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类KBe2BO3F2结构硼酸盐深紫外非线性光学材料的研究进展

盖敏强 王颖 潘世烈

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类KBe2BO3F2结构硼酸盐深紫外非线性光学材料的研究进展

盖敏强, 王颖, 潘世烈

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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  • 利用非线性光学(NLO)晶体材料和变频技术, 可以把波长范围有限的激光光源扩展到紫外、深紫外区, 这已成为深紫外光源的热点研究方向. 然而, 目前限制深紫外全固态激光器发展和应用的关键问题是缺乏能够在该波段进行频率转换并且产业化应用的NLO晶体材料. 因此, 该领域的各国科学家都在积极探索并发展新一代的深紫外NLO晶体材料. 目前仅有KBe2BO3F2 (KBBF)晶体能够实现Nd:YAG的直接六倍频深紫外激光(波长为177.3 nm)输出. 然而, KBBF晶体存在严重的层状生长习性, 并且其原料氧化铍有剧毒, 从而极大地制约了其商业化生产和应用进程. 根据阴离子基团理论, 以BO3基团为基本结构单元形成的类[Be2BO3F]层状结构特征仍然是目前最有利于产生深紫外谐波的适宜结构之一, 因此, 基于KBBF层状结构进行分子工程设计, 并开发类KBBF结构的硼酸盐可能是探索新材料的优选策略. 本文通过回顾类KBBF结构硼酸盐深紫外NLO晶体的发展历程, 系统梳理该类晶体材料层状结构特点、不同层间连接方式和光学性能, 分析限制深紫外NLO晶体发展的主要因素, 讨论目前发展类KBBF结构硼酸盐深紫外NLO晶体材料的主要矛盾和解决策略, 以期对未来新材料的创新探索提供借鉴.
    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.
      通信作者: 潘世烈, slpan@ms.xjb.ac.cn
    • 基金项目: 国家自然科学基金(批准号: 51602341, 51425206, 91622107)资助的课题.
      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

    Fig. 1.  Crystal structure model of KBBF family.

    图 2  从KBBF 到Pb2BO3I的倍频效应演进

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

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

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

    图 4  AZn2BO3X2 (A = K, Rb, NH4)系列晶体结构模型[6381] (a) NH4Zn2BO3Cl2; (b) KZn2BO3Cl2; (c) RbZn2BO3Cl2

    Fig. 4.  Ball-and-stick representations of AZn2BO3X2 (A = K, Rb, NH4) series[6381]: (a) NH4Zn2BO3Cl2; (b) KZn2BO3Cl2; (c) RbZn2BO3Cl2.

    图 5  KABO系列晶体结构模型[5052] (a) K2Al2B2O7; (b) $\beta$-Rb2Al2B2O7

    Fig. 5.  Ball-and-stick representations of KABO series[5052]: (a) K2Al2B2O7; (b) $\beta$-Rb2Al2B2O7.

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

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

    图 7  Sr2Be2B2O7和BaAl2B2O7晶体结构模型

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

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

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

    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]

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

    图 10  MB4O6F族氟化硼酸盐的晶体结构[92]

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

    图 11  层间由B—O共价键连接的系列硼酸盐晶体结构

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

    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+—F155deff = 1.7 × deff (NH4H2PO4)
    KBe2BO3F2[20]R32[Be2BO3F2]K+—F147d11 = 0.47 ± 0.01
    RbBe2BO3F2[21]R32[Be2BO3F2]Rb+—F160d11 = 0.45 ± 0.01
    CsBe2BO3F2[22]R32[Be2 BO3F2]Cs+—F151d11 = 0.5
    NH4Be2BO3F2[48]R32[Be2BO3F2]N—H·F1531.2
    $\gamma $-Be2BO3F[48]R32[Be2BO3F2]Be2+—F144.82.3
    RbZn2BO3Cl2[63,81]R32[Zn2BO3Cl2]Rb+—Cl1982.9
    KZn2BO3Cl2[63,81]R32[Zn2BO3Cl2]K+—Cl1933.0
    NH4Zn2BO3Cl2[63]R32[Zn2BO3Cl2]N—H·Cl1862.8
    Be2(BO3)F[43]C2[Be2BO3F2]Be2+—F150 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$[AlBO3F2]Ba2+—F1652.0
    Rb3Al3B3O10F[54]P31c[Al3(BO3)OF]Al3+—FAl3+—O2−< 2001.2
    BaZnBO3F[64]$ P{\overline 6}$[ZnBO3F]Zn2+—O2−3 × deff
    Ba3Mg3(BO3)3F3[87]Pna21[Mg3O2F3(BO3)2]Ba2+—F184d33 = 0.51
    注: 上标a为计算值.
    下载: 导出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
    下载: 导出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+—F1551.9
    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
    下载: 导出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
    下载: 导出CSV
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    [20] 陈创天. 晶体电光和非线性光学效应的离子基团理论(Ⅰ)——利用氧八面体畸变模型计算BaTiO3晶体电光及倍频系数. 物理学报, 1976, 25(2): 146-161. doi: 10.7498/aps.25.146
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出版历程
  • 收稿日期:  2018-12-06
  • 修回日期:  2018-12-25
  • 上网日期:  2019-01-01
  • 刊出日期:  2019-01-20

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