Wide Spectral Range Nonlinear Optical Crystals of One-Dimensional Coordination Solids [Et4N][Cd(SCN)3] and [Et4N][Cd(SeCN)3] and the General Design Criteria for [R4N][Cd(XCN)3] (Where R = Alkyl and X = S, Se, Te) as NLO Crystals
We report herein two new nonlinear optical (NLO) crystals, [Et4N][Cd(XCN)3], where X = S (1) and Se (2), that are transparent from 220 to 3300 nm, covering the entire near-ultraviolet, the visible, and the near-infrared spectral regions and giving rise to a very wide and continuous optical window, w...
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| Published in: | Inorganic chemistry Vol. 39; no. 9; pp. 1868 - 1873 |
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| Main Authors: | , , , |
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| Language: | English |
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01-05-2000
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| Abstract | We report herein two new nonlinear optical (NLO) crystals, [Et4N][Cd(XCN)3], where X = S (1) and Se (2), that are transparent from 220 to 3300 nm, covering the entire near-ultraviolet, the visible, and the near-infrared spectral regions and giving rise to a very wide and continuous optical window, which is useful for many frequency conversion applications. Both 1 and 2 exhibit highly efficient second harmonic generation (SHG) as measured via the Kurtz−Perry method. The corresponding [Me4N]+ salts, [Me4N][Cd(XCN)3 where X = S (3) and Se (4), show no SHG effects. All four structures adopt noncentrosymmetric space groups (Cmc21 for 1 and 2 and Pna21 for 3 and presumably 4) and are based on one-dimensional anionic [Cd(XCN)3 -]∞ zigzag chains. However, a detailed analysis of the structures of [R4N][Cd(XCN)3], where R = Et, Me, and X = S, Se revealed that the difference in the second-order nonlinear responses of the Et4N+ salts (1 and 2) and the Me4N+ salts (3 and 4) is attributable to the relative alignment of the [Cd(XCN)3 -]∞ zigzag chains, being parallel in the crystals of 1 and 2 but antiparallel in the crystals of 3 and 4. Also reported, for the first time, are the synthesis and crystal structure of [Et4N][Cd(SeCN)3] (2). Compound 2 crystallizes in an orthorhombic unit cell of Cmc21 space group symmetry with lattice parameters of 9.938(1) Å, 16.868(2) Å, 11.054(1) Å, and Z = 4. Other issues related to the molecular and crystal engineering of this class of NLO materials are also discussed. |
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| AbstractList | We report herein two new nonlinear optical (NLO) crystals, [Et4N][Cd(XCN)3], where X = S (1) and Se (2), that are transparent from 220 to 3300 nm, covering the entire near-ultraviolet, the visible, and the near-infrared spectral regions and giving rise to a very wide and continuous optical window, which is useful for many frequency conversion applications. Both 1 and 2 exhibit highly efficient second harmonic generation (SHG) as measured via the Kurtz−Perry method. The corresponding [Me4N]+ salts, [Me4N][Cd(XCN)3 where X = S (3) and Se (4), show no SHG effects. All four structures adopt noncentrosymmetric space groups (Cmc21 for 1 and 2 and Pna21 for 3 and presumably 4) and are based on one-dimensional anionic [Cd(XCN)3 -]∞ zigzag chains. However, a detailed analysis of the structures of [R4N][Cd(XCN)3], where R = Et, Me, and X = S, Se revealed that the difference in the second-order nonlinear responses of the Et4N+ salts (1 and 2) and the Me4N+ salts (3 and 4) is attributable to the relative alignment of the [Cd(XCN)3 -]∞ zigzag chains, being parallel in the crystals of 1 and 2 but antiparallel in the crystals of 3 and 4. Also reported, for the first time, are the synthesis and crystal structure of [Et4N][Cd(SeCN)3] (2). Compound 2 crystallizes in an orthorhombic unit cell of Cmc21 space group symmetry with lattice parameters of 9.938(1) Å, 16.868(2) Å, 11.054(1) Å, and Z = 4. Other issues related to the molecular and crystal engineering of this class of NLO materials are also discussed. We report herein two new nonlinear optical (NLO) crystals, [Et4N][Cd(XCN)3], where X = S (1) and Se (2), that are transparent from 220 to 3300 nm, covering the entire near-ultraviolet, the visible, and the near-infrared spectral regions and giving rise to a very wide and continuous optical window, which is useful for many frequency conversion applications. Both 1 and 2 exhibit highly efficient second harmonic generation (SHG) as measured via the Kurtz-Perry method. The corresponding [Me4N]+ salts, [Me4N][Cd(XCN)3 where X = S (3) and Se (4), show no SHG effects. All four structures adopt noncentrosymmetric space groups (Cmc2(1) for 1 and 2 and Pna2(1) for 3 and presumably 4) and are based on one-dimensional anionic [Cd(XCN)3-] infinity zigzag chains. However, a detailed analysis of the structures of [R4N][Cd(XCN)3], where R = Et, Me and X = S, Se revealed that the difference in the second-order nonlinear responses of the Et4N+ salts (1 and 2) and the Me4N+ salts (3 and 4) is attributable to the relative alignment of the [Cd(XCN)3-] infinity zigzag chains, being parallel in the crystals of 1 and 2 but antiparallel in the crystals of 3 and 4. Also reported, for the first time, are the synthesis and crystal structure of [Et4N][Cd(SeCN)3] (2). Compound 2 crystallizes in an orthorhombic unit cell of Cmc21 space group symmetry with lattice parameters of 9.938(1) A, 16.868(2) A, 11.054(1) A, and Z = 4. Other issues related to the molecular and crystal engineering of this class of NLO materials are also discussed. |
| Author | Zhang, Hong Price, Gary E Teo, Boon K Zelmon, David E |
| Author_xml | – sequence: 1 givenname: Hong surname: Zhang fullname: Zhang, Hong – sequence: 2 givenname: David E surname: Zelmon fullname: Zelmon, David E – sequence: 3 givenname: Gary E surname: Price fullname: Price, Gary E – sequence: 4 givenname: Boon K surname: Teo fullname: Teo, Boon K |
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| Cites_doi | 10.1107/S056774087400793X 10.1364/JOSAB.15.000751 10.1016/S0010-8545(00)80113-7 10.1021/ja9605230 10.1039/p29720000345 10.1246/bcsj.60.179 10.1039/a703434b 10.1021/ja970264u 10.1063/1.1656857 10.1126/science.247.4943.669 10.1016/S0010-8545(00)80114-9 10.1021/ja972830r 10.1039/cs9790800085 10.1021/ic971487o 10.1007/978-3-662-13830-4 10.1021/ja00052a035 10.1246/bcsj.62.424 10.1016/0022-0248(95)00983-3 10.1021/ar50121a002 10.1002/zaac.19804640124 10.1088/0963-9659/5/5/020 10.1021/ja00034a024 10.1021/ic980387v 10.1021/ja952836l 10.1038/42190 10.1021/ja00986a052 10.1364/JOSAB.9.000534 10.1021/ic00091a017 10.1002/anie.199611541 10.1016/S1350-4495(97)00017-0 10.1021/ar50122a001 10.1002/hlca.19640470728 10.1107/S0567740874007965 10.1039/dt9750002374 10.1016/S0065-2792(08)60202-2 10.1063/1.364706 10.1016/S0010-8545(98)00270-7 |
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| Snippet | We report herein two new nonlinear optical (NLO) crystals, [Et4N][Cd(XCN)3], where X = S (1) and Se (2), that are transparent from 220 to 3300 nm, covering the... |
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| Title | Wide Spectral Range Nonlinear Optical Crystals of One-Dimensional Coordination Solids [Et4N][Cd(SCN)3] and [Et4N][Cd(SeCN)3] and the General Design Criteria for [R4N][Cd(XCN)3] (Where R = Alkyl and X = S, Se, Te) as NLO Crystals |
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