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Abstract Discovery of new materials with enhanced optical properties in the visible and UV‐C range can impact applications in lasers, nonlinear optics, and quantum optics. Here, the optical floating zone growth of a family of rare earth borates,RBa3(B3O6)3(R= Nd, Sm, Tb, Dy, and Er), with promising linear and nonlinear optical (NLO) properties is reported. Although previously identified to be centrosymmetric, the X‐ray analysis combined with optical second harmonic generation (SHG) assigns the noncentrosymmetricPspace group to these crystals. Characterization of linear optical properties reveals a direct bandgap of ≈5.61–5.72 eV and strong photoluminescence in both the visible and mid‐IR regions. Anisotropic linear and nonlinear optical characterization reveals both Type‐I and Type‐II SHG phase matchability, with the highest effective phase‐matched SHG coefficient of 1.2 pm V−1at 800‐nm fundamental wavelength (for DyBa3(B3O6)3), comparable to β‐BaB2O4(phase‐matchedd22≈ 1.9 pm V−1). Laser‐induced surface damage threshold for these environmentally stable crystals is 650–900 GW cm−2, which is four to five times higher than that of β‐BaB2O4, thus providing an opportunity to pump with significantly higher power to generate about six to seven times stronger SHG light. Since the SHG arises from disorder on the Ba‐site, significantly larger SHG coefficients may be realized by “poling” the crystals to align the Ba displacements. These properties motivate further development of this crystal family for laser and wide bandgap NLO applications.
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MgSiP 2 : An Infrared Nonlinear Optical Crystal with a Large Non‐Resonant Phase‐Matchable Second Harmonic Coefficient and High Laser Damage Threshold
Abstract 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 ofd14≈d36= 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 ofdeff,I≈80.2 pm V−1anddeff,II≈73.4 pm V−1. The outstanding properties of MgSiP2make it a highly attractive candidate for optical frequency conversion in the infrared.
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- PAR ID:
- 10441907
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Optical Materials
- Volume:
- 11
- Issue:
- 24
- ISSN:
- 2195-1071
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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