Advances in organic nonlinear crystals and ultra-wideband terahertz radiation sources
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摘要:非线性光学晶体是非线性光学频率变换技术中的核心器件。近些年，为进一步提高基于非线性光学频率变换技术产生太赫兹波的输出能量、转换效率，拓宽产生太赫兹波的带宽，多种新型有机晶体得以发展，并凭借其更加出色的非线性光学性质，成为产生太赫兹波的理想材料。本文按照晶体类型介绍了目前可产生THz波的多种有机晶体的性质，并总结了基于多种有机晶体的超宽带太赫兹辐射源的国内外研究进展，同时结合THz光谱检测技术的应用需求分析了基于有机晶体宽带THz辐射源的发展趋势以及所面临的关键科学问题。Abstract:Nonlinear optical(NLO) crystals are the determinant in nonlinear optics. Recently, a variety of new organic crystals have been developed to further improve the output energy and conversion efficiency and to broaden the bandwidth of THz waves based on nonlinear optical frequency conversion technology. These crystals have become an ideal material for generating THz waves with their excellent performance in nonlinear optics. In this paper, the properties of different organic crystals are introduced in the classification of ionic crystals and nonionic molecular crystals, and the progress of THz sources that use the different organic crystals are summarized. At the same time, the applications and the trends in the development of broadband THz radiation using organic crystals are analyzed.
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Key words:
- terahertz/
- organic crystal/
- ultra-wideband/
- nonlinear frequency conversion
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图 6(a) Cherenkov相位匹配示意图[57]；(b)Si棱镜耦合Cherenkov相位匹配中DAST晶体示意图[57]；(c)基于Cherenkov相位匹配的DAST晶体THz辐射源[58]；(d)Cherenkov相位匹配与传统共线相位匹配的输出谱[58]
Figure 6.(a)Diagram of Cherenkov phase matching[57]; (b)diagram of DAST crystal in Si prism-coupled Cherenkov phase matching[57]; (c)experimental set-up of THz source based on DAST crystal under Cherenkov phase matching condition[58]; (d)output spectra of Cherenkov phase matching and traditional collinearity phase matching[58]
图 7(a) 基于双波长可调谐连续光纤 器泵浦DAST晶体产生THz波实验系统[61]；(b)基于Nd:YAG双波长 器泵浦DAST晶体产生THz波实验系统[62]；(c)基于非共线相位匹配BBO-OPO泵浦DAST晶体产生THz波实验系统[64]
Figure 7.(a)Experimental set-up of THz waves generated from DAST pumped by tunable continuous fiber lasers[61]; (b)experimental set-up of THz waves generated from DAST pumped by dual-wavelength Nd:YAG laser; (c)experimental set-up of THz waves generated from DAST crystal pumped by BBO-OPO under non-collinear phase matching condition[64]
图 9(a) DSTMS晶体红外波段色散特性[70]；(b)DSTMS晶体红外吸收特性[70]；(c)DSTMS晶体a轴在THz波段色散和吸收特性[71]；(d)DAST与DSTMS晶体光整流产生THz波最佳长度计算[71]
Figure 9.(a)Infrared dispersion characteristics of DSTMS crystals[70]; (b)infrared absorption characteristics of DSTMS crystals[70]; (c)dispersion and absorption characteristics of thea-axis of the DSTMS crystal in the THz band[71]; (d)comparison of maximum effective length of THz waves generated by DAST and DSTMS crystal in THz genenration based on optical rectification[71]
图 10(a) PCS-DSTMS晶体实物图[73]；(b)基于PCS-DSTMS晶体产生THz波的能量分布[73]；(c)基于DSTMS晶体差频输出超宽带可调谐THz波[74]
Figure 10.(a)Physical map of PCS-DSTMS crystals[73]; (b)energy distribution of THz waves based on PCS-DSTMS crystals[73]; (c)ultra-wideband tunable THz waves based on DSTMS crystals different frequency technology[74]
图 13(a) 光整流效应激发BNA晶体产生THz波中剩余泵浦频移现象；(b)THz能量与泵浦脉宽之间的关系；(c)THz转换效率与泵浦中心波长之间的关系[86]
Figure 13.(a)Residual pump frequency shift in the THz waves generated by the BNA crystals excited by optics rectification technology; (b)relationship between the THz energy and the pump pulse width; (c)relationship between the THz conversion efficiency and pump center wavelength[86]
表 1离子型晶体DAST、DSTMS、HMQ-T、HMQ-TMS、HMB-TMS的性质[24,28,34-36]
Table 1.Properties of ionic crystals DAST, DSTMS, HMQ-T, HMQ-TMS, HMB-TMS
吡啶盐体系 喹啉体系 苯并噻唑体系 晶体 DAST DSTMS HMQ-T HMQ-TMS HMB-TMS 化学式 C23H26N2O3S C25H30N2O3S C26H25NO5S C28H29NO5S C25H27NO5S2 晶系 单斜 单斜 单斜 单斜 单斜 空间群 Cc Cc Pn Pn Pn 点群 m m m m m 熔点(℃) 256 258 273 257 257 水溶性 溶 溶 不溶 不溶 不溶 
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晶体 OH1 BNA 化学式 C19H18N2O C14H14N2O2 晶系 正交 正交(亚稳态) 单斜(稳定态) 空间群 Pna21 Pna21(C2V9) P21/c(C2h5) a(Å) 15.441 3 7.327 3 16.457 b(Å) 10.998 8 21.386 7.131 9 c(Å) 9.569 9 8.084 5 20.992 Z 4 4 8 熔点(℃) 212 106 NLO系数 d33=285 pm/V@1 300 nm d33=234 pm/V@1 064 nm 下载:
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表 3基于洛伦兹模型拟合DAST晶体色散方程的相关参数[56]
Table 3.Fit parameters of DAST dispersion function by Lorentz osciliator model[56]
DAST晶体a轴εEL=5.48 Ω/2π εSTj γj 1.1 0.79 0.39 3.1 0.15 4.2 5.2 0.03 1.9 7.1 0.16 11 8.4 0.02 0.85 11 0.002 1.3 12.3 0.01 2.1 DAST晶体b轴εEL=2.81 Ω/2π εSTj γj 1.1 0.27 0.31 1.3 0.43 0.84 1.6 0.10 0.20 2.2 0.05 1.3 3 0.12 1.6 5.2 0.03 1.1 7.2 0.02 3.4 9.6 0.02 1.7 11.7 0.004 5.2 下载:
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表 4基于洛伦兹模型拟合OH1晶体色散、吸收方程参数[42]
Table 4.Fitting parameters of OH1 dispersion and absorption function based on Lorentz oscillator model[42]
OH1晶体b轴 j ωj/2π fj γj 1 0.368 0.027 0.18 2 0.595 0.020 0.26 3 1.467 0.0175 0.97 4 2.85 0.23 3.06 OH1晶体c轴 j ωj/2π fj γj 1 0.820 0.015 0.34 2 1.772 0.146 1.84 3 2.64 0.127 1.8 下载:
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