• Journal of Inorganic Materials
  • Vol. 36, Issue 8, 865 (2021)
Jingsan HU1, Jianfei GU1, and Weiyi ZHANG1,2,*
Author Affiliations
  • 11. School of Physics, Nanjing University, Nanjing 210093, China
  • 22. National Laboratory of Solid State Microstructures and Department of Physics, Nanjing University, Nanjing 210093, China
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    DOI: 10.15541/jim20200623 Cite this Article
    Jingsan HU, Jianfei GU, Weiyi ZHANG. Mechanism of the Magnetic and Specific-heat Anomalies in Rare-earth Dodecaborides RB12 (R=Tb-Tm): an Effect of Crystal-field-splitting Order Parameter [J]. Journal of Inorganic Materials, 2021, 36(8): 865 Copy Citation Text show less

    Abstract

    Rare-earth dodecaborides RB12 (R=Tb, Dy, Ho, Er, Tm) are all characterized by a controversial and unresolved magnetic and specific-heat anomaly at low temperature (TC≈3-22 K) except LuB12 with closed f-shell. Although the bump feature in magnetic susceptibilities resembles that of antiferromagnetically ordered R3+ ions, no definite magnetic structure was identified by either neutron scattering or Mössbauer spectra. The anomalies in susceptibilities, entropy, and low temperature neutron diffraction pattern all pointed to the amplitude-modulated nature of complex magnetic structure. In view of the rather small crystal-field-splitting energies of the order of meV, we propose to treat crystal-field-splitting (CFS) energy as an order parameter rather than a quantum mechanical quantity. In this way, we found that not only the magnetic and specific-heat anomalies can be explained properly by a gradual quenching of R orbital moments, but also the low temperature satellite peaks of neutron scattering spectra can be understood in terms of the spontaneously (111) dimerised structure and inelastically absorbed rattling phonon modes.
    $H0=HSO+HCF+HZS$

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    $Yl{m}'σ|HSO|Ylmσ=0.5ξ[(lσm)(l+σm+1)    δmm+σδσσ¯+σmδmmδσσ]$

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    $Yl{m}'σ|HZS|Ylmσ=μBB    [0.5(nxiny)(lm)(l+m+1)δmm+1δσσ+    0.5(nx+iny)(l+m)(lm+1)δmm1δσσ+    (nx+iσny)δmmδσσ¯+nz(m+σ)δmmδσσ]$

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    $HCF=7i=1,σJifiσfiσ$

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    $V(r)=αe24 π ϵ0a+280Ze24 π ϵ0a5[(x4+y4+z4)35r4]    1344Ze24 π ϵ0a7[(x6+y6+z6)+ 154(x2y4+y2z4+    z2x4+x2z4+y2x4+z2y4)1514r6] $

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    $ Δ 10=2Ze24 π ϵ0a[56033r4a46720143r6a6] $

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    $ Δ 20=2Ze24 π ϵ0a[33611r4a42240143r6a6] $

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    $ΔV=ZNαe24 π ϵ023Qa2$

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    $TCNθD2kBθDMRB122(2 π /a)24 π ϵ0aZαe2 Δ 20$

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    $rin[1+βaiaTmrinn+γ]nrin$

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    $ χ nN=μBBIC14NμINexp(EIN/kBT)IC14Nexp(EIN/kBT)$

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    $C_{V}^{N}=\frac{1}{{{k}_{\text{B}}}{{T}^{2}}}\left\{ \frac{\sum\limits_{I}^{C_{14}^{N}}{{{(E_{I}^{N})}^{2}}\exp (-E_{I}^{N}/{{k}_{\text{B}}}T)}}{\sum\limits_{I}^{C_{14}^{N}}{\exp (-E_{I}^{N}/{{k}_{\text{B}}}T)}}- \right.\ \left. {{\left[ \frac{\sum\limits_{I}^{C_{14}^{N}}{E_{I}^{N}\exp (-E_{I}^{N}/{{k}_{\text{B}}}T)}}{\sum\limits_{I}^{C_{14}^{N}}{\exp (-E_{I}^{N}/{{k}_{\text{B}}}T)}} \right]}^{2}} \right\}$

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    Jingsan HU, Jianfei GU, Weiyi ZHANG. Mechanism of the Magnetic and Specific-heat Anomalies in Rare-earth Dodecaborides RB12 (R=Tb-Tm): an Effect of Crystal-field-splitting Order Parameter [J]. Journal of Inorganic Materials, 2021, 36(8): 865
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