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arXiv 2004.14038cond-mat.str-el
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Fe $_2$ Mo $_3$ O $_8$的结构、声子和轨道自由度

Structure, phonons, and orbital degrees of freedom in Fe$_2$Mo$_3$O$_8$

S. Reschke, A. A. Tsirlin, N. Khan, L. Prodan, V. Tsurkan, I. Kézsmárki, J. Deisenhofer

摘要:

我们报告了多铁性Fe $_2$ Mo $_3$ O $_8$的结构和光谱表征。同步辐射X射线和中子衍射,以及热膨胀测量揭示了晶格异常在$T_{\mathrm{N}}\simeq 60\,$ K,但没有显示任何对称性降低的磁有序状态。晶格参数$c$表现出非单调行为,在$200\,$ K附近具有明显的最小值,这也反映在一些观察到的红外活性光激发的异常行为中,并且与短程磁序的开始平行。在5和300 $\,$ K之间测量的红外反射率光谱的频率范围为$100-8000\,$ cm $^{-1}$揭示了大多数预期的声子模式与密度泛函计算得到的本征频率相比。的$A_1$声子显示整体硬化冷却后,而观察到的一些$E_1$模式的非单调行为。这些模式也显示出强烈增加的声子寿命低于$T_\mathrm{N}$,这与磁有序状态中的轨道矩的淬灭方向。在四面体Fe $^{2+}$位点的较高位置的$d$-$d$激发的寿命中观察到类似的增加,其仅在$T_\mathrm{N}$下方变得清晰可见。

英文摘要:

We report on the structural and spectroscopic characterization of the multiferroic Fe$_2$Mo$_3$O$_8$. Synchrotron x-ray and neutron diffraction, as well as thermal expansion measurements reveal a lattice anomaly at $T_{\mathrm{N}}\simeq 60\,$K but do not show any symmetry lowering in the magnetically ordered state. The lattice parameter $c$ exhibits a non-monotonic behavior with a pronounced minimum around $200\,$K, which is also reflected in an anomalous behavior of some of the observed infrared-active optical excitations and parallels the onset of short-range magnetic order. The infrared reflectivity spectra measured between 5 and 300$\,$K in the frequency range of $100-8000\,$cm$^{-1}$ reveal most of the expected phonon modes in comparison with the eigenfrequencies obtained by density-functional calculations. The $A_1$ phonons show an overall hardening upon cooling, whereas a non-monotonic behavior is observed for some of the $E_1$ modes. These modes also show a strongly increased phonon lifetime below $T_\mathrm{N}$, which we associate with the quenched direction of the orbital moment in the magnetically ordered state. A similar increase is observed in the lifetime of the higher-lying $d$-$d$ excitations of the tetrahedral Fe$^{2+}$ site, which become clearly visible below $T_\mathrm{N}$ only.

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