Prediction of Novel van der Waals Boron Oxides with Superior Deep‐Ultraviolet Nonlinear Optical Performance

Abstract

Deep‐ultraviolet nonlinear optical (DUV NLO) materials are attracting increasing attention because of their structural diversity and complexity. Using the two‐dimensional (2D) crystal structure prediction method combined with the first‐principles calculations, here we propose layered 18‐membered‐ring (18MR) boron oxide B2O3 polymorphs as high‐performance NLO materials. 18MR‐B2O3 with the AA and AB stackings are potential DUV NLO materials. The superior performing 18MR‐B2O3AB has an unprecedentedly high second harmonic generation coefficient of 1.63 pm V−1, the largest among the DUV NLO materials, three times larger than that of the advanced DUV NLO material KBe2BO3F2 and comparable to that of β‐BaB2O4. Its unusually large birefringence of 0.196 at 400 nm guarantees the phase‐matching wavelength λPM to reach this material's extreme absorption edge of ≈154 nm.

KPb3(o-C5H4NCOO)2Cl5: a brand-new stable lead chloride with good comprehensive nonlinear optical performance

“…[1][2][3][4] Actuated by the rapid development of advanced technology, NLO crystals have significant applications in all-solid-lasers, laser guidance, precise micro-manufacturing, biological tissue imaging and advanced scientific instruments. [5][6][7][8][9][10][11] Over the past decades, scientists have made great efforts to explore NLO crystals and elucidate the relationship between their structures and NLO properties. Consequently, some famous NLO crystals, like β-BaB 2 O 4 (BBO), LiB 3 O 5 (LBO), KBe 2 BO 3 F 2 (KBBF), KH 2 PO 4 (KDP), KTiOPO 4 (KTP) and AgGaS 2 , have been commercialized.…”

An excellent lead oxyiodide with a strong second-harmonic generation response and a large birefringence induced by the oriented arrangement of highly distorted [PbO4I2] polyhedra

“…Nonlinear optical (NLO) crystals are of great interest in solidstate lasers and laser technology because their capability of frequency conversion can extend the output spectral ranges of laser sources. [1][2][3][4][5][6][7] NLO crystals like β-BaB 2 O 4 (BBO), LiB 3 O 5 (LBO), KBe 2 BO 3 F 2 (KBBF), KH 2 PO 4 (KDP), KTiOPO 4 (KTP) and AgGaS 2 (AGS) are widely used in precision micromanufacturing, medical treatment, information processing and laser nuclear fusion. [8][9][10][11] Motivated by the rapid development of advanced technology and modern equipment, the demands on NLO crystals have increased.…”

APb2(C7H3NO4)2I (A = K, Rb, Cs): rare stable nonlinear optical crystals with second-harmonic generation response and highly distorted lead core coordination polyhedra

“…Nonlinear optical (NLO) crystals are able to generate coherent lasers through frequency conversions, such as the second-harmonic generation (SHG) response. [1][2][3][4][5][6] Therefore, NLO crystals play a significant role in all-solid-state lasers, optical communication, integrated optics, laser guidance, precise micromanufacturing, biological tissue imaging and advanced scientific instruments. [7][8][9][10][11][12][13][14] Several well-known NLO crystals are widely used from the region of deep UV to IR, such as KBe 2 BO 3 F 2 (KBBF), β-BaB 2 O 4 (BBO), LiB 3 O 5 (LBO), KH 2 PO 4 (KDP), KTiOPO 4 (KTP), ZnGeP 2 and AgGaS 2 .…”