Superior infrared nonlinear optical (NLO) crystals are in urgent demand in the development of lasers and optical technologies for communications and computing. The critical challenge is to find a crystal with large non‐resonant phase‐matchable NLO coefficients and high laser damage threshold (LDTs) simultaneously, which however scale inversely. This work reports such a material, MgSiP2,that exhibits a large second harmonic generation (SHG) coefficient of
Nonlinear optical (NLO) crystals with superior properties are significant for advancing laser technologies and applications. Introducing rare earth metals to borates is a promising and effective way to modify the electronic structure of a crystal to improve its optical properties in the visible and ultraviolet range. In this work, we computationally discover inversion symmetry breaking in EuBa3(B3O6)3, which was previously identified as centric, and demonstrate noncentrosymmetry via synthesizing single crystals for the first time by the floating zone method. We determine the correct space group to be
- NSF-PAR ID:
- 10472877
- Publisher / Repository:
- Optical Society of America
- Date Published:
- Journal Name:
- Optical Materials Express
- Volume:
- 13
- Issue:
- 12
- ISSN:
- 2159-3930
- Format(s):
- Medium: X Size: Article No. 3416
- Size(s):
- ["Article No. 3416"]
- Sponsoring Org:
- National Science Foundation
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Abstract d 14≈d 36= 89 ± 5 pm V−1at 1550 nm fundamental wavelength, surpassing the commercial NLO crystals AgGaS2, AgGaSe2, and ZnGeP2. First principles theory reveals the polarizability and geometric arrangement of the [SiP4] tetrahedral units as the origin of this large nonlinear response. Remarkably, it also exhibits a high LDT value of 684 GW cm−2, which is six times larger than ZnGeP2and three times larger than CdSiP2. It has a wide transparency window of 0.53–10.35 µm, allowing broadband tunability. Further, it is Type I and Type II phase‐matchable with large effective SHG coefficients ofd eff,I≈80.2 pm V−1andd eff,II≈73.4 pm V−1. The outstanding properties of MgSiP2make it a highly attractive candidate for optical frequency conversion in the infrared. -
Abstract Nonlinear optical (NLO) materials are of intense academic and technological interest attributable to their ability to generate coherent radiation over a range of different wavelengths. The requirements for a viable NLO material are rather strict, and their discovery has mainly been serendipitous. This study reports synthesis, characterization, and, most importantly, growth of large single crystals of a technologically viable NLO material—Rb3Ba3Li2Al4B6O20F. Through the judicious selection of cations, Rb3Ba3Li2Al4B6O20F exhibits a 3D structure that facilitates the growth of large single crystals along the optical axis direction. Measurements on these crystals indicate that Rb3Ba3Li2Al4B6O20F exhibits a moderate birefringence of 0.057 at 1064 nm enabling Type I phase‐matching down to 243 nm. Theoretical calculations indicate the symmetry adapted mode displacement (SAMD) parameter scales with the second‐harmonic generation intensity.
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Abstract Borate halides are an ideal materials class from which to design high‐performance nonlinear optical (NLO) materials. Currently, borate fluorides, chlorides, and bromides are extensively investigated while borate iodide materials discovery remains rare because of the perceived synthetic challenges. We report a new borate iodide, Pb2BO3I, synthesized by a straightforward hydrothermal method. The Pb2BO3I chemical formula conceals that the compound exhibits a structure similar to the well‐established KBe2BO3F2(KBBF), which we show supports the highest second‐harmonic generation (SHG) at 1064 nm in the KBBF family, 10 × KH2PO4(KDP), arising from the inclusion of Pb2+and I−and the crystal chemistry. Our work shows that KBBF‐related compounds can be synthesized incorporating iodide and exhibit superior NLO responses.
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Abstract Borate halides are an ideal materials class from which to design high‐performance nonlinear optical (NLO) materials. Currently, borate fluorides, chlorides, and bromides are extensively investigated while borate iodide materials discovery remains rare because of the perceived synthetic challenges. We report a new borate iodide, Pb2BO3I, synthesized by a straightforward hydrothermal method. The Pb2BO3I chemical formula conceals that the compound exhibits a structure similar to the well‐established KBe2BO3F2(KBBF), which we show supports the highest second‐harmonic generation (SHG) at 1064 nm in the KBBF family, 10 × KH2PO4(KDP), arising from the inclusion of Pb2+and I−and the crystal chemistry. Our work shows that KBBF‐related compounds can be synthesized incorporating iodide and exhibit superior NLO responses.
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Abstract Calcium germanides with two mid‐late rare‐earth metals, Ca5−
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