微纳光纤—金纳米棒复合结构：微纳尺度“光子—表面等离激元”研究新平台
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摘要
得益于其独特的局域表面等离激元共振(1ocalized surface plasmon resonance, LSPR)特性,金属纳米颗粒在生物化学传感、表面增强拉曼光谱、生物医学和纳米光子学等领域有着广泛的应用前景。到目前为止,金属纳米颗粒LSPR的激发一般采用自由空间光束直接照射方式。一方面,由于单个金属纳米颗粒消光截面很小而照射光斑面积相对较大,激发效率受到很大限制(一般小于1%)；另一方面,这种激发方式往往需要利用大体积的光学元件(如物镜或棱镜等)来转折光路。这些均使得研制基于金属纳米颗粒的小型化和低功耗的光子器件变得相对困难。此外,在金属纳米颗粒中,金属材料的本征吸收和纳米颗粒的散射损耗一般比较大,导致其LSPR线宽相对较宽,严重限制了金属纳米颗粒在很多领域如高灵敏度生物化学传感或表面增强拉曼光谱中的应用。因此,如何提高金属纳米颗粒LSPR的激发效率和集成度,以及如何降低金属纳米颗粒LSPR的线宽,是目前金属纳米颗粒LSPR研究领域所面临的关键问题。基于上述考虑,我们提出了使用金属纳米颗粒和微纳光纤组成的复合结构(金纳米棒掺杂的聚合物纳米光纤和表面沉积金纳米棒的微光纤)来提高金属纳米颗粒LSPR激发效率和降低金属纳米颗粒LSPR线宽的方案,成功地将其应用于光学传感,并演示了金纳米棒LSPR峰的动态调控。
在本论文的第一章,我们综述了微纳光波导和金属纳米颗粒LSPR的研究背景以及典型的金属纳米颗粒-微纳光波导复合结构的研究进展。
在本论文的第二章,我们主要介绍了微纳光纤的基本光学特性。首先,我们简单介绍了氧化硅和聚合物微纳光纤的制备方法。其次,通过计算机数值模拟,我们分析了微纳光纤的光学传输特性,结果表明微纳光纤具有强的光场束缚能力和大比例倏逝场,同时我们还介绍了微纳光纤的光学输入输出方法。接着,我们介绍了微纳光纤常用的功能化方法,包括表面修饰、掺杂和电子束活化等。最后,我们演示了将微纳光纤组装成各种复杂结构的微纳操作技术。上述研究为我们后续的微纳光纤-金纳米棒复合结构研究准备了理论和技术基础。
在本论文的第三章,我们研究了纳米光纤导波高效激发金纳米棒的LSPR。首先,我们将金纳米棒掺杂进聚丙烯酰胺(polyacrylamide, PAM)溶液并制备聚合物纳米光纤,实现了金纳米棒在PAM纳米光纤中的高度有序排列。其次,我们通过倏逝波耦合方式将激发光耦合进聚合物纳米光纤,首次利用纳米光纤中的导波模式实现了掺杂金纳米棒LSPR的激发。实验测得,在纵向表面等离激元共振峰处,单个金纳米棒中的光子-激元转换效率高达70%。这一高效且紧凑的激发方式为发展小型化和低功耗的基于金属纳米颗粒的微纳光子器件提供了新的思路。
作为上述金纳米棒-聚合物纳米光纤复合结构的应用之一,我们演示了基于纳米光纤导波激发的金纳米棒的光学相对湿度(relative humidity, RH)传感。我们通过监测掺杂的单个金纳米棒LSPR峰的移动来实现湿度传感,获得了约0.19nm/%RH的灵敏度,比其它基于裸露的金纳米颗粒的传感器的灵敏度高一个数量级；另外,我们也通过监测纳米光纤输出端光功率变化来实现传感,获得的灵敏度约为0.07dB/%RH,分辨率低于1%RH,响应时间优于110ms,光功耗只需500pW。
在本论文的第四章,我们提出了将金纳米棒沉积在微光纤表面来实现对金纳米棒LSPR线宽的压缩的方案。当金纳米棒沉积在微光纤表面时,金纳米棒的LSPR模式和微光纤截面的回音壁模式发生耦合,其散射谱受到明显的周期性调制。在与直径为1.46μm的氧化硅微光纤耦合时,我们得到了约3.4nm线宽的单个散射峰,相比于正常的线宽压缩了将近15倍,同时散射峰的强度增强了约30倍。当用PAM微光纤代替氧化硅微光纤时,我们可以实现对耦合的金纳米棒散射峰的动态调控,可调范围约为40nm。
最后,在第五章中,我们总结了本论文的主要工作、创新点及未来可开展的研究计划。微纳光纤-金纳米棒组成的复合结构为微纳尺度“光子-表面等离激元”研究提供了一个新的平台,在高灵敏度生物化学传感、表面增强拉曼光谱、等离激元激光器和光学调制等领域具有广泛的应用前景。
Owing to their shape-and size-dependent optical properties know as localized surface plasmon resonance (LSPR), metal nanoparticles are finding use in a range of emerging applications such as biological and chemical sensing, surface-enhanced Raman spectroscopy, biomedicine and nanophotonics. To date, LSPR excitation in metal nanoparticles is commonly realized using free-space irradiation. Because of the small extinction cross section of a single nanoparticle and the relatively large irradiation area of a free-space light beam, the efficiency of photon-to-plasmon conversion is rather limited (usually less than1%). In addition, to redirect a light beam to a nanoparticle in free space, bulky components such as prisms or objectives are often required, making it difficult to realize nanoparticle-based photonic devices with miniaturized sizes and low operation optical powers. And at the same time, metal nanoparticles usually suffer from large losses because of metal's intrinsic absorption and nanoparticles" radiative scattering, which significantly broaden the plasmonic resonance linewidths of single metal nanoparticles, severely deteriorating the performance of metal nanoparticles in applications such as high-sensitivity biological and chemical sensing and surface-enhanced Raman spectroscopy. Therefore, the development of a highly efficient and compact approach for LSPR excitation in metal nanoparticles, and also a method for the dramatic reduction of plasmonic resonance linewidths of single metal nanoparticles are the current critical issues faced by the research fields of LSPR in metal nanoparticles. With this regard, we propose to integrate metal nanoparticles and one-dimensional optical waveguides (optical micro-/nanofibers), including Au nanorods embedded polymer nanofibers and Au nanorods surface-deposited optical microfibers. for the efficient and compact excitation of LSPR in Au nanorods, and also for the dramatic reduction of localized plasmonic resonance linewidths of single Au nanorods. Furthermore, we successfully apply these hybrid plasmonic-photonic structures to optical sensing, and demonstrate the dynamical tuning of plasmonic resonance wavelength of Au nanorods.
In the first chapter of the work, we briefly review the backgrounds of optical micro-/nanofibers and LSPR in Au nanorods. and also the research progress in hybrid metal nanoparticle-optical micro-/nanowaveguide structure.
In the second chapter of the work, we mainly introduce the optical properties of single optical micro-/nanofibers. Firstly, we briefly introduce the fabrication of silica and polymer micro-/nanofibers. Secondly, based on theoretical analysis and numerical calculations, we investigate the waveguiding properties of single optical micro-/nanofibers. which offer many fascinating properties such as tight optical confinement and large fraction of evanescent fields. At the same time, we introduce methods for launching light into or out of single optical micro-/nanofibers. Thirdly, we introduce methods for micro-/nanofiber functionalization, including surface modification, doping, and electron-beam activation. Finally, we introduce micromanipulation technique used to assemble micro-/nanofibers into desired structures or patterns. Above research backgrounds provide theoretical and technical basis for our following research on optical micro-/nanofiber-Au nanorod hybrid structures.
In the third chapter of the work, with the use of waveguiding polymer nanofibers embedded with Au nanorods, we demonstrate a highly efficient approach to photon-to-plasmon conversion in Au nanorods. The nanofibers are directly drawn from a polyacrylamide (PAM) solution containing Au nanorods. which are uniaxially aligned along the long axes of the fibers. When light is coupled into and guided through a single nanofiber. LSPR in the embedded Au nanorods could be efficiently excited with a photon-to-plasmon-conversion efficiency as high as70%for a single nanorod at its longitudinal plasmonic resonance wavelength. The highly efficient waveguiding excitation approach demonstrated here may open up new opportunities for developing Au-nanorod-based photonic components and devices with miniaturized sizes, high compactness, and low optical power consumption.
To demonstrate this capability, we also apply the Au-nanorod-embedded waveguiding PAM nanofibers to optical relative humidity (RH) sensing. We first investigate the spectral shift of LSPR of a single embedded Au nanorod when exposed to different levels of humidity. The sensitivity of the single Au nanorod is estimated to be～0.19nm/%RH. which is1order of magnitude higher than that of bare Au nanoparticles. Also, we realize intensity-dependent RH sensing using PAM nanofibers containing multiple Au nanorods by measuring the intensity of light output. The sensor offers a sensitivity of～0.07dB/%RH and an estimated resolution better than1%RH with a response time of110ms and an operation optical power as low as500pW.
In the fourth chapter of the work, we demonstrate dramatic reduction in plasmonic resonance linewidths of single Au nanorods by coupling them with optical microfibers. The LSPR modes of Au nanorods couple with whispering gallery modes of optical microfibers when Au nanorods are deposited on the surface of optical microfibers, which results in dramatic modulation in the scattering spectra of single Au nanorods. When the diameter of a silica microfiber goes down to1.46μm,there is only one main peak exists in the scattering spectrum of an Au nanorod with a linewidth of about3.4nm. providing a15-fold spectral narrowing as compared with linewidths of uncoupled single Au nanorods. Also, there is about30-time increase in the scattering intensities of coupled Au nanorods, which is of great importance in the enhancement of light-matter interactions. Moreover, based on PAM microfiber coupled Au nanorods, we demonstrate dynamical tuning of plasmonic resonance wavelength of Au nanorods by controlling the environmental RH, with a spectral tunability as large as～40nm.
Finally, in the fifth chapter, we provide a brief summary of our work, the innovations, and future research plans. The optical micro-/nanofiber-Au nanorod hybrid structures demonstrated here provide a new platform for "photonic-plasmonic" research at nanoscale, and show great potential in applications such as high-sensitivity biological and chemical sensing, surface enhanced Raman spectroscopy, plasmonic lasing. and optical modulations.
在本论文的第一章,我们综述了微纳光波导和金属纳米颗粒LSPR的研究背景以及典型的金属纳米颗粒-微纳光波导复合结构的研究进展。
在本论文的第二章,我们主要介绍了微纳光纤的基本光学特性。首先,我们简单介绍了氧化硅和聚合物微纳光纤的制备方法。其次,通过计算机数值模拟,我们分析了微纳光纤的光学传输特性,结果表明微纳光纤具有强的光场束缚能力和大比例倏逝场,同时我们还介绍了微纳光纤的光学输入输出方法。接着,我们介绍了微纳光纤常用的功能化方法,包括表面修饰、掺杂和电子束活化等。最后,我们演示了将微纳光纤组装成各种复杂结构的微纳操作技术。上述研究为我们后续的微纳光纤-金纳米棒复合结构研究准备了理论和技术基础。
在本论文的第三章,我们研究了纳米光纤导波高效激发金纳米棒的LSPR。首先,我们将金纳米棒掺杂进聚丙烯酰胺(polyacrylamide, PAM)溶液并制备聚合物纳米光纤,实现了金纳米棒在PAM纳米光纤中的高度有序排列。其次,我们通过倏逝波耦合方式将激发光耦合进聚合物纳米光纤,首次利用纳米光纤中的导波模式实现了掺杂金纳米棒LSPR的激发。实验测得,在纵向表面等离激元共振峰处,单个金纳米棒中的光子-激元转换效率高达70%。这一高效且紧凑的激发方式为发展小型化和低功耗的基于金属纳米颗粒的微纳光子器件提供了新的思路。
作为上述金纳米棒-聚合物纳米光纤复合结构的应用之一,我们演示了基于纳米光纤导波激发的金纳米棒的光学相对湿度(relative humidity, RH)传感。我们通过监测掺杂的单个金纳米棒LSPR峰的移动来实现湿度传感,获得了约0.19nm/%RH的灵敏度,比其它基于裸露的金纳米颗粒的传感器的灵敏度高一个数量级；另外,我们也通过监测纳米光纤输出端光功率变化来实现传感,获得的灵敏度约为0.07dB/%RH,分辨率低于1%RH,响应时间优于110ms,光功耗只需500pW。
在本论文的第四章,我们提出了将金纳米棒沉积在微光纤表面来实现对金纳米棒LSPR线宽的压缩的方案。当金纳米棒沉积在微光纤表面时,金纳米棒的LSPR模式和微光纤截面的回音壁模式发生耦合,其散射谱受到明显的周期性调制。在与直径为1.46μm的氧化硅微光纤耦合时,我们得到了约3.4nm线宽的单个散射峰,相比于正常的线宽压缩了将近15倍,同时散射峰的强度增强了约30倍。当用PAM微光纤代替氧化硅微光纤时,我们可以实现对耦合的金纳米棒散射峰的动态调控,可调范围约为40nm。
最后,在第五章中,我们总结了本论文的主要工作、创新点及未来可开展的研究计划。微纳光纤-金纳米棒组成的复合结构为微纳尺度“光子-表面等离激元”研究提供了一个新的平台,在高灵敏度生物化学传感、表面增强拉曼光谱、等离激元激光器和光学调制等领域具有广泛的应用前景。
Owing to their shape-and size-dependent optical properties know as localized surface plasmon resonance (LSPR), metal nanoparticles are finding use in a range of emerging applications such as biological and chemical sensing, surface-enhanced Raman spectroscopy, biomedicine and nanophotonics. To date, LSPR excitation in metal nanoparticles is commonly realized using free-space irradiation. Because of the small extinction cross section of a single nanoparticle and the relatively large irradiation area of a free-space light beam, the efficiency of photon-to-plasmon conversion is rather limited (usually less than1%). In addition, to redirect a light beam to a nanoparticle in free space, bulky components such as prisms or objectives are often required, making it difficult to realize nanoparticle-based photonic devices with miniaturized sizes and low operation optical powers. And at the same time, metal nanoparticles usually suffer from large losses because of metal's intrinsic absorption and nanoparticles" radiative scattering, which significantly broaden the plasmonic resonance linewidths of single metal nanoparticles, severely deteriorating the performance of metal nanoparticles in applications such as high-sensitivity biological and chemical sensing and surface-enhanced Raman spectroscopy. Therefore, the development of a highly efficient and compact approach for LSPR excitation in metal nanoparticles, and also a method for the dramatic reduction of plasmonic resonance linewidths of single metal nanoparticles are the current critical issues faced by the research fields of LSPR in metal nanoparticles. With this regard, we propose to integrate metal nanoparticles and one-dimensional optical waveguides (optical micro-/nanofibers), including Au nanorods embedded polymer nanofibers and Au nanorods surface-deposited optical microfibers. for the efficient and compact excitation of LSPR in Au nanorods, and also for the dramatic reduction of localized plasmonic resonance linewidths of single Au nanorods. Furthermore, we successfully apply these hybrid plasmonic-photonic structures to optical sensing, and demonstrate the dynamical tuning of plasmonic resonance wavelength of Au nanorods.
In the first chapter of the work, we briefly review the backgrounds of optical micro-/nanofibers and LSPR in Au nanorods. and also the research progress in hybrid metal nanoparticle-optical micro-/nanowaveguide structure.
In the second chapter of the work, we mainly introduce the optical properties of single optical micro-/nanofibers. Firstly, we briefly introduce the fabrication of silica and polymer micro-/nanofibers. Secondly, based on theoretical analysis and numerical calculations, we investigate the waveguiding properties of single optical micro-/nanofibers. which offer many fascinating properties such as tight optical confinement and large fraction of evanescent fields. At the same time, we introduce methods for launching light into or out of single optical micro-/nanofibers. Thirdly, we introduce methods for micro-/nanofiber functionalization, including surface modification, doping, and electron-beam activation. Finally, we introduce micromanipulation technique used to assemble micro-/nanofibers into desired structures or patterns. Above research backgrounds provide theoretical and technical basis for our following research on optical micro-/nanofiber-Au nanorod hybrid structures.
In the third chapter of the work, with the use of waveguiding polymer nanofibers embedded with Au nanorods, we demonstrate a highly efficient approach to photon-to-plasmon conversion in Au nanorods. The nanofibers are directly drawn from a polyacrylamide (PAM) solution containing Au nanorods. which are uniaxially aligned along the long axes of the fibers. When light is coupled into and guided through a single nanofiber. LSPR in the embedded Au nanorods could be efficiently excited with a photon-to-plasmon-conversion efficiency as high as70%for a single nanorod at its longitudinal plasmonic resonance wavelength. The highly efficient waveguiding excitation approach demonstrated here may open up new opportunities for developing Au-nanorod-based photonic components and devices with miniaturized sizes, high compactness, and low optical power consumption.
To demonstrate this capability, we also apply the Au-nanorod-embedded waveguiding PAM nanofibers to optical relative humidity (RH) sensing. We first investigate the spectral shift of LSPR of a single embedded Au nanorod when exposed to different levels of humidity. The sensitivity of the single Au nanorod is estimated to be～0.19nm/%RH. which is1order of magnitude higher than that of bare Au nanoparticles. Also, we realize intensity-dependent RH sensing using PAM nanofibers containing multiple Au nanorods by measuring the intensity of light output. The sensor offers a sensitivity of～0.07dB/%RH and an estimated resolution better than1%RH with a response time of110ms and an operation optical power as low as500pW.
In the fourth chapter of the work, we demonstrate dramatic reduction in plasmonic resonance linewidths of single Au nanorods by coupling them with optical microfibers. The LSPR modes of Au nanorods couple with whispering gallery modes of optical microfibers when Au nanorods are deposited on the surface of optical microfibers, which results in dramatic modulation in the scattering spectra of single Au nanorods. When the diameter of a silica microfiber goes down to1.46μm,there is only one main peak exists in the scattering spectrum of an Au nanorod with a linewidth of about3.4nm. providing a15-fold spectral narrowing as compared with linewidths of uncoupled single Au nanorods. Also, there is about30-time increase in the scattering intensities of coupled Au nanorods, which is of great importance in the enhancement of light-matter interactions. Moreover, based on PAM microfiber coupled Au nanorods, we demonstrate dynamical tuning of plasmonic resonance wavelength of Au nanorods by controlling the environmental RH, with a spectral tunability as large as～40nm.
Finally, in the fifth chapter, we provide a brief summary of our work, the innovations, and future research plans. The optical micro-/nanofiber-Au nanorod hybrid structures demonstrated here provide a new platform for "photonic-plasmonic" research at nanoscale, and show great potential in applications such as high-sensitivity biological and chemical sensing, surface enhanced Raman spectroscopy, plasmonic lasing. and optical modulations.
引文
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