Nonlinear optical materials are essential for the development of solid-state lasers. KBe2BO3F2 (KBBF) is a unique nonlinear optical material for generation of deep-ultraviolet coherent light; however, its industrial application is limited. Here, we report a new material NH4B4O6F, which exhibits a wide deep-ultraviolet transparent range and suitable birefringence that enables frequency doubling below 200 nm. NH4B4O6F possesses large nonlinear coefficients about 2.5 times that of KBBF. In addition, it is easy to grow bulk crystals and does not contain toxic elements.

Finding the Next Deep-Ultraviolet Nonlinear Optical Material: NH4B4O6F

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.

Deep ultraviolet (absorption edge 6.2 eV) nonlinear optical (NLO) materials are of current interest owing to their technological applications and materials design challenges. Technologically, the materials are used in laser systems, atto-second pulse generation, semiconductor manufacturing, and photolithography. Designing and synthesizing a deep UV NLO material requires crystallographic non-centrosymmetry, a wide UV transparency range, a large second-harmonic generating coefficient (dij > 0.39 pm/V), moderate birefringence (Δn ∼ 0.07), chemical stability and resistance to laser damage, and ease in the growth of large high-quality single crystals. This review examines the known deep UV NLO materials with respect to their crystal structure, band gap, SHG efficiency, laser damage threshold, and birefringence. Finally, future directions with respect to new deep UV NLO materials are discussed.

Deep Ultraviolet Nonlinear Optical Materials

Owing to their vital role in creating and controlling polarized light, birefringent materials are used extensively in various advanced optical systems which in turn impact a large, rapidly increasing range of applications in science and technology. Currently, the fairly small birefringence of MgF2 and the low transmittance of α-BaB2O4 (α-BBO) hinder their efficient application for wavelength below 200 nm. For example, deep-ultraviolet (DUV) birefringent materials for light polarization are urgently needed for DUV lithography. Here we demonstrate based on computational and experimental results that parallel chains of corner-connected planar sp2-hybridized BO3 groups found in Ca(BO2)2 effectively produce large birefringence. Ca(BO2)2 achieves three vital “best” properties including the shortest UV cutoff edge, the largest birefringence, and the highest laser-induced damage threshold (LIDT) compared to all the reported borate birefringent materials. On the basis of a Ca(BO2)2 single crystal, a DUV Glan polar...

Designing an Excellent Deep-Ultraviolet Birefringent Material for Light Polarization.

Optical anisotropy is a fundamental building block for linear and nonlinear optical components such as polarizers, wave plates, and phase-matching elements1–4. In solid homogeneous materials, the strongest optical anisotropy is found in crystals such as calcite and rutile5,6. Attempts to enhance anisotropic light–matter interaction often rely on artificial anisotropic micro/nanostructures (form birefringence)7–11. Here, we demonstrate rationally designed, giant optical anisotropy in single crystals of barium titanium sulfide (BaTiS3). This material shows an unprecedented, broadband birefringence of up to 0.76 in the mid- to long-wave infrared, as well as a large dichroism window with absorption edges at 1.6 μm and 4.5 μm for light with polarization along two crystallographic axes on an easily accessible cleavage plane. The unusually large anisotropy is a result of the quasi-one-dimensional structure, combined with rational selection of the constituent ions to maximize the polarizability difference along different axes.

Giant optical anisotropy in a quasi-one-dimensional crystal

A new nonlinear optical (NLO) material, Bi3TeBO9 (BTBO), is successfully grown from high temperature solution method. BTBO crystallizes in a polar space group of P63 with a framework structure composed of [Bi3O9] blocks, with TeO6 and BO3 interconnection. It is interesting that in the BTBO structure three types of NLO-active units, including stereochemically active lone pair cations (Bi3+ cations), second-order Jahn–Teller distorted octahedra (TeO6 octahedra) and π-orbital planar groups (BO3 groups), simultaneously exist. The additive contribution from these three types of groups results in an extremely large second harmonic generation (SHG) response in BTBO (about 20 times that of KDP), exhibiting the largest SHG effect among the known borate NLO materials. The enhancement of the nonlinear optical property is elucidated by the first-principles analysis.

“All-Three-in-One”: A New Bismuth–Tellurium–Borate Bi3TeBO9 Exhibiting Strong Second Harmonic Generation Response

Single crystals of the birefringent material Ba2Ca(B3O6)2 (BCBO) with dimensions up to 40 × 28 × 10 mm3 were successfully grown by top-seeded solution growth (TSSG) method from B2O3–NaF flux. It exhibits high transmittance in the range of 190–3000 nm with UV cutoff of 178 nm, which is much shorter than that (189 nm) of the commercial UV birefringent crystal, the high-temperature phase of BaB2O4 (α-BBO). Meanwhile, BCBO crystal has large birefringence (Δn = no – ne = 0.2524–0.0862) in the wavelength range from 178 to 3000 nm and without phase transition from room temperature to the melting point. A prototype of Glan–Taylor polarizer made from BCBO crystal showed an optical extinction ratio of 104:1, which is comparable to those of commercial birefringence crystals. The experimental results demonstrate that the BCBO crystal can be a new promising birefringent crystal for UV, especially the sub-200 nm deep-UV range.

Top-Seeded Solution Growth and Optical Properties of Deep-UV Birefringent Crystal Ba2Ca(B3O6)2

Cyanurates consisting of intrinsic planar π-conjugated 6-membered rings: An emerging source of optical functional materials

BaBe2BO3F3: A KBBF-Type Deep-Ultraviolet Nonlinear Optical Material with Reinforced [Be2BO3F2]∞ Layers and Short Phase-Matching Wavelength

Cs3Na(H2C3N3O3)4·3H2O: A Mixed Alkali‐Metal Hydroisocyanurate Nonlinear Optical Material Containing π‐Conjugated Six‐Membered‐Ring Units

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