Simultaneous Control of Light Polarization and Phase Distributions Using Plasmonic Metasurfaces

Harnessing light for modern photonic applications often involves the control and manipulation of light polarization and phase. Traditional methods require a combination of multiple discrete optical components, each of which contributes to a specific functionality. Here, plasmonic metasurfaces are proposed that accomplish the simultaneous manipulation of polarization and phase of the transmitted light. Arbitrary spatial field distribution of the optical phase and polarization direction can be obtained. The multifunctional metasurfaces are validated by demonstrating a broadband near‐perfect anomalous refraction with controllable linear polarization through introducing a constant phase gradient along the interface. Furthermore, the power of the proposed metasurfaces is demonstrated by generating a radially polarized beam. The new degrees of freedom of metasurfaces facilitate arbitrary manipulation of light and will profoundly affect a wide range of photonic applications.     

All‐Dielectric Programmable Huygens' Metasurfaces

Low‐loss nanostructured dielectric metasurfaces have emerged as a breakthrough platform for ultrathin optics and cutting‐edge photonic applications, including beam shaping, focusing, and holography. However, the static nature of their constituent materials has traditionally limited them to fixed functionalities. Tunable all‐dielectric infrared Huygens' metasurfaces consisting of multi‐layer Ge disk meta‐units with strategically incorporated non‐volatile phase change material Ge₃Sb₂Te₆ are introduced. Switching the phase‐change material between its amorphous and crystalline structural state enables nearly full dynamic light phase control with high transmittance in the mid‐IR spectrum. The metasurface is realized experimentally, showing post‐fabrication tuning of the light phase within a range of 81% of the full 2π phase shift. Additionally, the versatility of the tunable Huygen's metasurfaces is demonstrated by optically programming the spatial light phase distribution of the metasurface with single meta‐unit precision and retrieving high‐resolution phase‐encoded images using hyperspectral measurements. The programmable metasurface concept overcomes the static limitations of previous dielectric metasurfaces, paving the way for “universal” metasurfaces and highly efficient, ultracompact active optical elements like tunable lenses, dynamic holograms, and spatial light modulators.     

Full‐State Synthesis of Electromagnetic Fields using High Efficiency Phase‐Only Metasurfaces

A metasurface is a thin array of subwavelength elements with designable scattering responses, and metasurface holography is a powerful tool for imaging and field control. The existing metasurface holograms are classified into two types: one is based on phase‐only metasurfaces (including the recently presented vectorial metasurface holography), which has high power efficiency but cannot control the phases of generated fields; while the other is based on phase‐amplitude‐modulated metasurfaces, which can control both field amplitudes and phases in the region of interest (ROI) but has very low efficiency. Here, for the first time, it is proposed to synthesize the field amplitudes and phases in ROI simultaneously and independently by using high‐efficiency phase‐only metasurfaces. All points in ROI may have independent values of field amplitudes and phases, and the requirements for X and Y components may be different in achieving spatially varied polarization states. To this end, an efficient design method based on equivalent electromagnetic model and gradient‐based nonlinear optimization is proposed. Full‐wave simulations and experimental results demonstrate that the phase‐only metasurface designed by the method has 10 times higher efficiency than the phase‐amplitude‐modulated metasurface. This work opens a way to realize more complicated and high‐efficiency metasurface holography.     

宽带消色差红外光学超构透镜研究进展（特邀）

超构透镜是由亚波长散射单元结构排列而成的具有聚焦功能的平面二维超构表面。超构表面能够在亚波长尺度上操控光场的振幅、相位、色散和偏振态,是近年来迅速发展起来的新型光场调控载体。亚波长共振纳米结构使得高阶衍射被抑制,入射光场可以完美地被调制到设计的衍射级次上,从而确保了超构表面器件具有高的光子调控效率。同时,超构单元在设计上的灵活性及其特定的电磁响应使得超构表面可以实现对光场多个维度的定制化操控。不同于传统光学透镜依赖光传播的相位累积效应,宽带消色差超构透镜通过对光场相位和相位色散的同时独立调控解决了传统通过级联多个透镜修正色差造成的光学系统复杂和体积庞大限制,为发展小型化片上集成光学提供了全新的思路。文中围绕超构透镜的相关研究,首先介绍了超构表面调控光场振幅、相位和偏振态的基本原理,在此基础上,重点回顾了近年来关于超透镜的研究发展,包括通过单一参量调控的单波长超透镜的实现,以及通过对光场偏振、相位及相位色散的多参量联合调控的多功能宽带消色差超构透镜的发展现状,最后讨论其进一步发展的可能挑战与应用前景。     

Full‐Color Complex‐Amplitude Vectorial Holograms Based on Multi‐Freedom Metasurfaces

Phase, polarization, amplitude, and frequency represent the basic dimensions of light, playing crucial roles for both fundamental light–material interactions and all major optical applications. Metasurfaces have emerged as a compact platform to manipulate these knobs, but previous metasurfaces have limited flexibility to simultaneous control them. A multi‐freedom metasurface that can simultaneously and independently modulate phase, polarization, and amplitude in an analytical form is introduced, and frequency multiplexing is further realized by a k‐space engineering technique. The multi‐freedom metasurface seamlessly combines geometric Pancharatnam–Berry phase and detour phase, both of which are frequency independent. As a result, it allows complex‐amplitude vectorial hologram at various frequencies based on the same design strategy, without sophisticated nanostructure searching of massive geometric parameters. Based on this principle, full‐color complex‐amplitude vectorial meta‐holograms in the visible are experimentally demonstrated with a metal–insulator–metal architecture, unlocking the long‐sought full potential of advanced light field manipulation through ultrathin metasurfaces.     

太赫兹波前调制超表面器件研究进展

超表面是一种由人工微结构组成的超薄平面器件,能够实现对电磁波振幅、相位以及偏振态的调控,具有体积小、重量轻、集成度高、可灵活操控电磁波等优势,在电磁波谱、波前调制中发挥着巨大的作用。综述了近年来基于超表面的太赫兹波前调制器件的研究进展。总结了基于Pancharatnam-Berry相位、基于局域表面等离子体共振(LSPR)、基于Mie共振的三种超表面单元结构对电磁波的振幅、相位调控机理,并讨论了实现高效率超表面的方法。之后,介绍了用于设计波前调制超表面器件的纯相位调制方法和复振幅调制方法。综述了在太赫兹波段典型的超表面波前调制器,包括单一功能、复合功能以及可调谐功能的超表面波前调制器件。在早期的研究工作中,设计的超表面可实现波束偏转、波束聚焦、全息成像、以及涡旋光束、自聚焦光束、洛伦兹光束等特殊光束产生等功能。为提高太赫兹器件的利用率,波分复用、偏振复用等功能复用的太赫兹超表面器件被提出。随着对太赫兹波前动态调控需求的增长, 一些主动的太赫兹超表面器件被提出并在实验上被验证。共有两种主动的超表面器件。其中一种主动超表面是通过将超表面结构与半导体材料或相变材料结合形成的,另一种是通过光泵浦硅片形成的全光器件。全光超表面在不用重新加工的前提下能够被重复使用。通过调整投影在硅片上的超表面图像即可动态操控太赫兹波前。全光超表面具有动态控制波束扫描和波束聚焦的能力,将来可应用于太赫兹通信、太赫兹雷达等领域。最后,对太赫兹波前调制超表面器件的发展趋势与应用前景进行了展望。     

Flexible Plasmonic Metasurfaces with User‐Designed Patterns for Molecular Sensing and Cryptography

Flexible plasmonic metasurfaces have garnered considerable attention because the material's mechanical flexibility enables new functionalities and integrated applications. Here, by adopting low‐cost materials and simple techniques, we demonstrate a method of fabricating large flexible metasurfaces with arbitrary user‐designed iridescent patterns. These naked‐eye recognizable patterns together with their excellent plasmonic activities have yielded new functionalities and novel applications. Demonstrations include plasmonic sensing, reflective displays, developing new encryption strategies and integrated devices, etc. Moreover, the low fabrication cost (?2) would enable the practical use of the material. The metasurface can even be fashioned into an innovative, multifunctional medical ID bracelet. We believe our flexible plasmonic metafilm will inspire the fabrication of many novel applications and open up new horizons in various fields.     

新型功能超颖表面波前调制技术的发展与应用(特邀)

超颖表面作为一类智能表面,通常由特殊设计、加工而得到的特征尺寸接近或小于波长的亚波长纳米天线阵列构成。超颖表面能够实现光场的振幅、相位和偏振的人为调控,具有超薄、超小像素、宽带、低损耗、易加工等优势,设计灵活,功能强大。文中针对超颖表面在全息显示、波前调制和偏振转换、主动可调、非线性波前调控等方向进行综述,并展望未来发展趋势。超颖表面作为一种超薄的、微型化的波前调制器件,具有极大的信息容量,且更能适应未来高度集成的微型光电系统的发展要求,在全息显示、光束整形、涡旋光束的产生、数据存储、加密与防伪、超透镜与色散控制、彩色印刷、非对称传输、非线性光学、光的自旋霍尔效应、光通信与集成光电子学等应用领域提供了潜在的可行性和新的视角,有望取代传统光电器件,展现出了广阔的发展前景。     

Decahedral-shaped Au nanoparticles as plasmonic centers for high performance polymer solar cells

The photon harvesting of the photoactive layer within a multilayered polymer solar cells (PSCs) greatly affects the output electric power of the devices. For PSCs, the device performance is very sensitive to the photoactive layer thickness. Therefore, how to enhance the light absorption of the photoactive film with fixed thickness is still a big challenge. Plasmonic enhancement induced by noble metal nanoparticles has been proved to be an effective way to enhance light trapping inside the photoactive film without increasing the thickness of film. By incorporating Au decahedra into the poly(3,4-ethylenedioxythiophene): poly(4-styrenesulfonate) (PEDOT:PSS) anode buffer layer, high performance plasmonic PSCs based on P3HT:PC₆₀BM and PBDT-TS1:PC₇₀BM were fabricated and the light response of the PSCs are greatly improved in a broadband wavelength, resulting in a remarkable enhancement in short-circuit current density. The calculation results of finite difference time domain (FDTD) confirm that the plasmonic effects induce enhancement in device performance. Upon optimization, the best power conversion efficiency (PCE) of the device based on P3HT:PC₆₀BM and PBDT-TS1:PC₇₀BM reaches 4.14% and 10.29%, respectively, among the best values reported in literature. These results can provide valuable guidelines for the design of metal nanostructures for organic photovoltaic applications.     

圆极化复用型多功能超构表面研究进展

文中回顾并总结了课题组近期关于圆极化复用型多功能超构表面的研究进展. 从几何相位在正交圆极化波作用下的共轭对称响应出发,基于超构表面的等效琼斯矩阵提出了交叉极化双通道复用的独立调控方法,突破了几何相位的交叉极化耦合限制. 进一步,基于同极化与交叉极化分量间的幅相关系,提出了三通道复用的多元波前集成方法,实现了对透射圆极化电磁能量的全场调控. 在此基础上,通过引入手性诱导相位提出了圆极化四（全）通道复用的波前调控方法,有效提高了对圆极化电磁能量的利用效率,为提高现代通信系统信道容量及信息传输速率打下理论基础.     

基于电介质超表面的光场复振幅调制及应用

超表面作为一种人工设计的二维阵列纳米结构,能够在亚波长尺度上实现光场波前振幅、相位和偏振态的灵活调控,为现代光学器件的小型化、集成化提供了全新的实现途径。随着光学成像、显示等应用的发展,在可见光波段具有高工作效率的微型光学器件的需求日益凸显。近年来,由高折射率、低损耗电介质材料制备的光学超表面得到了极大地发展,在消色差光学超透镜、偏振相关全息显示等方面展现出广泛的应用前景。文中围绕电介质超表面的相关研究,首先介绍广义斯涅耳定律及电介质超表面结构调控光场振幅、相位和偏振态的基本原理,在此基础上,重点回顾近年来关于光场波前单一参量调控和多参量联合调控在全息显示、结构光场产生等方面的研究进展,最后讨论电介质超表面发展的可能挑战与前景。     

多维度超表面及其在信息加密防伪上的应用

超表面是一种厚度在亚波长或波长量级的人工层状材料。可通过调控超表面单元结构上的大小、形状、转角、位移量等自由度，实现对电磁波频率、振幅、相位、偏振等特性的灵活有效调控。超表面具有超薄、宽带、低损耗、易加工、灵活设计，功能强大等特点。文中综述了具有单维度、双维度、多维度光场调控功能的超表面及其在外部激励作用下具有主动可调特性超表面的发展历程，并特别介绍了这些超表面用于信息加密防伪领域的实现方式与优势特点。相比于传统的信息加密防伪技术，超表面信息加密防伪术具有亚波长像素，精密控制，安全系数高等特点，展现了全新视角，拥有广阔的发展前景。     

Efficiency Enhancement of Organic Solar Cells by Using Shape‐Dependent Broadband Plasmonic Absorption in Metallic Nanoparticles

It is been widely reported that plasmonic effects in metallic nanomaterials can enhance light trapping in organix solar cells (OSCs). However, typical nanoparticles (NP) of high quality (i.e., mono‐dispersive) only possess a single resonant absorption peak, which inevitably limits the power conversion efficiency (PCE) enhancement to a narrow spectral range. Broadband plasmonic absorption is obviously highly desirable. In this paper, a combination of Ag nanomaterials of different shapes, including nanoparticles and nanoprisms, is proposed for this purpose. The nanomaterials are synthesized using a simple wet chemical method. Theoretical and experimental studies show that the origin of the observed PCE enhancement is the simultaneous excitation of many plasmonic low‐ and high‐order resonances modes, which are material‐, shape‐, size‐, and polarization‐dependent. Particularly for the Ag nanoprisms studied here, the high‐order resonances result in higher contribution than low‐order resonances to the absorption enhancement of OSCs through an improved overlap with the active material absorption spectrum. With the incorporation of the mixed nanomaterials into the active layer, a wide‐band absorption improvement is demonstrated and the short‐circuit photocurrent density (J_sc) improves by 17.91%. Finally, PCE is enhanced by 19.44% as compared to pre‐optimized control OSCs. These results suggest a new approach to achieve higher overall enhancement through improving broadband absorption.     

Laser-Empowered Random Metasurfaces for White Light Printed Image Multiplexing

Printed image multiplexing based on the design of metasurfaces has attracted much interest in the past decade. Optical switching between different images displayed directly on the metasurface is performed by altering the parameters of the incident light such as polarization, wavelength, or incidence angle. When using white light, only two-image multiplexing is implemented with polarization switching. Such metasurfaces are made of nanostructures perfectly controlled individually, which provide high-resolution pixels but small images and involve long fabrication processes. Here, it is demonstrated that laser processing of nanocomposites offers a versatile low-cost, high-speed method with large area processing capabilities for controlling the statistical properties of random metasurfaces, allowing up to three-image multiplexing under white light illumination. By independently controlling absorption and interference effects, colors in reflection and transmission can be varied independently yielding two-image multiplexing under white light. Using anisotropy of plasmonic nanoparticles, a third image can be multiplexed and revealed through polarization changes. The design strategy, the fundamental properties, and the versatility of implementation of these laser-empowered random metasurfaces are discussed. The technique, applied on flexible substrate, can find applications in information encryption or functional switchable optical devices, and offers many advantages for visual security and anticounterfeiting.     

Hybrid Metasurfaces of Plasmonic Lattices and 2D Materials

Plasmonic metasurfaces can significantly enhance the interaction between light and 2D materials. Hybrid structures of plasmonic lattices and 2D materials show great promise for both fundamental and practical studies because of their unprecedented ability for precise manipulation of light at the nanoscale. This review starts with an overview of the basic concepts of plasmonic lattices and optical properties of 2D materials, as well as fabrication strategies for hybrid metasurfaces. Then, the enhanced photoluminescence, quantum emission, optoelectronic detection, nonlinear process, and valleytronics in hybrid metasurfaces are summarized, and their development for nanophotonic functional devices are reviewed. Further, several compelling topics are also outlined that provide outlooks for future directions of hybrid metasurfaces such as novel structural design and high-quality fabrication, all-dielectric metasurfaces, dynamic metasurfaces, and plasmonic mediation of chemical reactions and physical processes. It is believed that hybrid metasurfaces of plasmonic lattices and 2D materials can open prospects for versatile platforms for light-matter interactions and contribute to the revolutions on nanophotonic devices.     

Nonvolatile Reconfigurable Phase‐Change Metadevices for Beam Steering in the Near Infrared

The development of flat, compact beam‐steering devices with no bulky moving parts is opening up a new route to a variety of exciting applications, such as LIDAR scanning systems for autonomous vehicles, robotics and sensing, free‐space, and even surface wave optical signal coupling. In this paper, the design, fabrication and characterization of innovative, nonvolatile, and reconfigurable beam‐steering metadevices enabled by a combination of optical metasurfaces and chalcogenide phase‐change materials is reported. The metadevices reflect an incident optical beam in a mirror‐like fashion when the phase‐change layer is in the crystalline state, but reflect anomalously at predesigned angles when the phase‐change layer is switched into its amorphous state. Experimental angle‐resolved spectrometry measurements verify that fabricated devices perform as designed, with high efficiencies, up to 40%, when operating at 1550 nm. Laser‐induced crystallization and reamorphization experiments confirm reversible switching of the device. It is believed that reconfigurable phase‐change‐based beam‐steering and beam‐shaping metadevices, such as those reported here, can offer real applications advantages, such as high efficiency, compactness, fast switching times and, due to the nonvolatile nature of chalcogenide phase‐change materials, low power consumption.     

High‐Temperature Large‐Scale Self‐Assembly of Highly Faceted Monocrystalline Au Metasurfaces

Localized surface plasmon resonance (LSPR) devices based on resonant metallic metasurfaces have shown disruptive potential for many applications including biosensing and photocatalysis. Despite significant progress, highly performing Au plasmonic nanotextures often suffer of suboptimal electric field enhancement, due to damping effects in multicrystalline domains. Fabricating well‐defined Au nanocrystals over large surfaces is very challenging, and usually requires time‐intensive multi‐step processes. Here, presented are first insights on the large‐scale self‐assembly of monocrystalline Au nano‐islands with tunable size and separation, and their application as efficient LSPR surfaces. Highly homogeneous centimeter‐sized Au metasurfaces are fabricated by one‐step deposition and in situ coalescence of hot nanoparticle aerosols into a discontinuous monolayer of highly faceted monocrystals. First insights on the mechanisms driving the high‐temperature synthesis of these highly faceted Au nanotextures are obtained by molecular dynamic and detailed experimental investigation of their growth kinetics. Notably, these metasurfaces demonstrat high‐quality and tunable LSPR, enabling the fabrication of highly performing optical gas molecule sensors detecting down to 3 × 10^?6 variations in refractive index at room temperature. It is believed that these findings provide a rapid, low‐cost nanofabrication tool for the engineering of highly homogenous Au metasurfaces for large‐scale LSPR devices with application ranging from ultrasensitive optical gas sensors to photocatalytic macroreactors.     

Smart Nanostructured Materials based on Self‐Assembly of Block Copolymers

Nanoscale fabrication of smart materials relying on the molecular self‐assembly of block copolymers (BCPs) has been recognized as a valuable platform for various next‐generation functional structures. In this Progress Report, the recent advances in the BCP self‐assembly process, which has paved the way for viable applications of emerging nanotechnologies, are highlighted. Effective light‐induced self‐assembly based on photothermal annealing of high‐χ BCPs and conformal 3D surface nanopatterning exploiting chemically modified graphene flexible substrates are reviewed as the typical instances of advanced BCP‐based nanofabrication methodologies. Additionally, relevant potential application fields are suggested, namely, graphene nanoribbon field effect transistors, highly tunable refractive index metasurfaces for visible light, high‐sensitivity surface‐enhanced Raman spectroscopy, 2D transition metal dichalcogenide nanopatterning, sequential infiltration synthesis, and organic photovoltaics. Finally, the future research direction as well as innovative applications of these smart nanostructured materials is proposed.     

Highly Stable Plasmon Induced Hot Hole Transfer into Silicon via a SrTiO3 Passivation Interface

Extracting plasmon‐induced hot carriers over a metal–semiconductor Schottky barrier enables photodetection below the semiconductor bandgap energy. However, interfacial carrier recombination hinders the efficiency and stability of this process, severely limiting its implementation in telecommunication. This study proposes and demonstrates the use of epitaxially grown lattice‐matched SrTiO₃ for interfacial passivation of silicon‐based plasmonic Schottky devices. The devices are activated by an electrical soft‐breakdown of the interfacial SrTiO₃ layer, resulting in reproducible rectified Schottky characteristics. The transition to a low resistance state of the SrTiO₃ layer boosts the extraction efficiency of hot holes upon resonant plasmonic excitation, giving rise to a two orders of magnitude higher photocurrent compared to devices with a native oxide layer. Photoresponse, tunability, and barrier height studies under reverse biases as high as 100 V present superior stability with the incorporation of the SrTiO₃ layer. The investigation paves the way toward plasmon‐induced photodetection for practical applications including those under challenging operating conditions.     

Plasmonic Au nanoparticles for enhanced broadband light absorption in inverted organic photovoltaic devices by plasma assisted physical vapour deposition

We use a low vacuum plasma assisted physical vapour deposition (PAPVD) method to deposit a Au nanoparticles (NPs) thin film onto the poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) layer in inverted poly(3-hexylthiophene):[6,6]-phenyl C61-butyric acid methylester (P3HT:PCBM) organic photovoltaic (OPV) devices. The Au NPs that incorporated into the PEDOT:PSS layer and reached to the active P3HT:PCBM layer can provide significant plasmonic broadband light absorption enhancement to the active layer. An approximately 50–90% improvement in short-circuit current density and in power convention efficiency has been achieved compared with those OPV devices without the plasmonic light absorption enhancement. This technique can be adopted and easily fit into most OPV device fabrication processes without changing other layers’ processing methods, morphologies, and properties.