单个等离激元纳米颗粒和纳米间隙结构与量子发光体的强耦合

闫晓宏; 牛亦杰; 徐红星; 魏红

doi:10.7498/aps.71.20211900

摘要

在腔量子电动力学中, 如果量子发光体与腔模式的耦合强度超过二者的平均损耗, 就进入了强耦合区域, 此时会形成部分光部分物质的新量子态—极化激元态. 强耦合在室温玻色-爱因斯坦凝聚、极化激元激光、单光子非线性、量子信息等领域有重要的应用价值. 基于单个金属纳米颗粒的结构可以支持局域表面等离激元共振, 拥有极小的模式体积, 非常有利于强耦合现象的发生. 本文主要介绍了强耦合的理论背景、单个金属纳米颗粒和纳米间隙结构与量子发光体的强耦合、以及强耦合的动态调控, 并展望了该领域的研究前景.

关键词:

Abstract

In cavity quantum electrodynamics, when the interaction between quantum emitter and cavity mode is strong enough to overcome the mean decay rate of the system, it will enter into a strong coupling regime, thereby forming part-light part-matter polariton states. Strong coupling can serve as a promising platform for room temperature Bose-Einstein condensation, polariton lasing, single photon nonlinearity, quantum information, etc. Localized surface plasmons supported by single metal nanostructures possess extremely small mode volume, which is favorable for realizing strong coupling. Moreover, the nanoscale dimensions of plasmonic structures can facilitate the miniaturization of strong coupling systems. Here, the research progress of strong plasmon-exciton coupling between single metal nanoparticles/nanogaps and quantum emitters is reviewed. The theory background of strong coupling is first introduced, including quantum treatment, classical coupled oscillator model, as well as the analytical expressions for scattering and photoluminescence spectra. Then, strong coupling between different kinds of plasmonic nanostructures and quantum emitters is reviewed. Single metal nanoparticles, nanoparticle dimers, and nanoparticle-on-mirror structures constitute the most typical plasmonic nanostructures. The nanogaps in the latter two systems can highly concentrate electromagnetic field, providing optical nanocavities with smaller mode volume than single nanoparticles. Therefore, the larger coupling strength can be achieved in the nanogap systems, which is conducive to strong coupling at the single-exciton level. In addition, the active tuning of strong coupling based separately on thermal, electrical and optical means are reviewed. The energy and oscillator strength of the excitons in transition metal dichalcogenide (TMDC) monolayers are dependent on temperature. Therefore, the strong coupling can be tuned by heating or cooling the system. The excitons in TMDC monolayers can also be tuned by electrical gating, enabling electrical control of strong coupling. Optically tuning the quantum emitters provides another way to actively control the strong coupling. Overall, the research on active tuning of strong plasmon-exciton coupling is still very limited, and more investigations are needed. Finally, this review is concluded with a short summary and the prospect of this field.

Keywords:

作者及机构信息

1.
中国科学院物理研究所, 北京凝聚态物理国家研究中心, 北京　100190

2.
中国科学院大学物理科学学院, 北京　100049

3.
武汉大学物理科学与技术学院, 武汉　430072

4.
松山湖材料实验室, 东莞　523808

通信作者: 魏红, weihong@iphy.ac.cn

基金项目: 国家自然科学基金(批准号: 11774413, 12074421, 91850207)和中国科学院战略性先导科技专项(B类)(批准号: XDB33000000)资助的课题

Authors and contacts

1.
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

2.
School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China

3.
School of Physics and Technology, Wuhan University, Wuhan 430072, China

4.
Songshan Lake Materials Laboratory, Dongguan 523808, China

Corresponding author: Wei Hong, weihong@iphy.ac.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 11774413, 12074421, 91850207) and the Strategic Priority Research Program of Chinese Academy of Sciences (Grant No. XDB33000000).

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参考文献

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施引文献

图 1 单个金属纳米颗粒与量子发光体的强耦合　(a), (b)单个纳米棒与量子发光体的强耦合, (a)左上图为单个银纳米棒在单层WSe₂上的示意图, 插图展示了银纳米棒上第3阶等离激元模式电场分布的计算结果, 右图为银纳米棒-WSe₂耦合体系随氧化铝薄膜厚度增加的暗场散射光谱, 左下图为极化激元的色散曲线, 实线表示拟合结果^[19]; (b) 上图为金纳米棒和Au@Ag长方体纳米棒的透射电子显微镜(transmission electron microscopy, TEM)图像、示意图以及纵向等离激元模式电场分布的计算结果, 下图为Au@Ag长方体纳米棒与J-聚体耦合体系拉比劈裂的测量值及平均激子数目的计算值随分子浓度的变化关系^[23]; (c)—(e) 单个纳米片与量子发光体的强耦合, (c) 银纳米片(青色)以及银纳米片与J-聚体耦合体系(蓝色)的暗场散射光谱^[30]; (d)银纳米片与J-聚体耦合体系的暗场散射光谱和荧光光谱(分别通过532和568 nm的激光激发)的峰位^[31]; (e) 银纳米片-六层WS₂耦合体系的暗场散射光谱及对应的EELS谱^[32]; (f) 单个纳米双锥体与量子发光体的强耦合, 上图为金纳米双锥体在单层WSe₂上的能量密度分布, 插图为尖端附近的放大图, 下图为拉比劈裂值和耦合强度随WSe₂层数的变化关系^[35]; (g) 5个不同金纳米盘-单层WS₂耦合体系的散射光谱和反射光谱^[37]

Fig. 1. Strong coupling of single metal nanoparticles and quantum emitters: (a), (b) Single nanorods strongly coupled with quantum emitters. (a) Left-top panel shows the schematic of a single Ag nanorod on monolayer WSe₂. The inset indicates the calculated electric field distribution of the 3rd order plasmon mode of a Ag nanorod. Right panel shows a set of scattering spectra of Ag nanorod-WSe₂ coupled system with increasing alumina thickness. Left-bottom panel shows the dispersion of plexcitons. The solid lines are the fitting results^[19]. (b) Top panel shows transmission electron microscopy (TEM) images, schematics and calculated electric field distributions of Au nanorod and Au@Ag cuboid, respectively. Bottom panel shows the statistics of the Rabi splitting measured for individual coupled systems and the corresponding calculated mean exciton numbers for each dye concentration^[23]. (c)–(e) Single nanoprisms strongly coupled with quantum emitters. (c) Dark-field scattering spectra of a Ag nanoprism (cyan) and a coupled system of Ag nanoprism and J-aggregates (blue)^[30]. (d) Correlations between the peaks of dark-field scattering spectra and photoluminescence spectra of the coupled system of Ag nanoprism and J-aggregates ^[31]. (e) Correlated dark-field scattering spectrum and EELS spectrum for the coupled system of Ag nanoprism and six-layer WS₂^[32]. (f) Single bipyramids strongly coupled with quantum emitters. Top panel shows the energy density cross-section of a Au bipyramid on top of WSe₂ monolayer. The inset shows the enlarged view around the tip. Bottom panel shows the Rabi splitting and coupling strength as a function of the number of WSe₂ layers^[35]. (g) Experimental scattering and reflection spectra for five different individual Au nanodisk-monolayer WS₂ coupled systems^[37].

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图 2 单个等离激元二聚体与量子发光体的强耦合　(a) 左图为金纳米盘二聚体和J-聚体耦合体系的散射光谱及对应尺寸的金纳米盘二聚体的扫描电子显微镜(scanning electron microscopy, SEM)图, 比例尺是100 nm, 右图为该耦合体系中极化激元的色散曲线^[40]; (b) 金纳米颗粒二聚体(黑色)及其与J-聚体耦合体系(蓝色)的散射光谱及相应的SEM和暗场显微图, 比例尺是100 nm^[41]; (c) 间隙中分别有1, 2和3个量子点的银纳米蝴蝶结结构的散射光谱及相应的SEM图, 比例尺是20 nm^[44]; (d) 左图为金纳米蝴蝶结(蓝色)及覆盖有单层WSe₂的同一纳米蝴蝶结结构(红色)的暗场散射光谱和相应的SEM图, 右图为耦合强度g的实验值、模拟值和$1/\sqrt V $的模拟值随失谐量的变化关系^[46]

Fig. 2. Strong coupling of single plasmonic dimers and quantum emitters: (a) Left panel shows the scattering spectra of Au nanodisk dimers coupled with J-aggregates and the corresponding scanning electron microscopy (SEM) images of bare Au nanodisk dimers with the same sizes. The scale bars are 100 nm. Right panel shows the dispersion of plexcitons for this system^[40]. (b) Scattering spectra of nanoparticle dimers with (blue) and without (black) J-aggregates, as well as the corresponding SEM and dark-field microscopy images^[41]. The scale bars are 100 nm. (c) Scattering spectra of Ag nanobowties with one, two and three quantum dots in the gap and the corresponding SEM images. The scale bars are 20 nm^[44]. (d) Left panel shows the scattering spectra of bare Au nanobowties (blue) and the same nanobowties coated with WSe₂ monolayers (red), as well as the corresponding SEM images of the hybrid systems. Right panel shows the experimental and simulated coupling strength g and simulated $1/\sqrt V $ as a function of detuning ^[46].

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图 3 单个NPoM结构与量子发光体的强耦合　(a) 单个CdSe/CdS量子点位于准球状金纳米颗粒和银膜间隙中的耦合体系的制备过程示意图(上)及其暗场散射光谱和荧光光谱(下)^[13]; (b) 金纳米立方体和金膜的间隙中放入J-聚体的示意图(上)及散射光谱(下), 插图分别表示通过650 nm 短通(绿色)和长通(红色)滤波片的远场散射图像^[55]; (c) 单层WS₂、金纳米片放置在金膜上的结构及单层WS₂与NPoM耦合体系对应的光谱、结构示意图以及光学或者SEM图像^[60]; (d) 左图为金针尖-量子点的横向距离从30 nm缩减到0所对应的荧光光谱, 右图为由不同量子点的荧光光谱获得的极化激元能量相对失谐量的变化关系^[61]

Fig. 3. Strong coupling of single NPoM structures and quantum emitters: (a) Sketch of the assembly process for the coupled system of a single CdSe/CdS quantum dot located in the nanogap between a quasi-spherical Au nanoparticle and Ag film (top) as well as the scattering and photoluminescence spectra of the coupled system (bottom)^[13]. (b) Schematic (top) and scattering spectrum (bottom) of a Au nanocube on Au film with J-aggregates in the gap. The insets show the far-field scattering images collected through short-pass (green) and long-pass (red) filers, respectively^[55]. (c) Spectra, schematics and optical or SEM images of monolayer WS₂ on Au film, NPoM structure composed of a Au nanoprism and Au film, and monolayer WS₂-NPoM coupled system, respectively^[60]. (d) Left panel shows the photoluminescence spectra as the lateral distances between the Au tip and quantum dot are varied from 30 to 0 nm. Right panel shows the plexciton energies as a function of detuning extracted from the photoluminescence spectra of different quantum dots^[61].

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图 4 强耦合体系的热调控　(a) 单个金纳米棒与单层WS₂强耦合体系的示意图(左上)、不同温度下的暗场散射光谱(右)和耦合体系散射光谱峰位相对失谐量的关系图(左下)^[20]; (b) 单个Au@Ag纳米长方体置于单层过渡金属硫属化合物之上的示意图(左), 单个Au@Ag纳米长方体与单层WS₂的耦合强度(中)及单层WS₂的振子强度(右)随温度的变化^[14]; (c) 单个银纳米片与单层WS₂强耦合体系的示意图(上)及不同温度下的暗场散射光谱(下)^[33]

Fig. 4. Active tuning of strongly coupled systems by heat: (a) Sketch (left-top), temperature dependent scattering spectra (right) and the extracted peak energies of the scattering spectra as a function of detuning (left-bottom) for a Au nanorod strongly coupled with monolayer WS₂^[20]. (b) Sketch of a Au@Ag nanocuboid on top of monolayer transition metal dichalcogenides (left), temperature dependent coupling strength between a Au@Ag nanocuboid and monolayer WS₂ (middle) and temperature dependent oscillator strength for monolayer WS₂ (right) ^[14]. (c) Sketch (top) and temperature dependent scattering spectra (bottom) for a Ag nanoprism strongly coupled with monolayer WS₂^[33].

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图 5 强耦合体系的电调控和光调控　(a) 背栅压调控单个银纳米片与单层WS₂强耦合的示意图(左), 该体系在77 K温度下激子的振子强度(中)及表面等离激元-激子耦合强度(右)随背栅压的变化^[24]; (b) 利用光漂白作用调控单个银纳米片与J-聚体强耦合的示意图(左), 该体系在不同光照时间下的散射光谱(中)及活性分子相对浓度随光照时间的变化(右)^[28]

Fig. 5. Active tuning of strongly coupled systems by electrical and optical means: (a) Sketch of a single Ag nanoprism strongly coupled with monolayer WS₂ under back gating (left), and exciton oscillator strength (middle) and plasmon-exciton coupling strength (right) of the system under different gate voltages at 77 K^[24]. (b) Sketch of strongly coupled Ag nanoprism and J-aggregates (left), scattering spectra of the coupled system for different irradiation time (middle) and relative change in the concentration of active molecules as a function of irradiation time (right)^[28].

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map

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[3]	Rodriguez S R K, Feist J, Verschuuren M A, Garcia Vidal F J, Gómez Rivas J 2013 Phys. Rev. Lett. 111 166802 Google Scholar
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[11]	Wu X H, Gray S K, Pelton M 2010 Opt. Express 18 23633 Google Scholar
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[13]	Leng H X, Szychowski B, Daniel M C, Pelton M 2018 Nat. Commun. 9 4012 Google Scholar
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单个等离激元纳米颗粒和纳米间隙结构与量子发光体的强耦合