The primary goal of this review is to present a clear chemical perspective of borates in order to stimulate and facilitate the discovery of new borate-based optical materials. These materials, whic...

Borates: A Rich Source for Optical Materials.

A novel noncentrosymmetric (NCS) polar fluoride sulfate, CsSbF2 SO4 , was obtained by ionothermal synthesis. A meticulously designed co-substitution approach was used to successfully replace the [TiO6 ]8- and [PO4 ]3- functional groups in KTiOPO4 (KTP) with [SbO4 F2 ]7- and [SO4 ]2- units, respectively. The structure of CsSbF2 SO4 features a pseudo-3D framework consisting of interconnected 1D [SbF2 O2 SO4 ]5- chains of corner-sharing [SbO4 F2 ]7- octahedra and [SO4 ]2- tetrahedra. The title compound exhibits a sharply enlarged band gap compared to its parent compound, KTP, benefitting from the introduction of F- ions and the displacement of Sb3+ cations. Second harmonic generation (SHG) measurements manifested that CsSbF2 SO4 is phase-matchable and revealed a strong SHG response of about 3.0 KH2 PO4 (KDP), which is the highest value reported for any metal sulfate reported to date. The reported fluoride sulfate is a promising near ultraviolet (UV) nonlinear optical (NLO) material.

CsSbF 2 SO 4 : An Excellent Ultraviolet Nonlinear Optical Sulfate with a KTiOPO 4 (KTP)-type Structure.

The precision of array of laser applications and manipulation on smaller scales are limited by the so-called 200 nm wall, and breakthroughs rely on the discovery of new materials with transparency ...

Uniform Alignment of Non-π-Conjugated Species Enhances Deep Ultraviolet Optical Nonlinearity.

Advances in the generation of coherent lasers at wavelengths below 200 nm as well as the associated equipment and technologies have greatly spurred the development of nonlinear optical (NLO) materials that are capable of phase-matching in the deep-ultraviolet (deep-UV) spectral regions. However, few crystals can meet the technical demands, and studies to date have focused mainly on finding the next competitive candidates. Consequently, several crystals have emerged that hold great potential for the production of deep-UV harmonic coherent light, which benefit from newly developed systems with novel NLO-active units and chromophores. This Review provides a comprehensive overview of the developments of emergent candidates in the field of deep-UV NLO materials, discussing the recent efforts and active advances in the search for superior systems and in understanding their structure-property relationships. The intention is to provide a clear perspective on the current emergent deep-UV NLO candidates, and to accelerate the discovery of next candidates with high performances to meet the urgent demands.

Emergent Deep-Ultraviolet Nonlinear Optical Candidates.

Exploring novel functional materials via chemical substitution-oriented design is an emerging strategy. The method can be expanded to the discovery of high performance ultraviolet (UV) nonlinear optical (NLO) solid state materials by a careful tuning of the substituted atoms. This minireview presents a brief introduction to chemical substitution-oriented design including single-site substitution, dual-site substitution, and multisite substitution. Several state-of-the-art UV NLO materials such as K3VO(O2)2CO3-type, KBe2BO3F2 (KBBF)-type, Ca5(PO4)3(OH)-type, and KTiOPO4 (KTP)-type phases successfully discovered by the chemical substitution method are discussed.

/pdf/novel-ultraviolet-uv-nonlinear-optical-nlo-materials-4v0hm2uvzp.pdf

Novel ultraviolet (UV) nonlinear optical (NLO) materials discovered by chemical substitution-oriented design

To combine noncentrosymmetry, large second order nonlinear optical (NLO) susceptibility, deep UV transparency, and phase matchability simultaneously into a single structure is a great challenge. Especially, the relationship between the macrophase matchability and microstructure has been less investigated. Herein, we report a unique Ba2NaClP2O7 representing the first phase-matchable example of the fresnoite family, which exhibits excellent NLO properties, including short absorption edge (<176 nm, ca. 7.0 eV), strong second-harmonic generations at the incident lasers of 850–1110 nm (obv. 0.9–1.3 × KDP; cal. dave, 1.11 vs 0.96 pm/V of KDP), and large laser-induced damage threshold (1.4 × KDP). More interestingly, Ba2NaClP2O7 illustrates an unprecedented mechanism of phase matchability that is promoted by crystallographic disorder. The uniaxial symmetry breaking caused by the disorder of [P2O7]4– group results in a structural anisotropy that changes the band dispersions along k-paths of G–Y and G–X, resulting...

Ba2NaClP2O7: Unprecedented Phase Matchability Induced by Symmetry Breaking and Its Unique Fresnoite-Type Structure.

Deep-ultraviolet (DUV) nonlinear optical (NLO) materials that have attracted considerable renewed interest are in great demand by the relevant industries, but there is a severe shortage of these materials. The existence of such a dilemma may be attributed to the extremely rigorous prerequisite for such materials, including a very wide energy gap (>6.2 eV), which can be met by only a few borates, phosphates, and carbonates; among them, only one, KBe2BO3F2 (KBBF), is practically usable. Herein, we theoretically identify PO3F2– as a novel DUV NLO building unit based on first-principles studies. In addition, we thoroughly survey more than 100 known monofluorophosphates and identify three of them, (NH4)2PO3F, [C(NH2)3]2PO3F, and NaNH4PO3F·H2O, as promising DUV NLO candidates. To confirm our prediction, we experimentally synthesize all of them. Interestingly, these compounds exhibit remarkably strong second harmonic generations [0.9–1.1 × KH2PO4 (KDP) at 1064 nm and 0.2–0.3 × β-Ba2B2O4 (BBO) at 532 nm] and high...

Monofluorophosphates: A New Source of Deep-Ultraviolet Nonlinear Optical Materials

Disclosed is a class of non-linear optical crystals, and specifically disclosed is a class of deep ultraviolet non-linear optical crystal monoflurophospates. A monoflurophospate crystal is firstly used as a deep ultraviolet non-linear optical crystal, and the class of crystals are a class of fully new non-linear optical materials. The crystal shows an excellent optical performance, has a relatively large non-linear response, a relatively large polarizability (up to 25.6) and a relatively wide transparent range, can achieve phase matching, has a relatively large band gap (with band gaps all above 6.5 eV), a relatively high frequency multiplication factor and a relatively high birefringence, and can be used as a deep ultraviolet non-linear optical crystal with better performances.

Non-linear optical crystal monoflurophospate

The invention provides a phosphate compound, the molecular formula of which is shown as NaBa2P2O7Cl. The compound is a nonlinear optical crystal. Preferably, the crystal has a non-centrosymmetric structure, the space group is P4bm, and the cell parameters are shown as the specification. The invention provides an NaBa2P2O7Cl compound and a preparation method thereof. The compound NaBa2P2O7Cl crystal has the advantages of good SHG performance and large band gap, is stable in air, is insoluble in water and insoluble in ethanol, and is a new deep ultraviolet nonlinear optical phosphate material. The synthesis method of NaBa2P2O7Cl is novel and simple, and greatly shortens the synthetic period.

Deep ultraviolet nonlinear optical phosphate crystal NaBa2P2O7Cl, preparation method and application thereof

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Ba2NaClP2O7: Unprecedented Phase Matchability Induced by Symmetry Breaking and Its Unique Fresnoite-Type Structure.

Monofluorophosphates: A New Source of Deep-Ultraviolet Nonlinear Optical Materials

Non-linear optical crystal monoflurophospate

Deep ultraviolet nonlinear optical phosphate crystal NaBa2P2O7Cl, preparation method and application thereof