skip to main content


Title: Successive Phase Transitions and Multiferroicity in Deformed Triangular-Lattice Antiferromagnets Ca 3 MNb 2 O 9 (M=Co, Ni) with Spatial Anisotropy
We constructed the magnetic field-temperature phase diagrams of new quasi-two-dimensional isosceles triangular lattice antiferromagnets (TLAF) Ca 3 MNb 2 O 9 (M=Co, Ni) from dc and ac magnetic susceptibilities, specific heat, dielectric constant, and electric polarization measurements on single crystalline samples. Ca 3 CoNb 2 O 9 with effective spin-1/2 Co 2+ ions undergoes a two-step antiferromagnetic phase transition at T N1 = 1.3 K and T N2 = 1.5 K and enters a stripe ordered state at zero magnetic field. With increasing field, successive magnetic phase transitions, reminiscent of the up-up-down ( uud ) and the oblique phases, are observed. The dielectric constant of Ca 3 CoNb 2 O 9 shows anomalies related to the magnetic phase transitions, but clear evidence of ferroelectricity is absent. Meanwhile, Ca 3 NiNb 2 O 9 with spin-1 Ni 2+ ions also shows a two-step antiferromagnetic transition at T N1 = 3.8 K and T N2 = 4.2 K at zero field. For Ca 3 NiNb 2 O 9 , the electric polarization in the magnetic ordered phases was clearly observed from the pyroelectric current measurements, which indicates its coexistence of magnetic ordering and ferroelectricity.  more » « less
Award ID(s):
2003117
NSF-PAR ID:
10417692
Author(s) / Creator(s):
; ; ; ; ;
Date Published:
Journal Name:
ECS Journal of Solid State Science and Technology
Volume:
11
Issue:
6
ISSN:
2162-8769
Page Range / eLocation ID:
063004
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract With the motivation to study how non-magnetic ion site disorder affects the quantum magnetism of Ba 3 CoSb 2 O 9 , a spin-1/2 equilateral triangular lattice antiferromagnet, we performed DC and AC susceptibility, specific heat, elastic and inelastic neutron scattering measurements on single crystalline samples of Ba 2.87 Sr 0.13 CoSb 2 O 9 with Sr doping on non-magnetic Ba 2+ ion sites. The results show that Ba 2.87 Sr 0.13 CoSb 2 O 9 exhibits (i) a two-step magnetic transition at 2.7 K and 3.3 K, respectively; (ii) a possible canted 120 degree spin structure at zero field with reduced ordered moment as 1.24 μ B /Co; (iii) a series of spin state transitions for both H ∥ ab -plane and H ∥ c -axis. For H ∥ ab -plane, the magnetization plateau feature related to the up–up–down phase is significantly suppressed; (iv) an inelastic neutron scattering spectrum with only one gapped mode at zero field, which splits to one gapless and one gapped mode at 9 T. All these features are distinctly different from those observed for the parent compound Ba 3 CoSb 2 O 9 , which demonstrates that the non-magnetic ion site disorder (the Sr doping) plays a complex role on the magnetic properties beyond the conventionally expected randomization of the exchange interactions. We propose the additional effects including the enhancement of quantum spin fluctuations and introduction of a possible spatial anisotropy through the local structural distortions. 
    more » « less
  2. null (Ed.)
    Abstract Multi-functional thin films of boron (B) doped Cr 2 O 3 exhibit voltage-controlled and nonvolatile Néel vector reorientation in the absence of an applied magnetic field, H . Toggling of antiferromagnetic states is demonstrated in prototype device structures at CMOS compatible temperatures between 300 and 400 K. The boundary magnetization associated with the Néel vector orientation serves as state variable which is read via magnetoresistive detection in a Pt Hall bar adjacent to the B:Cr 2 O 3 film. Switching of the Hall voltage between zero and non-zero values implies Néel vector rotation by 90 degrees. Combined magnetometry, spin resolved inverse photoemission, electric transport and scanning probe microscopy measurements reveal B-dependent T N and resistivity enhancement, spin-canting, anisotropy reduction, dynamic polarization hysteresis and gate voltage dependent orientation of boundary magnetization. The combined effect enables H  = 0, voltage controlled, nonvolatile Néel vector rotation at high-temperature. Theoretical modeling estimates switching speeds of about 100 ps making B:Cr 2 O 3 a promising multifunctional single-phase material for energy efficient nonvolatile CMOS compatible memory applications. 
    more » « less
  3. Abstract

    Next‐generation electronics and energy technologies can now be developed as a result of the design, discovery, and development of novel, environmental friendly lead (Pb)‐free ferroelectric materials with improved characteristics and performance. However, there have only been a few reports of such complex materials’ design with multi‐phase interfacial chemistry, which can facilitate enhanced properties and performance. In this context, herein, novel lead‐free piezoelectric materials (1‐x)Ba0.95Ca0.05Ti0.95Zr0.05O3‐(x)Ba0.95Ca0.05Ti0.95Sn0.05O3, are reported, which are represented as (1‐x)BCZT‐(x)BCST, with demonstrated excellent properties and energy harvesting performance. The (1‐x)BCZT‐(x)BCST materials are synthesized by high‐temperature solid‐state ceramic reaction method by varyingxin the full range (x= 0.00–1.00). In‐depth exploration research is performed on the structural, dielectric, ferroelectric, and electro‐mechanical properties of (1‐x)BCZT‐(x)BCST ceramics. The formation of perovskite structure for all ceramics without the presence of any impurity phases is confirmed by X‐ray diffraction (XRD) analyses, which also reveals that the Ca2+, Zr4+, and Sn4+are well dispersed within the BaTiO3lattice. For all (1‐x)BCZT‐(x)BCST ceramics, thorough investigation of phase formation and phase‐stability using XRD, Rietveld refinement, Raman spectroscopy, high‐resolution transmission electron microscopy (HRTEM), and temperature‐dependent dielectric measurements provide conclusive evidence for the coexistence of orthorhombic + tetragonal (Amm2+P4mm) phases at room temperature. The steady transition ofAmm2crystal symmetry toP4mmcrystal symmetry with increasingxcontent is also demonstrated by Rietveld refinement data and related analyses. The phase transition temperatures, rhombohedral‐orthorhombic (TR‐O), orthorhombic‐ tetragonal (TO‐T), and tetragonal‐cubic (TC), gradually shift toward lower temperature with increasingxcontent. For (1‐x)BCZT‐(x)BCST ceramics, significantly improved dielectric and ferroelectric properties are observed, including relatively high dielectric constantεr≈ 1900–3300 (near room temperature),εr≈ 8800–12 900 (near Curie temperature), dielectric loss, tanδ≈ 0.01–0.02, remanent polarizationPr≈ 9.4–14 µC cm−2, coercive electric fieldEc≈ 2.5–3.6 kV cm−1. Further, high electric field‐induced strainS≈ 0.12–0.175%, piezoelectric charge coefficientd33≈ 296–360 pC N−1, converse piezoelectric coefficient ≈ 240–340 pm V−1, planar electromechanical coupling coefficientkp≈ 0.34–0.45, and electrostrictive coefficient (Q33)avg≈ 0.026–0.038 m4C−2are attained. Output performance with respect to mechanical energy demonstrates that the (0.6)BCZT‐(0.4)BCST composition (x= 0.4) displays better efficiency for generating electrical energy and, thus, the synthesized lead‐free piezoelectric (1‐x)BCZT‐(x)BCST samples are suitable for energy harvesting applications. The results and analyses point to the outcome that the (1‐x)BCZT‐(x)BCST ceramics as a potentially strong contender within the family of Pb‐free piezoelectric materials for future electronics and energy harvesting device technologies.

     
    more » « less
  4. Abstract

    The crystal structure, electron energy-loss spectroscopy (EELS), heat capacity, and anisotropic magnetic and resistivity measurements are reported for Sn flux grown single crystals of orthorhombic Pr2Co3Ge5(U2Co3Si5-type,Ibam). Our findings show thato-Pr2Co3Ge5hosts nearly trivalent Pr ions, as evidenced by EELS and fits to temperature dependent magnetic susceptibility measurements. Complex magnetic ordering with a partially spin-polarized state emerges nearTsp= 32 K, with a spin reconfiguration transition nearTM= 15 K. Heat capacity measurements show that the phase transitions appear as broad peaks in the vicinity ofTspandTM. The magnetic entropy further reveals that crystal electric field splitting lifts the Hund’s rule degeneracy at low temperatures. Taken together, these measurements show that Pr2Co3Ge5is an environment for complexfstate magnetism with potential strongly correlated electron states.

     
    more » « less
  5. The sawtooth chain compound CsCo 2 (MoO 4 ) 2 (OH) is a complex magnetic system and here, we present a comprehensive series of magnetic and neutron scattering measurements to determine its magnetic phase diagram. The magnetic properties of CsCo 2 (MoO 4 ) 2 (OH) exhibit a strong coupling to the crystal lattice and its magnetic ground state can be easily manipulated by applied magnetic fields. There are two unique Co 2+ ions, base and vertex, with J bb and J bv magnetic exchange. The magnetism is highly anisotropic with the b -axis (chain) along the easy axis and the material orders antiferromagnetically at T N = 5 K. There are two successive metamagnetic transitions, the first at H c 1 = 0.2 kOe into a ferrimagnetic structure, and the other at H c 2 = 20 kOe to a ferromagnetic phase. Heat capacity measurements in various fields support the metamagnetic phase transformations, and the magnetic entropy value is intermediate between S = 3/2 and 1/2 states. The zero field antiferromagnetic phase contains vertex magnetic vectors (Co(1)) aligned parallel to the b -axis, while the base vectors (Co(2)) are canted by 34° and aligned in an opposite direction to the vertex vectors. The spins in parallel adjacent chains align in opposite directions, creating an overall antiferromagnetic structure. At a 3 kOe applied magnetic field, adjacent chains flip by 180° to generate a ferrimagnetic phase. An increase in field gradually induces the Co(1) moment to rotate along the b -axis and align in the same direction with Co(2) generating a ferromagnetic structure. The antiferromagnetic exchange parameters are calculated to be J bb = 0.028 meV and J bv = 0.13 meV, while the interchain exchange parameter is considerably weaker at J ch = (0.0047/ N ch ) meV. Our results demonstrate that the CsCo 2 (MoO 4 ) 2 (OH) is a promising candidate to study new physics associated with sawtooth chain magnetism and it encourages further theoretical studies as well as the synthesis of other sawtooth chain structures with different magnetic ions. 
    more » « less