论文标题

II型II多种候选物RBFE(AO4)2(A = MO,SE,S)的二阶非线性光学和线性UV-VIS吸收特性

Second-order nonlinear optical and linear UV-VIS absorption properties of type-II multiferroic candidates RbFe(AO4)2 (A = Mo, Se, S)

论文作者

Owen, Rachel, Drueke, Elizabeth, Albunio, Charlotte, Kaczmarek, Austin, Jin, Wencan, Obeysekera, Dimuthu, Cheong, Sang-Wook, Yang, Junjie, Cundiff, Steven, Zhao, Liuyan

论文摘要

通过搜索II型多表情的启发,我们提供了一项复杂的II型氧化物家族的全面光学研究:RBFE(MOO4)2,RBFE(SEO4)2和RBFE(SO4)2。我们采用旋转 - 动构第二谐波生成光谱(RA SHG),一种对点对称性敏感的技术,以解决文献分配的点/空间组中的差异并识别正确的晶体结构。在室温下,我们发现我们的RA SHG图案从RBFE(AO4)2(A = SE,S)的晶轴旋转,这表明缺乏镜子对称性和平面内旋转对称性。同样,RBFE(SEO4)2的SHG效率比RBFE(AO4)2(A = MO,S)强两个数量级,这表明反转对称性破裂。此外,我们使用紫外线可见(UV-VIS)吸收光谱谱图在该材料家族的带边缘附近呈现温度依赖性线性光学特性。其中包括该家族的带隙能量和带隙过渡类型的实验证据。还提出了以前未报告的子带间隙吸收,这揭示了突出的光学转变,其中一些具有不寻常的中央能量依赖性。此外,我们发现,通过在RBFE(AO4)2(A = MO,SE,S)中取代A位点,上述过渡是可以调节的。最后,我们讨论了这些可调节过渡的潜在起源和影响。

Motivated by the search for type-II multiferroics, we present a comprehensive optical study of a complex oxide family of type-II multiferroic candidates: RbFe(MoO4)2, RbFe(SeO4)2, and RbFe(SO4)2. We employ rotational-anisotropy second harmonic generation spectroscopy (RA SHG), a technique sensitive to point symmetries, to address discrepancies in literature-assigned point/space groups and to identify the correct crystal structures. At room temperature we find that our RA SHG patterns rotate away from the crystal axes in RbFe(AO4)2 (A = Se, S), which identifies the lack of mirror symmetry and in-plane two-fold rotational symmetry. Also, the SHG efficiency of RbFe(SeO4)2 is two orders of magnitude stronger than RbFe(AO4)2 (A = Mo, S), which suggests broken inversion symmetry. Additionally, we present temperature-dependent linear optical characterizations near the band edge of this family of materials using ultraviolet-visible (UV-VIS) absorption spectroscopy. Included is experimental evidence of the band gap energy and band gap transition type for this family. Previously unreported sub-band gap absorption is also presented, which reveals prominent optical transitions, some with an unusual central energy temperature dependence. Furthermore, we find that by substituting the A-site in RbFe(AO4)2 (A = Mo, Se, S), the aforementioned transitions are spectrally tunable. Finally, we discuss the potential origin and impact of these tunable transitions.

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