基于人工局域表面等离激元的高灵敏传感研究进展(特邀)
0 引言
人工局域表面等离激元(Spoof Localized Surface Plasmons,SLSPs)基于电磁超材料的人工微结构,在微波、毫米波等频段构造等效的负介电常数,从而重现光学频段局域表面等离激元的谐振模场分布、亚波长场局域性、对介电环境的高度敏感性等优异特性[1,2]。此概念在2012年由英国帝国理工学院的PENDRY John教授首次提出,并在二维无限深的金属刻槽结构中进行了理论和仿真分析[2]。2014年,东南大学的崔铁军院士团队通过理论和实验证明,超薄金属图形也可以支持人工局域表面等离激元谐振模式,从而将人工局域表面等离激元从物理概念推向了平面印刷电路应用[3,4]。之后,人工局域表面等离激元得到了国内外学者的广泛关注和跟踪研究,并在微带滤波器、小型化谐振天线等器件设计、微波和太赫兹高灵敏传感等领域中得到应用验证[1,5-9]。
人工局域表面等离激元作为一种新型的电磁谐振模式,有望解决传统微波谐振传感发展的瓶颈问题。微波谐振传感表现为谐振频率随周围介电环境的变化,具有实时无标记的传感能力和优异的环境适应性,基于不同的敏感材料(transducer materials)可以实现灵活多样的物理、化学和生物传感功能。但受限于波长,微波谐振传感无法达到光学谐振传感的单分子检测精度[10,11],难以满足微量目标检测的实际需求。近年来的研究证实,人工局域表面等离激元的深亚波长场束缚性已经突破百分之一波长[12],有望在鲁棒性高、造价经济的低频段,实现等效波长所对应的高灵敏度,从而突破微波谐振传感对微量目标的检测极限[13]。并且,得益于金属在微波等低频段的低欧姆损耗,以及人工微结构的设计灵活性,人工局域表面等离激元可以实现丰富的高阶谐振模式以及高品质因子[5,12]。此外,人工局域表面等离激元可以和信号检测电路以及通信电路集成,从而发展出高度集成化小型化的传感系统,有望推动万物互联时代下传感技术的发展升级[1]。
1 人工局域表面等离激元传感的新探索
人工局域表面等离激元是2012年提出的新概念,其在印刷电路中的典型结构和谐振模式如
图 1. 人工局域表面等离激元典型的结构和模式性质[3-5,12]
Fig. 1. Typical spoof localized surface plasmons' structures and modal properties[3-5,12]
1.1 人工局域表面等离激元的新型电磁模式
连续体中的束缚态是一类不具有辐射的电磁本征态,不能被直接激发。研究发现通过调整系统构型、周期边界等可以获得连续体中束缚态的辐射泄漏模式,即连续体中的准束缚态,表现为在亚波长尺度形成高密度、局域化的电磁场能量增强,具有高品质因子的特性。近几年,人工局域表面等离激元单元及阵列结构中的准连续体中束缚态效应被陆续报道,实现了品质因子的持续提升[12,14,15]。2021年东南大学崔铁军和张璇如团队[12]基于微带电路激励的人工局域表面等离激元谐振器,通过引入狭缝破坏结构的对称性,极大抑制了辐射损耗,实现了电偶极子和磁偶极子的混合模式,将谐振器直径压缩至1/20波长以内,并实验测得了53.3的品质因子,如
图 2. 人工局域表面等离激元的新型电磁模式[12,15,18,19,25,26]
Fig. 2. Novel electromagnetic modes of spoof localized surface plasmons[12,15,18,19,25,26]
斯格明子由于其特殊的拓扑不变性而引起了广泛的关注,为矢量场拓扑特性的分析和控制提供了新的方法[16,17]。2021年暨南大学的邓子岚和李向平团队[18]基于单螺旋人工局域表面等离激元谐振结构实现了磁质斯格明子并证明了该斯格明子的拓扑不变性,如
除谐振频移检测之外,谐振传感还存在另外一种重要的形式,即对微扰散射体引起的谐振峰劈裂信号的传感。应用非厄米系统中的特殊模态简并现象——奇异点,可以使得共振频移或分裂与扰动强度呈平方根依赖性,极大增强了谐振峰劈裂传感对极微小扰动信号检测的灵敏度。奇异点现象最初用于增强光学微腔对微小散射体的检测信号[21-24],近两年才发展到微波段的人工局域表面等离激元领域。2023年韩国国立蔚山科学技术院JUN Y C等[25]通过变容二极管的容值调节人工局域表面等离激元谐振模态间的耦合作用,实现了对奇异点的主动调控,如
涡旋波表现为电磁场涡旋状的相位波前,此概念经常与轨道角动量(Orbital Angular Momentum,OAM)联系在一起,可以为电磁波提供频率、幅度、相位、极化之外的又一信息维度,在超高速超大容量通信、涡旋波雷达等领域展示了丰富的应用潜力[27-31]。常见涡旋波产生技术都依赖于螺旋相位板、阵列天线、超表面等提供相位梯度的阵列结构[32-36],而单个人工局域表面等离激元谐振单元也可产生多阶涡旋波模态,展示出更紧凑的结构尺寸、更灵活可调谐性、和更丰富的应用场景[37-40]。2018年南京大学的王振林团队[37]利用人工表面等离激元(Spoof Surface Plasmons,SSPs)波导的传输模式,选择性激发人工局域表面等离激元中的涡旋波模式,如
图 3. 基于人工局域表面等离激元的微波涡旋波研究[37,38,40,44]
Fig. 3. Microwave vortex wave studies based on spoof localized surface plasmons[37,38,40,44]
涡旋波的螺旋相位波前可以提供丰富的信息维度,有望提升其对散射体形状、方位角、旋转速度等物理量的探测能力[41-44]。2020年东南大学的崔铁军和张璇如团队[44]在人工局域表面等离激元结构中激励了束缚态的涡旋波模态,将一阶涡旋波模态压缩至1/11波长直径以内,并利用其高品质因子的谐振峰,实现了对直径1/60波长手性颗粒的实验探测,如
1.2 人工局域表面等离激元的新型谐振结构
随着人工局域表面等离激元的蓬勃发展,扇形结构、折纸超材料等新型谐振结构的出现,为人工局域表面等离激元传感器设计提供了新思路和新方法。2016年新加坡南洋理工大学的张柏乐和南方科技大学的高振等[45]研究了扇形的人工局域表面等离激元结构,如
图 4. 人工局域表面等离激元的新型谐振结构[45,46]
Fig. 4. Novel resonance structures of spoof localized surface plasmons[45,46]
2023年浙江大学陈红胜和王作佳团队[46]报道了一种折纸超材料结构中的一阶杂化等离激元共振,该结构由相互连接的网格型超表面作为超薄金属薄膜进行折叠得到,可构建正方形、三棱柱形、圆柱形等三维结构,这些结构都支持三维的人工局域表面等离激元共振,如
1.3 太赫兹人工局域表面等离激元传感
太赫兹(terahertz)频段位于微波毫米波与红外可见光之间,连接了电子学和光子学领域,具有独特的性质。由于大量有机分子的振动转动能级都落在太赫兹频段,表现为太赫兹特征吸收峰,因此,太赫兹传感受到了极为广泛的关注。人工局域表面等离激元可以在太赫兹频段产生[47-49],然而,受限于加工精度、材料属性、以及太赫兹产生探测技术,太赫兹人工局域表面等离激元难以实现微波频段那样灵活多变的设计,品质因子等指标的提升也面临更大的挑战。
2016年东南大学崔铁军、廖臻等[50]用螺旋形人工局域表面等离激元谐振器与短截线间耦合,在太赫兹频率下实现电磁诱导的透明效应(Electromagnetically Induced Transparency,EIT),如
上述太赫兹人工局域表面等离激元的研究都是基于太赫兹时域光谱技术(Terahertz Time-Domain Spectroscopy,THz-TDS)对空间波激励下的阵列结构进行测量,适用于较高太赫兹频段的宽频响应研究。为实现更高的集成度,半导体集成电路成为太赫兹技术发展的趋势。2020上海理工大学朱亦鸣团队[54]通过人工表面等离激元波导激发人工局域表面等离激元高阶径向模式,如
2 人工局域表面等离激元的传感增强技术
电磁谐振传感技术的核心指标包括传感灵敏度、品质因子和激励效率。传感灵敏度决定了相同检测目标下谐振峰频移量的大小,而品质因子和激励效率决定了谐振峰频移量的检测难度。对于人工局域表面等离激元传感,在谐振器结构和电磁模式设计之外,可以通过模式耦合构造电磁能量高速汇聚的传感热点结构,或构造高灵敏的杂化模式,进而提升传感灵敏度。加载有源放大器来补偿传感结构中的损耗,也可以实现品质因子和激励效率的提升。
2.1 人工局域表面等离激元的耦合增强原理
多层印刷电路板结构为人工局域表面等离激元的耦合增强研究提供了丰富的可能:在人工局域表面等离激元结构之间,可以灵活地构造平面内耦合、层间耦合,在单个人工局域表面等离激元结构内部,也可以构造不同模式间的耦合,如
围绕人工局域表面等离激元的层间耦合形式,2016年新加坡南洋理工大学张柏乐与浙江大学高飞等[58]通过垂直堆叠的两个人工局域表面等离激元之间的强耦合,观察到一个具有不对称法诺线形的谐振谱,如
考虑传感应用需求,需要将人工局域表面等离激元在微带电路中激励,并在单个人工局域表面等离激元单元内部构造耦合效应,以减小器件尺寸。2020年东南大学崔铁军、张璇如[60]将一个扇形的扰动谐振(Perturbing Resonator,PR)结构与人工局域表面等离激元谐振器叠放,形成混合模式的人工局域表面等离激元谐振器,如
2.2 人工局域表面等离激元的放大增强技术
为提升谐振的品质因子,除无源结构优化和耦合效应之外,最常用的方式是引入有源增益补偿损耗;对于微波谐振器而言,可以方便地利用集总的放大器芯片实现[62,63]。人工局域表面等离激元具有灵活多变的结构设计可能,可以将低噪声放大器芯片加载在单元内部。2018年上海大学周永金等[64]率先提出了利用放大器芯片提升人工局域表面等离激元品质因子的方案。2019年东南大学崔铁军和上海大学周永金等[65]提出了一种方形双层结构的人工局域表面等离激元谐振器,利用层间杂化的作用产生法诺共振,再将放大器芯片加载到人工局域表面等离激元结构中,实现了对法诺共振模式的放大增强,如
图 7. 人工局域表面等离激元的有源放大增强[65-68]
Fig. 7. Active amplification enhancement of spoof localized surface plasmons[65-68]
放大增强的另一种结构是在谐振器外侧引入耦合电路,将有源放大芯片置于耦合电路中。2019年上海大学周永金团队[66]设计了一种 金属-绝缘体-金属(Metal-Insulator-Metal,MIM)环形人工局域表面等离激元谐振器。通过在背部引入耦合枝节,使得只有四极模式被放大芯片选择性放大,通过调整偏置电压,测量的传输强度从-6.46 dB增加到10.74 dB,如
3 人工局域表面等离激元传感的应用研究
人工局域表面等离激元传感与其他电磁谐振传感技术一样,采用不同的敏感材料,可灵活应用于多种物理和化学传感器:如基于介电常数随溶液浓度或成分变化的生化传感器[69-73],以特异性吸附聚合物为敏感材料层的气体传感器[74-77]、基于柔性介质基板的力学量传感器[78-83]等。人工局域表面等离激元作为2012年提出的新概念,其应用研究尚处于探索阶段,本节将具体介绍部分代表性工作。
3.1 基于人工局域表面等离激元的溶液浓度传感
基于人工局域表面等离激元的溶液浓度传感已被报道应用于葡萄糖溶液、酒精溶液、油水混合物的检测,通常采用微流体通道来控制待测溶液形成一个相对稳定的传感环境[13,67]。水溶液在微波频段的高介电常数和高介电损耗特性[84],对微波谐振传感的品质因子和谐振强度都提出了更高的要求。随着研究的推进,人工局域表面等离激元溶液浓度传感也从最初的传感功能演示,进入对检测极限指标的持续提升阶段。
2022年东南大学的崔铁军和张璇如课题组[13]提出了一种深亚波长的人工局域表面等离激元谐振结构,将基模谐振压缩至1/41波长,测量品质因子达到187,如
图 8. 基于人工局域表面等离激元的溶液浓度传感[13,54,70]
Fig. 8. Solution concentration sensing based on spoof localized surface plasmons[13,54,70]
3.2 基于人工局域表面等离激元的细胞传感
相比于溶液浓度传感,单细胞传感需要更高的检测精度[85,86]。近年来,随着微波谐振传感灵敏度和检测极限等指标日益提升,基于微波谐振的细胞传感工作也在逐步展开[87,88]。2021年德国杜伊斯堡-埃森大学团队[89,90]制备了太赫兹频段的人工局域表面等离激元谐振结构,并实现从太赫兹天线到波导的高效耦合。该团队展示了此人工局域表面等离激元谐振器在细菌计数中的应用潜力,如
3.3 基于人工局域表面等离激元的力学传感
印刷电路的介质基板在压力、拉力等作用下会产生形变,导致等效介电常数的变化,引起谐振峰频移。基于此原理,人工局域表面等离激元也可应用于力学量的传感,并用于柔性可穿戴设备中。2016年新加坡南洋理工大学的SOH C K团队[91]通过非接触、近场测量的人工局域表面等离激元传感器,实现对工程结构横向(垂直于表面)载荷的测量,示意图如
图 10. 基于人工局域表面等离激元的力学量传感[84,91-95]
Fig. 10. Force sensing based on spoof localized surface plasmons[84,91-95]
4 人工局域表面等离激元传感的系统集成
电磁谐振传感器对谐振峰频率的相对移动信号进行测量,相比于幅度或强度检测,易于获得更高的检测信噪比。然而,谐振峰频移信号的检测也更加复杂,现有的微波谐振传感大多依赖于矢量网络分析仪等台式仪器进行检测,小型化检测系统的研究方兴未艾。对于传统的叉指电极等微波谐振传感器,可以采用有源振荡和锁相环技术,将无源谐振信号转化为有源振荡信号,从而进行检测[96-98]。但深亚波长人工局域表面等离激元独特的振幅和相位响应,为有源振荡电路带来更大的挑战[99]。
2023年东南大学的崔铁军和张璇如课题组[100]提出并完成了一款小型化、智能化、无线物联的人工局域表面等离激元传感系统,如
5 总结与展望
从2012年人工局域表面等离激元传感提出至今的十多年里,该领域经历了高速发展,在新原理新现象持续涌现的同时,其小型化传感系统已初见雏形。万物互联时代对小型化、便携式传感技术的新需求,赋予了人工局域表面等离激元传感重要的实用价值和广阔的发展空间。
针对实际应用需求,人工局域表面等离激元传感领域面临着以下亟待解决的问题:1)持续挖掘人工局域表面等离激元微结构中可能存在的谐振新原理;2)持续突破传感相关指标,以满足实际传感的应用需要;3)致力于研究高精度、小型化的传感信号检测电路,推动小型化便携式传感系统的发展。最终,我们将实现小型化、物联化和高灵敏的传感系统,推进医疗、健康、环境等相关产业中传感技术发展升级。
在接下来的研究中,一方面迫切地需要面向生物医学、环境监测等实际应用需求,进行典型应用验证,明确人工局域表面等离激元相比于现有技术确有优势的应用场景,推动实质性的应用落地。另一方面,人工局域表面等离激元的结构设计仍然围绕提出初期的几种典型图形,人工微结构设计的灵活性尚未得到充分发挥,其中蕴含的新原理新现象也有待探究,并有望带来传感能力的大幅提升。因此,新物理研究和应用探索的同时进行和相互促进,还将是人工局域表面等离激元传感领域持续的发展趋势。
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Article Outline
白天硕, 王莞竹, 张龙飞, 张璇如, 崔铁军. 基于人工局域表面等离激元的高灵敏传感研究进展(特邀)[J]. 光子学报, 2023, 52(10): 1052401. Tianshuo BAI, Wanzhu WANG, Longfei ZHANG, Xuanru ZHANG, Tiejun CUI. Progress in Highly Sensitive Sensing Based on Spoof Localized Surface Plasmons(Invited)[J]. ACTA PHOTONICA SINICA, 2023, 52(10): 1052401.