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Exploration of the deep-ultraviolet nonlinear optical materials in the derivatives of KBe2BO3F2

Gai Min-Qiang ,  Wang Ying ,  Pan Shi-Lie

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Exploration of the deep-ultraviolet nonlinear optical materials in the derivatives of KBe2BO3F2

Gai Min-Qiang, Wang Ying, Pan Shi-Lie
Acta Phys. Sin., 2019, 68(2): 024208.
doi: 10.7498/aps.68.20182145
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  • Abstract

    The use of nonlinear optical crystal materials to extend the limited range of laser sources to the deep-ultraviolet (deep-UV, λ < 200 nm) regions by various frequency conversion techniques, has become an attractive field for generating deep-UV light. However, the lack of nonlinear optics (NLO) crystal materials capable of frequency conversion in the deep-UV light range, limits the development and application of deep-UV all-solid-state lasers. Therefore, scientists all over the world are actively exploring the new generation of deep-UV NLO crystal materials. At present, only the KBe2BO3F2 (KBBF) crystal is capable of generating deep-UV light through the direct sixth harmonic generation of the Nd:YAG laser. The infinite ∞[Be2BO3F2]− single layers, as the brilliant building blocks in the crystal structures of KBBF family, provide a relatively large second harmonic generation coefficient (d11 = 0.47 pm/V) and a sufficient birefringence (Δn = 0.07@1064 nm). However, the KBBF crystals have insurmountable intrinsic defects, such as the usage of high toxic beryllium oxide, and the serious layer growth habit, which greatly restrict its commercialization process. Since the layered structure of the KBBF crystal is still one of the most brilliant structures for generating deep-UV laser, an effective strategy is to change the interlayer connection mode and develop new NLO materials based on KBBF with less layering growth habit. In this paper, by reviewing the development history of borate deep-UV NLO crystals and the derivatives of KBBF, the relationship between layered structure and optical properties of different interlaminar connections of crystal materials is systematically analyzed. We discuss the main contradictions and solutions of the development of deep-UV NLO crystal materials which are similar to the KBBF structure. In order to provide a reference for the innovative exploration of new materials in the future, several design strategies are also proposed.

    Authors and contacts

    • 1.

      CAS Key Laboratory of Functional Materials and Devices for Special Environments, Xinjiang Key Laboratory of Electronic Information Materials and Devices, the Xinjiang Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Urumqi 830011, China

    • 2.

      Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

      • Corresponding author: Pan Shi-Lie, slpan@ms.xjb.ac.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51602341, 51425206, 91622107).

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  • 图 1  KBBF族晶体结构模型

    Figure 1.  Crystal structure model of KBBF family.

    DownLoad: Full-Size Img PowerPoint

    图 2  从KBBF 到Pb2BO3I的倍频效应演进

    Figure 2.  Second harmonic generation evolution from KBBF to Pb2BO3I.

    DownLoad: Full-Size Img PowerPoint

    图 3  NH4Be2BO3F2 (ABBF)晶体结构模型[79,80]

    Figure 3.  Ball-and-stick representations of NH4Be2BO3F2(ABBF)[79,80].

    DownLoad: Full-Size Img PowerPoint

    图 4  AZn2BO3X2 (A = K, Rb, NH4)系列晶体结构模型[63−81]　(a) NH4Zn2BO3Cl2; (b) KZn2BO3Cl2; (c) RbZn2BO3Cl2

    Figure 4.  Ball-and-stick representations of AZn2BO3X2 (A = K, Rb, NH4) series[63−81]: (a) NH4Zn2BO3Cl2; (b) KZn2BO3Cl2; (c) RbZn2BO3Cl2.

    DownLoad: Full-Size Img PowerPoint

    图 5  KABO系列晶体结构模型[50−52]　(a) K2Al2B2O7; (b) $\beta$-Rb2Al2B2O7

    Figure 5.  Ball-and-stick representations of KABO series[50−52]: (a) K2Al2B2O7; (b) $\beta$-Rb2Al2B2O7.

    DownLoad: Full-Size Img PowerPoint

    图 6  Ba3Mg3(BO3)3F3晶体结构模型[87]　(a) Sr2Be2B2O7; (b) Ba3Mg3(BO3)3F3

    Figure 6.  Ball-and-stick representations of Ba3Mg3(BO3)3F3[87]: (a) Sr2Be2B2O7; (b) Ba3Mg3(BO3)3F3.

    DownLoad: Full-Size Img PowerPoint

    图 7  Sr2Be2B2O7和BaAl2B2O7晶体结构模型

    Figure 7.  Ball-and-stick representations of Sr2Be2B2O7 and BaAl2B2O7.

    DownLoad: Full-Size Img PowerPoint

    图 8  K3Sr3Li2Al4B6O20F和K3Ba3Li2Al4B6O20F (KBLABF)的晶体结构模型

    Figure 8.  Ball-and-stick representations of K3Sr3Li2Al4B6O20F and K3Ba3Li2Al4B6O20F (KBLABF).

    DownLoad: Full-Size Img PowerPoint

    图 9  氟化硼酸盐的活性基团平衡“倍频效应-透过范围-双折射率”的关系[68]

    Figure 9.  Relationship of active group balance of fluorooxoborates among bandgap, NLO coefficient and birefringence[68].

    DownLoad: Full-Size Img PowerPoint

    图 10  MB4O6F族氟化硼酸盐的晶体结构[92]

    Figure 10.  Crystal structures of the MB4O6F family[92].

    DownLoad: Full-Size Img PowerPoint

    图 11  层间由B—O共价键连接的系列硼酸盐晶体结构

    Figure 11.  Crystal structures of the series borates contain B—O covalent bond.

    DownLoad: Full-Size Img PowerPoint

    表 1  层间含有离子键和氢键连接的类KBBF结构硼酸盐深紫外NLO材料的结构和光学性能比较

    Table 1.  Cmparison of structural and optical properties of some deep-UV NLO materials of KBBF family with adjacent layers connected by ionic bond and hydrogen bond.

    化合物空间群结构层间连接紫外截止边/nmdeff (KDP)或dij/pm·V—1
    NaBe2BO3F2[20]C2[Be2BO3F2]∞Na+—F−155deff = 1.7 × deff (NH4H2PO4)
    KBe2BO3F2[20]R32[Be2BO3F2]∞K+—F−147d11 = 0.47 ± 0.01
    RbBe2BO3F2[21]R32[Be2BO3F2]∞Rb+—F−160d11 = 0.45 ± 0.01
    CsBe2BO3F2[22]R32[Be2 BO3F2]∞Cs+—F−151d11 = 0.5
    NH4Be2BO3F2[48]R32[Be2BO3F2]∞N—H·F1531.2
    $\gamma $-Be2BO3F[48]R32[Be2BO3F2]∞Be2+—F−144.82.3
    RbZn2BO3Cl2[63,81]R32[Zn2BO3Cl2]∞Rb+—Cl−1982.9
    KZn2BO3Cl2[63,81]R32[Zn2BO3Cl2]∞K+—Cl−1933.0
    NH4Zn2BO3Cl2[63]R32[Zn2BO3Cl2]∞N—H·Cl1862.8
    Be2(BO3)F[43]C2[Be2BO3F2]∞Be2+—F−150 a0.25
    BaBe2BO3F3[43]P63[Be2BO3F2]∞Ba2+—F−< 1850.1
    K2Al2B2O7[50,52]P321[Al3B3O6]∞Al3+—O2−180 0.45
    K2(1-x)Na2xAl2BO7[88](0 < x < 0.6)P321[Al3B3O6]∞Al3+—O2−180 0.45
    K2(1−x)Rb2xAl2B2O7[82] (0 < x < 0.75)P321[Al3B3O6]∞Al3+—O2−—0.7
    K0.67Rb1.33Al2B2O7[83]P321[Al3B3O6]∞Al3+—O2−1880.9
    $\beta$-Rb2Al2B2O7[51]P321[Al3B3O6]∞Al3+—O2−< 2002.0
    BaAlBO3F2[84]$ P{\overline 6}2c$[AlBO3F2]∞Ba2+—F−1652.0
    Rb3Al3B3O10F[54]P31c[Al3(BO3)OF]∞Al3+—F−Al3+—O2−< 2001.2
    BaZnBO3F[64]$ P{\overline 6}$[ZnBO3F]∞Zn2+—O2−—3 × deff
    Ba3Mg3(BO3)3F3[87]Pna21[Mg3O2F3(BO3)2]∞Ba2+—F−184d33 = 0.51
    注: 上标a为计算值.
    DownLoad: CSV

    表 2  SBBO型硼酸盐深紫外NLO材料的结构和光学性能比较

    Table 2.  Comparison of structural and optical properties of some deep-UV NLO materials of SBBO family.

    化合物空间群结构层间连接紫外截止边/nm倍频效应(KDP)或dij//pm·V−1
    Sr2Be2B2O7[39]$ P{\overline 6}c2$[Be2(BO3)2O]∞Sr2+—O2−1552.5
    Ba2Be2B2O7[40,73]$ P{\overline 6}2c$[Be2(BO3)2O]∞Ba2+—O2−2152.0
    BaAl2B2O7[52]R32[Al6B6O12]∞Al3+—O2−—d11 = 0.75
    NaCaBe2B2O6F[41]Cc[Be3B3O6F3]∞Ca2+—O2−1900.3
    K3Ba3Li2Al4B6O20F[55]$ P{\overline 6}2c$[Li2Al4B6O20F]∞Ba2+—O2−1901.5
    Rb3Ba3Li2Al4B6O20F[89]$ P{\overline 6}2c$[Li2Al4B6O20F]∞Ba2+—O2−1951.4
    K3Sr3Li2Al4B6O20F[57]R32[Li2Al4B6O20F]∞Sr2+—O2−1901.7 (0.9)
    Cs2Al2(B3O6)2O[90]P63[Al2(B3O6)2O]Al3+—O2−185d31 = 0.032
    DownLoad: CSV

    表 3  部分氟化硼酸盐深紫外NLO材料的结构和光学性能比较

    Table 3.  Comparison of structural and optical properties of some fluorooxoborates deep-UV NLO materials.

    化合物空间群结构层间连接方式紫外截止边/nm倍频效应(KDP)
    NH4B4O6F[69]Pna21[B4O6F]∞N—H·F1563.0
    CsB4O6F[71]Pna21[B4O6F]∞Cs+—F−1551.9
    RbB4O6F[70]Pna21[B4O6F]∞Rb+—F−< 1900.8
    CsKB8O12F2[70]P321[B4O6F]∞Cs/K+—F−< 1901.9
    CsRbB8O12F2[70]$ P{\overline 6}2c$[B4O6F]∞Cs/K+—F−< 1901.1
    NaB4O6F[72]C2[B4O6F]∞Na+—F−< 1800.9
    SrB5O7F3[98]Cmc21[B5O7F3]∞Sr2+—F−< 1801.6
    Sr2B10O14F6[99]< 2002.5
    CaB5O7F3[97]Cmc21[B5O7F3]∞Ca2+—F−< 1802.0
    Ca2B10O14F6[99]< 2002.3
    DownLoad: CSV

    表 4  层间含有B—O共价键连接的类KBBF结构硼酸盐深紫外NLO材料的结构和光学性能比较

    Table 4.  Comparison of structural and optical properties of some deep-UV NLO materials of KBBF family with adjacent layers connected by rigid B—O groups.

    化合物空间群结构层间连接方式紫外截止边/nm倍频效应(KDP)
    $ \beta $-KBe2B3O7[44]Pmn21[Be2BO5]∞ [BO2]∞< 2000.75
    $\gamma $-KBe2B3O7[44]P21[Be2BO5]∞ [B3O6]< 2000.68
    RbBe2B3O7[44]Pmn21[Be2BO5]∞ [BO2]∞< 2000.79
    Na2CsBe6B5O15[45]C2[Be2BO5]∞ [BO3]< 2001.17
    Na2Be4B4O11[46]P1[Be2BO5]∞[B2O5]1711.30
    LiNa5Be12B12O23[46]Pc[Be2BO5]∞ [B2O5]1691.40
    Li4Sr(BO3)2[67]Cc[SrBO3]∞[B2O3]1862.00
    DownLoad: CSV
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  • Received Date:  06 December 2018
  • Accepted Date:  25 December 2018
  • Available Online:  01 January 2019
  • Published Online:  20 January 2019

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