prepared under high-pressure and high-temperature conditions and its magnetic ground state was investigated by measurements of specific heat, dc and ac magnetic susceptibility as functions of temperature, pressure, and magnetic field. We found that Er2Ge2O7 undergoes a long-range antiferromagnetic transition at TN ≈ 1.4 K, which can be further enhanced by applying external physical pressure. On the other hand, application of external magnetic fields suppresses the antiferromagnetic order to zero temperature around Hc ≈ 2.3 T, where a magnetic-field-induced spin-flop transition was observed. Hc increases accordingly with increasing TN under external pressure. A comparison of the magnetic ground states and structural variations along the isostructural series Er2B2O7 (B = Sn, Ti, Ge) together with the high-pressure study on Er2Ge2O7 indicated that the magnetic properties of these highly frustrated XY pyrochlore antiferromagnets are very sensitive to the minute structural changes that determine the anisotropic exchange interactions and the local crystal-electric-field environments of Er3+ ions.
    Phys. Rev. B. 02/2014; 89(6):064409.
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    ABSTRACT: We study vanadium spinels AV_{2}O_{4}(A=Cd,Mg) in pulsed magnetic fields up to 65 T. A jump in magnetization at μ_{0}H≈40 T is observed in the single-crystal MgV_{2}O_{4}, indicating a field induced quantum phase transition between two distinct magnetic orders. In the multiferroic CdV_{2}O_{4}, the field induced transition is accompanied by a suppression of the electric polarization. By modeling the magnetic properties in the presence of strong spin-orbit coupling characteristic of vanadium spinels, we show that both features of the field induced transition can be successfully explained by including the effects of the local trigonal crystal field.
    Physical Review Letters 01/2014; 112(1):017207. · 7.73 Impact Factor

Publication Stats

644 Citations
402.17 Total Impact Points

Institutions

  • 2014
    • Chinese Academy of Sciences
      • Institute of Physics
      Peping, Beijing, China
  • 2013–2014
    • University of Tennessee
      • Department of Physics & Astronomy
      Knoxville, Tennessee, United States
    • University of Manitoba
      • Department of Chemistry
      Winnipeg, Manitoba, Canada
  • 2012–2014
    • The University of Tennessee Medical Center at Knoxville
      Knoxville, Tennessee, United States
  • 2006–2014
    • Florida State University
      • • Department of Chemistry and Biochemistry
      • • Department of Physics
      Tallahassee, Florida, United States
  • 2007–2013
    • National High Magnetic Field Laboratory
      Tallahassee, Florida, United States
  • 2004–2013
    • University of Texas at Austin
      • Department of Materials Science and Engineering
      Austin, Texas, United States