Stereoactive oxysalts can exhibit excellent nonlinear optical coefficients and linear optical properties, like large birefringence and strong second harmonic generation (SHG) intensity, due to the stereo-chemically active lone pair electrons. Recently, a series of stereoactive oxysalts with new structures and strong performances have been reported, such as RbTeMo2O8F (27 × KDP, 0.263@546 nm), Pb2Bi(SeO3)2Cl3 (13.5 × KDP, 0.186@1064 nm), Y3F(SeO3)4 (5.5 × KDP, 5.03 eV), Bi(IO3)F2 (11.5 × KDP, 0.209@1064 nm) and K2Sb(P2O7)F (4.0 × KDP, 0.157@546 nm), etc. In this review, we summarized the recent progresses on stereoactive oxysalts by focusing on their structures and linear/nonlinear optical applications, surveying over a thousand newly reported compounds. Based on the different types of the centered cations, the reported stereoactive oxysalts compounds were classified into five different categories, metal antimonites, metal selenites, metal tellurites, metal iodates and metal bromates. We believe that stereoactive oxysalts are the promising candidates for many advanced functional materials and hope this paper can provide some perspectives for the development of new stereoactive oxysalts. More importantly, this comprehensive review not only introduces the rich structural and chemical properties of stereoactive oxysalts for graduate students and postdoctoral researchers, but also serves as a comprehensive reference for researchers studying optical properties of stereoactive oxysalts materials. 

A survey of stereoactive oxysalts for linear and nonlinear optical applications

/pdf/a-review-on-the-advancements-in-the-characterization-of-the-8370oim9.pdf

A review on the advancements in the characterization of the high-pressure properties of iodates

The nonlinear optical (NLO) crystals that can expand the wavelength of the laser to the deep-ultraviolet (DUV) region by the cascaded second harmonic generation (SHG) are of current research interest. It is well known that borates are the most ideal material class for the design of new DUV NLO crystals owing to the presence of good NLO genes, e.g., BO3 or B3O6 groups. However, the NLO pyro-borates with the B2O5 dimers as the sole basic building units are still rarely reported owing to their small SHG responses. In this communication, by constructing a planar pentagonal [Ca(B2O5)]∞ layer, the NLO pyro-borate Ba4Ca(B2O5)2F2 with a large SHG response (∼2.2 × KDP, or ∼7 × α-Li4B2O5) and a DUV transparent window has been designed and synthesized. The first-principles calculations show that the large SHG response of Ba4Ca(B2O5)2F2 mainly originates from the better π-conjugation of the coplanar B2O5 dimers in the [Ca(B2O5)]∞ layer. In addition, the planar pentagonal pattern in the [Ca(B2O5)]∞ layer provides an ideal template for designing the new DUV NLO crystals, apart from those in known DUV borates, e.g., the [Be2BO3F2]∞ layer in KBe2BO3F2 (KBBF).

/pdf/ba4ca-b2o5-2f2-p-conjugation-of-b2o5-in-the-planar-52tbuy61wp.pdf

Ba4Ca(B2O5)2F2: π-conjugation of B2O5 in the planar pentagonal layer achieving large second harmonic generation of pyro-borate.

Advances in aliovalent substitution strategy for the design and synthesis of nonlinear optical materials: d0 transition metal/gallium iodates and selenites

Nonlinear optical (NLO) crystals are an essential support for laser applications, as they could extend the tunable range of all-solid-state lasers. NLO inorganic sulfates always exhibit a large band gap and a moderate second harmonic generation response, which should be a rich source of NLO materials. However, due to the high symmetry of the [SO4] tetrahedron, most of the inorganic sulfates present insufficient phase matching ability, the improvement of which will bring the rapid advance of NLO materials. Therefore, in this review, the development of NLO inorganic sulfates is briefly discussed and the structures with a good phase matching ability are carefully investigated. On the basis of the structure–property relationships, four design strategies to improve their phase matching ability are summarized, including (1) the combination of the planar group; (2) the cooperation of highly polarized cations; (3) the synergy of multiple functional motifs such as [IO3] triangular pyramids and highly polarized cations; (4) the development of polar structures with ferroelectricity. All these strategies effectively improve the phase matching ability of sulfates, while most of them also bring the reduction of the band gap. In order to give full play of the large band gap of sulfates and develop deep-ultraviolet NLO inorganic sulfates, we propose that much attention should be paid to the combination of the planar group based on the birefringence phase matching and the polar structures with ferroelectricity based on the quasi-phase matching. Finally, we hope that this review could provide some inspiration for the design of NLO crystals. 

Nonlinear optical inorganic sulfates: The improvement of the phase matching ability driven by the structural modulation

A new borate fluoride, Li3CaB2O5F, has been synthesized. It features a sandwich-like structure with the adjacent [Li3OF]∞ and [CaO]∞ layers connected by the weak Li–O bonds and the [B2O5] dimers. Interestingly, Li3CaB2O5F has large ionic conductivity, which is attributed to the diverse and wide Li-ion diffusion pathways.

Li3CaB2O5F: a unique sandwich-like structure with diverse and wide Li ion diffusion pathways

F-containing early-transition-metal (ETM) iodates are an interesting materials class for the exploration of nonlinear optical (NLO) crystals. However, their rational structural design remains a great challenge due to the poor...

Cs2VOF4(IO2F2): Rationally Designing A Noncentrosymmetric Early-Transition-Metal Fluoroiodate

Na7(IO3)(SO4)3: the first noncentrosymmetric alkaline-metal iodate-sulfate with isolated [IO3] and [SO4] units.

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Li3CaB2O5F: a unique sandwich-like structure with diverse and wide Li ion diffusion pathways

Cs2VOF4(IO2F2): Rationally Designing A Noncentrosymmetric Early-Transition-Metal Fluoroiodate

Na7(IO3)(SO4)3: the first noncentrosymmetric alkaline-metal iodate-sulfate with isolated [IO3] and [SO4] units.