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Motivated by the search for type-II multiferroics, we present a comprehensiveoptical study of a complex oxide family of type-II multiferroic candidates:RbFe(MoO4)2, RbFe(SeO4)2, and RbFe(SO4)2. We employ rotational-anisotropysecond harmonic generation spectroscopy (RA SHG), a technique sensitive topoint symmetries, to address discrepancies in literature-assigned point/spacegroups and to identify the correct crystal structures. At room temperature wefind 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-foldrotational symmetry. Also, the SHG efficiency of RbFe(SeO4)2 is two orders ofmagnitude stronger than RbFe(AO4)2 (A = Mo, S), which suggests broken inversionsymmetry. Additionally, we present temperature-dependent linear opticalcharacterizations near the band edge of this family of materials usingultraviolet-visible (UV-VIS) absorption spectroscopy. Included is experimentalevidence of the band gap energy and band gap transition type for this family.Previously unreported sub-band gap absorption is also presented, which revealsprominent optical transitions, some with an unusual central energy temperaturedependence. 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 tunabletransitions.

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