基于局域表面等离激元共振的分子取向和分子光致异构效率调控
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摘要
纳米光子学研究纳米材料与物质的相互作用,是一门新兴学科。在纳米光子学中,金属纳米材料是最受研究关注的材料,利用金属纳米材料表面等离激元共振效应突破传统光学衍射极限,可以实现微电子与光子在同一芯片上的集成。此外,金属纳米材料表面等离激元共振效应可以增强荧光分子辐射效率,控制纳米颗粒取向和转动,是改变物质物理光学性质的理想选择。本博士论文围绕金纳米颗粒局域表面等离激元共振效应对偶氮分子光致异构量子效率的影响和对定向液晶盒中液晶分子光致取向增强效应进行了深入地探讨和研究。取得的成果包括：
1.首次测量得到偶氮分子顺式异构体(cis)的二阶光学超极化率数值,将cis分子对偶氮薄膜光学非线性系数的贡献考虑在内,完善了光泵浦下偶氮染料三阶光学非线性系数的理论模型。实验上测量了偶氮薄膜三次谐波信号与泵浦光强的关系,利用推导的理论模型对实验数据进行拟合,最终推出cis分子的二阶光学超极化率数值为5.6×10-33esu。
2.利用金纳米颗粒表面等离激元共振效应带来的局域场增强和能量转移成功调控偶氮染料分子的光致异构量子效率。可将该量子效率增大一倍,或显著降低。通过表面增强拉曼散射和荧光淬灭实验,证实了量子效率的提高或降低取决于金纳米颗粒局域场增强效应和能量共振转移作用的竞争。通过在金纳米颗粒薄膜和偶氮染料分子薄膜之间加入不同厚度的隔离层,实现量子效率的精确调控。
3.发现经金纳米颗粒修饰的液晶盒定向层受到与局域等离激元共振的激光辐照时,会有效降低液晶的锚定能。利用这一新的效应,观察到对应液晶分子转动的光学Freedericksz相变阈值下降1-2个量级。该效应也使液晶分子响应的动力学过程发生改变,缩短了液晶盒的光响应时间。
Nanophotonics is a new branch of science which studies the interaction between matter and nanomaterials. Among kinds of nanomaterials, metal nanomaterials are research concern. Surface plasmon resonance (SPR) of metal materials can break the diffraction limit of conventional optics, leading to the integration of light and electron on the same chip. Meantime, SPR is able to enhance the radiation efficiency of fluorescence molecules and control the rotation and orientation of nanoparticles, making metal nanomaterials a good choice to change the physical-optical properties of matter. This Ph.D thesis focuses on the research topic "Controlling photoisomerization quantum efficiency (PQE) of azobenzene dye and enhancing optical-induced reorientation of liquid crystals (LC) by localized surface plasmon resonance (LSPR) of gold nanoparticle film". The influence of LSPR to PQE of azobenzene dye and optical nonlinear property of LC has been investigated. The main achievements are as follow:
1. for first time we obtain the second order hyperpolarizability of cis isomer. Contribution of cis isomer to third-order nonlinear susceptibility of azobenzene film is brought in and the theory of optically induced anisotropy of third-order nonlinear susceptibility in azobenzene dye polymers is supplemented. Experimentally optical third harmonic generation (THG) of azobenzene dye polymer under various intensity of linearly polarized optical beam was recorded. Then experimental data was fitted by theory and finally the second order hyperpolarizability of cis isomer is deduced to be5.6×10-33esu.
2. trans-to-cis photoisomerization quantum efficiency (PQE) of azobenzene dye is artificially modified by surface plasmon resonance (SPR) induced local field enhancement and energy transfer of Au nanoparticles film. PQE can either increase one time larger or decrease dramatically. Using surface enhanced raman scattering and fluorescence quenching experiments, it is found that SPR of Au nanoparticles film enhances PQE and energy transfer lows it. PQE is further accurately modified by controlling the distance between azobenzene dye and Au nanoparticles film.
3. surface anchoring energy of Au nanoparticles coated liquid crystal cell can be effectively decreased when pumped by resonant optical beam. As a result, the threshold of optical Freedericksz phase transition is lowed by one to two orders of magnitude. Meanwhile, the response time of LC to optical pump is also shortened.
1.首次测量得到偶氮分子顺式异构体(cis)的二阶光学超极化率数值,将cis分子对偶氮薄膜光学非线性系数的贡献考虑在内,完善了光泵浦下偶氮染料三阶光学非线性系数的理论模型。实验上测量了偶氮薄膜三次谐波信号与泵浦光强的关系,利用推导的理论模型对实验数据进行拟合,最终推出cis分子的二阶光学超极化率数值为5.6×10-33esu。
2.利用金纳米颗粒表面等离激元共振效应带来的局域场增强和能量转移成功调控偶氮染料分子的光致异构量子效率。可将该量子效率增大一倍,或显著降低。通过表面增强拉曼散射和荧光淬灭实验,证实了量子效率的提高或降低取决于金纳米颗粒局域场增强效应和能量共振转移作用的竞争。通过在金纳米颗粒薄膜和偶氮染料分子薄膜之间加入不同厚度的隔离层,实现量子效率的精确调控。
3.发现经金纳米颗粒修饰的液晶盒定向层受到与局域等离激元共振的激光辐照时,会有效降低液晶的锚定能。利用这一新的效应,观察到对应液晶分子转动的光学Freedericksz相变阈值下降1-2个量级。该效应也使液晶分子响应的动力学过程发生改变,缩短了液晶盒的光响应时间。
Nanophotonics is a new branch of science which studies the interaction between matter and nanomaterials. Among kinds of nanomaterials, metal nanomaterials are research concern. Surface plasmon resonance (SPR) of metal materials can break the diffraction limit of conventional optics, leading to the integration of light and electron on the same chip. Meantime, SPR is able to enhance the radiation efficiency of fluorescence molecules and control the rotation and orientation of nanoparticles, making metal nanomaterials a good choice to change the physical-optical properties of matter. This Ph.D thesis focuses on the research topic "Controlling photoisomerization quantum efficiency (PQE) of azobenzene dye and enhancing optical-induced reorientation of liquid crystals (LC) by localized surface plasmon resonance (LSPR) of gold nanoparticle film". The influence of LSPR to PQE of azobenzene dye and optical nonlinear property of LC has been investigated. The main achievements are as follow:
1. for first time we obtain the second order hyperpolarizability of cis isomer. Contribution of cis isomer to third-order nonlinear susceptibility of azobenzene film is brought in and the theory of optically induced anisotropy of third-order nonlinear susceptibility in azobenzene dye polymers is supplemented. Experimentally optical third harmonic generation (THG) of azobenzene dye polymer under various intensity of linearly polarized optical beam was recorded. Then experimental data was fitted by theory and finally the second order hyperpolarizability of cis isomer is deduced to be5.6×10-33esu.
2. trans-to-cis photoisomerization quantum efficiency (PQE) of azobenzene dye is artificially modified by surface plasmon resonance (SPR) induced local field enhancement and energy transfer of Au nanoparticles film. PQE can either increase one time larger or decrease dramatically. Using surface enhanced raman scattering and fluorescence quenching experiments, it is found that SPR of Au nanoparticles film enhances PQE and energy transfer lows it. PQE is further accurately modified by controlling the distance between azobenzene dye and Au nanoparticles film.
3. surface anchoring energy of Au nanoparticles coated liquid crystal cell can be effectively decreased when pumped by resonant optical beam. As a result, the threshold of optical Freedericksz phase transition is lowed by one to two orders of magnitude. Meanwhile, the response time of LC to optical pump is also shortened.
引文
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