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Cs3[(BOP)2(B3O7)3]: A Deep-Ultraviolet Nonlinear Optical Crystal Designed by Optimizing Matching of Cation and Anion Groups
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-05-26 , DOI: 10.1021/jacs.3c02400 Haonan Liu 1 , Hongping Wu 1 , Zhanggui Hu 1 , Jiyang Wang 1 , Yicheng Wu 1 , Hongwei Yu 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-05-26 , DOI: 10.1021/jacs.3c02400 Haonan Liu 1 , Hongping Wu 1 , Zhanggui Hu 1 , Jiyang Wang 1 , Yicheng Wu 1 , Hongwei Yu 1
Affiliation
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Deep-ultraviolet nonlinear optical (DUV NLO) crystals are indispensable for solid-state lasers to produce coherent light with wavelengths shorter than 200 nm, yet their structure design still faces great challenges because two groups of conflicting properties must be satisfied simultaneously, i.e., “large second harmonic generation (SHG) response-large band gap” and “large birefringence-weak growth anisotropy”. Clearly, hitherto, no crystal can perfectly satisfy these properties, including KBe2BO3F2. Herein, we design a new mixed-coordinated borophosphate Cs3[(BOP)2(B3O7)3] (CBPO) by optimizing the matching of cation and anion groups, which unprecedentedly achieves a balance for two groups of contradictions concurrently for the first time. In the structure of CBPO, it has the coplanar and π-conjugated B3O7 groups, which can make it possess a large SHG response (3 × KDP) and large birefringence (0.075@532 nm). Then, terminal O atoms of these B3O7 groups are connected by BO4 and PO4 tetrahedra, which eliminates all dangling bonds and blue shifts the UV absorption edge to the DUV region (165 nm). More importantly, owing to the judicious selection of cations, the size of cations and void of anion groups is a perfect match, which makes CBPO possess a very stable three-dimensional anion framework and thus reduces the crystal growth anisotropy. A CBPO single crystal with a size of up to 20 × 17 × 8 mm3 has been successfully grown, through which a DUV coherent light has also been achieved in Be-free DUV NLO crystals for the first time. These indicate CBPO will be the next generation of DUV NLO crystals.
中文翻译：
Cs3[(BOP)2(B3O7)3]：阳离子和阴离子基团优化匹配设计的深紫外非线性光学晶体
深紫外非线性光学（DUV NLO）晶体对于固态激光器产生波长小于 200 nm 的相干光是不可或缺的，但其结构设计仍然面临巨大挑战，因为必须同时满足两组相互矛盾的特性，即，“大二次谐波产生（SHG）响应-大带隙”和“大双折射-弱生长各向异性”。显然，迄今为止，没有任何晶体能够完美地满足这些特性，包括 KBe 2 BO 3 F 2。在此，我们设计了一种新的混合配位硼磷酸盐 Cs 3 [(BOP) 2 (B 3 O 7 ) 3] (CBPO)通过优化阳离子和阴离子基团的匹配，史无前例地首次同时实现两组矛盾的平衡。CBPO结构中具有共面的π共轭B 3 O 7基团，使其具有较大的SHG响应（3×KDP）和较大的双折射（0.075@532 nm）。然后，这些B 3 O 7基团的末端O原子通过BO 4和PO 4连接四面体，它消除了所有悬空键，并且蓝移了 UV 吸收边缘到 DUV 区域（165 nm）。更重要的是，由于阳离子的选择合理，阳离子的大小与阴离子基团的空隙完美匹配，使得CBPO具有非常稳定的三维阴离子骨架，从而降低了晶体生长的各向异性。成功生长了尺寸高达20×17×8 mm 3的CBPO单晶，并首次在Be-free DUV NLO晶体中实现了DUV相干光。这些表明 CBPO 将成为下一代 DUV NLO 晶体。
更新日期：2023-05-26
中文翻译：
Cs3[(BOP)2(B3O7)3]：阳离子和阴离子基团优化匹配设计的深紫外非线性光学晶体
深紫外非线性光学（DUV NLO）晶体对于固态激光器产生波长小于 200 nm 的相干光是不可或缺的，但其结构设计仍然面临巨大挑战，因为必须同时满足两组相互矛盾的特性，即，“大二次谐波产生（SHG）响应-大带隙”和“大双折射-弱生长各向异性”。显然，迄今为止，没有任何晶体能够完美地满足这些特性，包括 KBe 2 BO 3 F 2。在此，我们设计了一种新的混合配位硼磷酸盐 Cs 3 [(BOP) 2 (B 3 O 7 ) 3] (CBPO)通过优化阳离子和阴离子基团的匹配，史无前例地首次同时实现两组矛盾的平衡。CBPO结构中具有共面的π共轭B 3 O 7基团，使其具有较大的SHG响应（3×KDP）和较大的双折射（0.075@532 nm）。然后，这些B 3 O 7基团的末端O原子通过BO 4和PO 4连接四面体，它消除了所有悬空键，并且蓝移了 UV 吸收边缘到 DUV 区域（165 nm）。更重要的是，由于阳离子的选择合理，阳离子的大小与阴离子基团的空隙完美匹配，使得CBPO具有非常稳定的三维阴离子骨架，从而降低了晶体生长的各向异性。成功生长了尺寸高达20×17×8 mm 3的CBPO单晶，并首次在Be-free DUV NLO晶体中实现了DUV相干光。这些表明 CBPO 将成为下一代 DUV NLO 晶体。
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