High Signal Reproducibility Research Articles

A novel controllable nanocyclic plasma coupled array in SERS trace detection of multi-component pollutants

The development and design of a novel, uniform and highly active local electromagnetic field enhanced structure is crucial for expanding Surface-enhanced Raman Scattering (SERS) applications. In this study, we developed Ag ring-coupled nanoarrays (Ag RCNAs) with controllable nanogaps using a substrate rotary evaporation coating technique with self-assembled polystyrene (PS) microspheres as templates. This straightforward and cost-effective method efficiently prepares plasma-coupled nanoarrays. Ag RCNAs demonstrated high sensitivity in detecting organic dyes, our prepared Ag RCNAs showed high sensitivity (with the limit of detection of 10−8 M), high signal reproducibility (with the relative standard deviation of 6.73 %). Furthermore, Ag RCNAs showed remarkable sensitivity to a broad spectrum of dyes in river water, indicating the large-area uniform and highly active circular-ring-shaped nanogaps can realize highly sensitive detection of various pollutants. This approach offers advantages in electromagnetic field enhancement, tunable nanogaps, uniformity, reproducibility, and recyclability, making it promising for applications in environmental monitoring, bioassays, food safety, and medical diagnostics.

SERS detection of dopamine in artificial cerebrospinal fluid and in Parkinson’s disease-induced mouse cortex using a hybrid ZnO@Ag nanostructured platform

Rapid, direct, and sensitive detection of metabolites or clinically relevant biomarkers in complex biological samples is still challenging. We report a label-free surface-enhanced Raman scattering (SERS)-based approach for highly sensitive detection of dopamine (DA) in artificial cerebrospinal fluid (aCSF) and mouse brain tissue samples. The hybrid SERS-active sensing platform was designed to maximize the hot spot distribution. It encompasses a network of flexible and polymeric nanotrenches and nanogaps fabricated by nanoimprint lithography (NIL) covered by thin films of zinc oxide (ZnO) and silver (Ag) deposited using pulsed laser deposition (PLD) and direct current magnetron sputtering (DC-MS), respectively. The growth of the ZnO and Ag thin films was assessed by scanning electron microscopy (SEM) technique. The proposed SERS substrate benefits from the interlayered semiconductor–metal contribution in SERS enhancement, leading to a versatile sensing platform with improved detection sensitivity through the increased hot spots distribution. Using this strategy, the proposed assay can achieve an ultralow DA determination at the nM level, a short testing time (<30 min), and high signal reproducibility (RSD 11 %). We also assessed the sensing attributes of our in house developed SERS platform to detect DA in spiked aCSF samples, and a limit of detection (LOD) of 10 μM was achieved. Additionally, after in vivo inducing Parkinson’s disease (PD) in mice, relevant biological samples (striatum and cortical brain tissue) were investigated by SERS and ELISA. Given its good stability and accuracy in complex samples, the SERS-ELISA analysis has great potential to be a powerful tool for the reliable detection of DA in remote conditions.

Sample-Specific MS/MS Methods in High-Throughput Mass Spectrometry.

The drug discovery process increasingly relies on high-throughput sample analysis to accelerate the identification of viable drug candidates. Recently, chromatographic-free high-throughput mass spectrometry (HT-MS) technologies have emerged, significantly increasing sample readout speed and enabling the analysis of large sample sets. These HT-MS platforms continuously acquire data from various samples into a single data file, presenting challenges in applying distinctive data acquisition methods to specific samples. This study introduces a novel approach that integrates real-time sample loading status to activate sample-specific MS/MS data acquisition methods on the high-throughput acoustic ejection mass spectrometry platform. Effective method switching and high signal reproducibility were demonstrated across different data acquisition window durations in multiple reaction monitoring (MRM), high-resolution MRM (MRMHR), and information-dependent acquisition modes. This advancement provides a user-friendly and robust solution to the method-setting challenges of HT-MS, expanding the implementation of HT-MS platforms in drug discovery and other high-throughput analytical applications.

Tailorable janus plasmonic SERS platform with hotspots integrating and analytes enriching property for multiple sensing

Electromagnetic hotspot engineering plays a crucial role in surface-enhanced Raman scattering (SERS) biosensors. However, the construction of optical hotspots with high density and the concentration of analytes into hotspot centers remain challenging tasks. Additionally, achieving high sensitivity and signal reproducibility in SERS biosensors is an ongoing challenge. In this study, we utilise Janus micro/nano arrays to develop a superhydrophobic SERS platform. The high roughness of these arrays facilitates the distribution of rich hotspots ranging from nano to microscale and encourages the concentration of analytes within hotspot centers. The Janus plasmonic micro/nano arrays were meticulously crafted through the synergy of site-specific growth and instant interfacial assembly of nanoparticles (NPs). In the realm of SERS measurements targeting organic dyes in river water, our sensing platform demonstrates high sensitivity (limit of detection (LOD): 10−9 M) and signal reproducibility (relative standard deviation (RSD)=4.25%). Furthermore, the SERS platform exhibited remarkable sensitivity to multiple dyes in river water. Thus, our superhydrophobic SERS platform lays the groundwork for sensitive analysis in diverse fields such as environmental analysis and healthcare monitoring.

High-Throughput Acoustic Ejection Mass Spectrometry with Adjustable Signal Durations.

High-throughput mass spectrometry (MS) has witnessed rapid advancements and has found extensive applications across various disciplines. It enables the fast and accurate analysis of large sample sets, delivering a 10-fold or greater enhancement in analytical throughput when compared to conventional LC-MS methods. However, the signal duration in these high-throughput MS technologies is typically confined to a narrow range, presenting challenges for workflows demanding prolonged signal durations. In this study, we introduce a method that enables precise modulation of the signal duration on an acoustic ejection mass spectrometry (AEMS) system while ensuring high signal reproducibility. This flexibility allows for simultaneous and precise analysis of a significantly greater number of MS/MS transitions in high-throughput MS environments. Additionally, it offers a unique approach for parameter optimization and method development with minimal sample volume requirements. This advancement enhances the efficiency of MS-based analyses across diverse applications and facilitates broader utilization of MS technologies in high-throughput settings, including data-dependent acquisition (DDA) and data-independent acquisition (DIA).

Multiwavelength SERS of Magneto-Plasmonic Nanoparticles Obtained by Combined Laser Ablation and Solvothermal Methods.

The present study introduces a novel method for the synthesis of magneto-plasmonic nanoparticles (MPNPs) with enhanced functionality for surface-enhanced Raman scattering (SERS) applications. By employing pulsed laser ablation in liquid (PLAL) to synthesize plasmonic nanoparticles and wet chemistry to synthesize magnetic nanoparticles, we successfully fabricated chemically pure hybrid Fe3O4@Au and Fe3O4@Ag nanoparticles. We demonstrated a straightforward approach of an electrostatic attachment of the plasmonic and magnetic parts using positively charged polyethylenimine. The MPNPs displayed high SERS sensitivity and reproducibility, and the magnetic part allowed for the controlled separation of the nanoparticles from the reaction mixture, their subsequent concentration, and their precise deposition onto a specified surface area. Additionally, we fabricated alloy based MPNPs from AgxAu100-x (x = 50 and 80 wt %) targets with distinct localized surface plasmon resonance (LSPR) wavelengths. The compositions, morphologies, and optical properties of the nanoparticles were characterized by using transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray diffraction (XRD), UV-vis spectroscopy, and multiwavelength Raman spectroscopy. A standard SERS marker, 4-mercaptobenzoic acid (4-MBA), validated the enhancement properties of the MPNPs and found an enhancement factor of 2 × 108 for the Fe3O4@Ag nanoparticles at 633 nm excitation. Lastly, we applied MPNP-enhanced Raman spectroscopy for the analysis of the biologically relevant molecule adenine and found a limit of detection of 10-7 M at 785 nm excitation. The integration of PLAL and wet chemical methods enabled the relatively fast and cost-effective production of MPNPs characterized by high SERS sensitivity and signal reproducibility that are required in various fields, including biomedicine, food safety, materials science, security, and defense.

Flexible, foldable and transparent SERS film with high sensitivity and signal homogeneity via silver ion exchange and in-situ reduction

The adhesion between metal plasma and substrate was the key of surface-enhanced Raman scattering (SERS) technology. The preparation of ideal SERS substrate with multiple advantages such as high sensitivity and good signal reproducibility was still the focus of research. A flexible foldable and transparent fluorinated polyimide/silver NPs (FPI@Ag) SERS film was fabricated by the ion exchange and in-situ reduction method in this work. The effects of KOH hydrolysis time, AgNO3 ion exchange time and concentration, the type and concentration of reducing agents on the SERS performance of the FPI@Ag film were systematically discussed. As a result, the hydrolysis time of KOH affected the thickness of the metallic silver layer, the concentration of AgNO3 affected the size and spacing of Ag NPs, and the Raman signal of was remarkably enhanced when borane dimethylamine complex (DMAB) was used as reducing agent. When the detection limit of 4-Aminothiophenol was as low as 1 × 10−11 mol·L−1, the obvious Raman characteristic peak still appeared. The enhancement factor (EF) was up to 9.4 × 107. The linear quantification range was achieved in the range from 10−3–10−11 mol·L−1, R2 = 0.9987. In addition, we also performed multi-cycle bending and torsion test on the FPI@Ag film, and obtained stable Raman signals. The prepared FPI@Ag film can be attached to the surface of uneven samples, which can be used for on-site Raman detection and analysis.

Paper-based 3D SERS immunoassay array based on self-assembly of AuNBPs@Ag nanorods for ultrasensitive and highly stable detection of α-fetoprotein

Establishing a simple, sensitive, and accurate α-fetoprotein (AFP) detection methods is of great significance for the early diagnosis of hepatocellular carcinoma (HCC). Surface-enhanced Raman spectroscopy (SERS) has been identified as one of the most promising techniques for clinical monitoring. However, accurate detection of AFP is still challenging due to the poor stability of SERS substrate and the low abundance of AFP in the early stages of HCC. Herein, we developed an ultrasensitive and highly stable paper-based 3D SERS immunoassay array for AFP detection, combining the superior advantages of self-assembled AuNBPs@Ag nanorods, filter paper, and sandwich immunoassay. In the immunoassay array, 4-mercaptobenzoic acid (4-MBA) linked to the secondary antibody was employed as the Raman reporter, while the array modified with antibodies was used to capture AFP. The SERS immunoassay array sensor exhibited a wide linear range (3 pg mL−1 to 10 µg mL−1), low detection limit (0.086 pg mL−1), good specificity, and high signal reproducibility (RSD < 5 %). Meanwhile, the sensor is further used for accurate detection of trace AFP in serum, which paves an avenue for the fabrication of SERS substrates with high stability and provides a new outlook for their application in the early diagnosis of cancer.

Optical bi-enzyme-titania biosensor system: A new way to detect lactose

Lactose concentration is a key parameter for assessing the quality of raw and processed milk and identifying abnormal milk. Current methods for lactose determination are laborious, time-consuming and oftentimes require skilled lab workers, expensive equipment, and special reagents. In this study, an optical biosensor system based on nanosized titanium dioxide (TiO2) is presented for routine measurement of lactose in milk without sample preparation. TiO2 was obtained via sol-gel synthesis and characterized using dynamic light scattering, microelectrophoresis, X-ray diffraction, transmission electron microscopy, and nitrogen adsorption-desorption analysis. The system, whose colorimetric response was based on the chromogen-free TiO2-based detection of hydrogen peroxide (H2O2), used β-galactosidase and/or glucose oxidase as the biorecognition elements. The selectivity and sensitivity of the biosensors for lactose and glucose was investigated by diffuse reflectance spectroscopy using standard aqueous lactose and glucose solutions and whole milk samples. The results showed that the proposed biosensors had high optical signal reproducibility (RSD = 5–6%), high sensitivity (LOD = 0.005 wt%), and high selectivity. The linear dynamic ranges of lactose and glucose detection were from 0.005 wt% to 0.100 wt%, and the optimal response time of the biosensor was 25 min. The listed features and advantages of label-free detection make the biosensor attractive for simple, inexpensive, sensitive, and selective determination of lactose in milk.

Microplotter Printing of Hierarchically Organized NiCo2O4 Films for Ethanol Gas Sensing

Using a combination of chemical coprecipitation and hydrothermal treatment of the resulting dispersed system, a hierarchically organized NiCo2O4 nanopowder was obtained, consisting of slightly elongated initial oxide nanoparticles self-organized into nanosheets about 10 nm thick, which in turn are combined into hierarchical cellular agglomerates of about 2 μm. Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction analysis (XRD), selected area electron diffraction (SAED) and high-resolution transmission electron microscopy (HR-TEM) allowed to confirm the formation of NiCo2O4 powder with the desired crystal structure via additional heat treatment of the intermediate product. Energy-dispersive X-ray spectroscopy (EDX) was used to confirm the target metal ratio, and the uniform distribution of the elements (Ni, Co and O) was shown by mapping. The resulting nanopowder was employed to prepare functional inks suitable for microplotter printing of the NiCo2O4 film. It was found that an oxide film morphology is fully inherited from the hierarchically organized oxide nanopowder used. Atomic force microscopy (AFM) revealed the film thickness (15 μm) and determined the maximum height difference of 500 nm over an area of 25 μm2. Kelvin probe force microscopy (KPFM) showed that the surface potential was shifted to the depths of the oxide film, and the work function value of the material surface was 4.54 eV, which is significantly lower compared to those reported in the literature. The electronic state of the elements in the NiCo2O4 film under study was analyzed by X-ray photoelectron spectroscopy (XPS). Chemosensor measurements showed that the printed receptor layer exhibited selectivity and high signal reproducibility for ethanol detection. As the relative humidity increases from 0 to 75%, the response value is reduced; however, the sensor response profile and signal-to-noise ratio remain without significant changes.

A Metallic Niobium Nitride with Open Nanocavities for Surface-Enhanced Raman Spectroscopy.

The construction of open hot-spot structures that facilitate the entry of analytes is crucial for surface-enhanced Raman spectroscopy. Here, metallic niobium nitride (NbN) three-dimensional (3D) hierarchical networks with open nanocavity structure are first found to exhibit a strong visible-light localized surface plasmon resonance (LSPR) effect and extraordinary surface-enhanced Raman scattering (SERS) performance. The unique nanocavity structure allows easy entry of molecules, promoting the utilization of electromagnetic hot spots. The NbN substrate has a lowest detection limit of 1.0 × 10-12 M and a Raman enhancement factor (EF) of 1.4 × 108 for contaminants. Furthermore, the NbN hierarchical networks possess outstanding environmental durability, high signal reproducibility, and detection universality. The remarkable SERS sensitivity of the NbN substrate can be attributed to the joint effect of LSPR and interfacial charge transport (CT).

Top-Down Rational Engineering of Heteroatom-Doped Graphene Quantum Dots for Laser Desorption/Ionization Mass Spectrometry Detection and Imaging of Small Biomolecules.

Matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI MSI) is widely applied in mapping macrobiomolecules in tissues, but it is still limited in profiling low-molecular-weight (MW) compounds (typically metabolites) due to ion interference and suppression by organic matrices. Here, we present a versatile "top-down" strategy for rational engineering of carbon material-based matrices, by which heteroatom-doped graphene quantum dots (HGQDs) were manufactured for LDI MS detection and imaging of small biomolecules. The HGQDs derived from parent materials inherited the π-conjugated networks and doping sites for promoting energy transfer and negative ion generation, while their extremely small size guaranteed the matrix uniformity and signal reproducibility in LDI MSI. Compared to other HGQDs, nitrogen-doped graphene quantum dots (NGQDs) exhibited superior capability of assisting LDI of various small molecules, including amino acids, fatty acids, saccharides, small peptides, nucleobases, anticancer drugs, and bisphenol pollutants. Density functional theory simulations also corroborated that the LDI efficiency was markedly raised by the proton-capturing pyridinic nitrogen species and compromised by the electron-deficient boron dopants. NGQDs-assisted LDI MS further enabled label-free investigation on enzyme kinetics using an ordinary short peptide as the substrate. Moreover, due to the high salt tolerance and signal reproducibility, the proposed negative-ion NGQDs-assisted LDI MSI was able to reveal the abundance and distribution of low-MW species in rat brain tissue and achieved the imaging of low-MW lipids in coronally sectioned rat brains subjected to traumatic brain injury. Our work offers a new route for customizing nanomaterial matrices toward LDI MSI of small biomolecules in biomedical and pathological research.

Ni Nanoparticles Embedded Ti3C2Tx-MXene Nanoarchitectures for Electrochemical Sensing of Methylmalonic Acid.

MXenes-Ti3C2Tx, based on their versatile surface characteristics, has rapidly advanced as an interactive substrate to develop electrochemical sensors for clinical applications. Herein, Ni embedded Ti3C2Tx (MX−Ni) composites were prepared using a self-assembly approach where Ti3C2Tx sheets served as an interactive conductive substrate as well as a protective layer to nickel nanoparticles (Ni NPs), preventing their surface oxidation and aggregation. The composite displayed a cluster-like morphology with an intimate interfacial arrangement between Ni, Ti3C2Tx and Ti3C2Tx-derived TiO2. The configuration of MX−Ni into an electrochemical sensor realized a robust cathodic reduction current against methylmalonic acid (MMA), a biomarker to vitamin B12 deficiency. The synergism of Ni NPs strong redox characteristics with conductive Ti3C2Tx enabled sensitive signal output in wide detection ranges of 0.001 to 0.003 µM and 0.0035 to 0.017 µM and a detection sensitivity down to 0.12 pM of MMA. Importantly, the sensor demonstrated high signal reproducibility and excellent operational capabilities for MMA in a complex biological matrix such as human urine samples.

ZIF-8 derived TiO2/ZnO heterostructure decorated with AgNPs as SERS sensor for sensitive identification of trace pesticides

Pesticides are still abused and overused in agricultural production. Food safety monitoring in terms of reliable detection and quantification of pesticide residues is an ever increasing need. Surface-Enhanced Raman Scattering (SERS)-based chemical sensors and adsorption materials crafted for specific pesticide should provide high sensitivity and selectivity. Herein, zeolitic imidazolate framework (ZIF-8) derived TiO2/ZnO three-dimensional (3D) heterostructures were constructed on FTO substrate and were utilized to assemble silver nanoparticles (AgNPs) to create electromagnetic hot spots. The formation of TiO2/ZnO heterostructure greatly improve the SERS performance of the substrate. The calculated enhancement factor (EF) of the TiO2/ZnO/Ag is 39-fold higher than the TiO2/Ag substrates. Furthermore, the substrate shows high signal sensitivity and reproducibility for rapid detection of multiple pesticides. Even with a portable Raman device, the substrate was found to be highly efficient for model molecules of crystal violet (CV) and 4-mercaptobenzoic acid (4-MBA), and the limit of detection (LOD) for both of 10−9 M was demonstrated. Importantly, real life detection of multiple pesticides residues can be achieved with the TiO2/ZnO/Ag sensor, which was demonstrated by the detection of three common pesticides, thiram, acephate and phoxim at trace concentrations.

Optically active plasmonic cellulose fibers based on Au nanorods for SERS applications

Cellulose might be a promising material for surface-enhanced Raman scattering (SERS) substrates due to its wide availability, low cost, ease of fabrication, high flexibility and low optical activity. This work shows, for the first time development of the cellulose-based substrate, that owes its SERS activity to the presence of gold nanorods in its internal structure, and not only on the surface, as it is shown elsewhere, thus ensuring superior stability of the obtained material. This flexible cellulose-based substrate exhibiting plasmonic activity, provide easy and reproducible detection of different analytes via SERS technique. The substrate was prepared by introduction of gold nanorods into the cellulose fibers matrix using an eco-friendly process based on N-Methylmorpholine-N-Oxide. Au-modified cellulose fibers were used for the detection of p-Mercaptobenzoic acid and Bovine Serum Albumin by the SERS method. The obtained results show that this substrate offers large signal enhancement of 6-orders of magnitude, and high signal reproducibility with a relative standard deviation of 8.3%. Additionally, washing tests (90 °C, 20 h) showed superior stability of the as prepared plasmonic fibers, thus proving the good reusability of the substrates and the long shelf life.

Modification of electrodes with self-assembled, close-packed AuNPs for improved signal reproducibility toward electrochemical detection of dopamine

Electrochemical sensors benefit from low cost and fast detection speeds, which makes them suitable for routine analysis of small biological molecules such as dopamine (DA). DA is a neurotransmitter that plays an important physiological role and can be used as a marker for conditions such as depressive disorder and Parkinson’s disease. In this communication, electrodes modified with self-assembled gold nanoparticles (SA-AuNPs) were used as electrochemical sensors for the detection of DA with the aim of achieving better signal stability among the same batch of electrodes. High signal reproducibility among the SA-AuNP-modified electrodes was obtained due to the more orderly packing of AuNPs leading to relatively consistent electrochemical resistance and homogeneous mass transport.

Surface-enhanced Raman scattering with gold-coated silicon nanopillars arrays: The influence of size and spatial order

Nanopillars have been extensively explored as promising substrates for surface-enhanced Raman scattering (SERS) owing to their high sensitivity and excellent reproducibility. Most of the researches have been focused on the fabrication methods of nanopillars, and the dependences of SERS effects on geometrical size and spatial order are rarely investigated. In this work, SERS properties of nanopillars with different sizes (115–185 nm) and spatial orders (square and rhombus orders) have been studied. The work has shown that the nanopillars not only have high enhancement capability and high signal reproducibility, but also the enhancement is insensitive to the size and spatial orders. The measured enhancement factors (EFs) are 2.3–4.0 × 106 and signal reproducibility (relative standard deviation, RSD) are ∼ 5.2%–6.9%, which are among the best of the similar SERS substrates reported. The variation of SERS intensity was as low as approximately 4.8% with the variation of pillar size from 115, 135, 145, to 160 nm. The insensitiveness and high reproducibility have been ascribed to the combined excitation of localized surface plasmon resonance (LSPR) and propagating surface plasmons (SPPs) of the nanopillars. Optical properties of the nanopillars are studied both experimentally and numerically to understand the physics behind the SERS performance.

2D GaN for Highly Reproducible Surface Enhanced Raman Scattering.

Surface-enhanced Raman scattering (SERS) based on 2D semiconductors has been rapidly developed due to their chemical stability and molecule-specific SERS activity. High signal reproducibility is urgently required towards practical SERS applications. 2D gallium nitride (GaN) with highly polar Ga-N bonds enables strong dipole-dipole interactions with the probe molecules, and abundant DOS (density of states) near its Fermi level increases the intermolecular charge transfer probability, making it a suitable SERS substrate. Herein, 2D micrometer-sized GaN crystals are demonstrated to be sensitive SERS platforms with excellent signal reproducibility and stability. Strong dipole-dipole interaction between the dye molecule and 2D GaN enhances the molecular polarizability. Furthermore, 2D GaN benefits its SERS enhancement by the combination of increased DOS and more efficient charge transfer resonances when compared with its bulk counterpart.

Fabrication of Multifunctional SERS Platform Based on Ag NPs Self-Assembly Ag-AAO Nanoarray for Direct Determination of Pesticide Residues and Baicalein in Real Samples

Aiming at the shortcomings of high cost and time-consumption in traditional liquid chromatography, an effective surface enhanced Raman scattering (SERS)-based trace detection method has been proposed to quantitatively identify the active component of traditional Chinese medicine. In this paper, a high-performance and versatile SERS platform based on Ag nanoparticles (NPs) self-assembly Ag-anodized aluminium (Ag NPs-Ag-AAO) nanoarray was fabricated by controllable physico-chemical preparation technology. The results indicated that the electromagnetic field enhancement effect was sharply strengthened as Ag NPs assembled, and the experimental enhancement factor (EEF) value was calculated to be 1.0083 × 106. This novel Ag NPs-Ag-AAO nanoarray with substantial “hot spots” exhibited high SERS signal reproducibility, with the relative standard deviation (RSD) value at less than 2.23%. More importantly, this SERS platform was applied to detect active component Baicalein in Scutellaria baicalensis, and the limit of detection (LOD) was located at 10 fg/mL. Therefore, this Ag NPs-Ag-AAO nanoarray with high sensitivity, strong Raman signal reproducibility and reliable practicability has broad application prospects in the rapid detection of trace substances in the active components of traditional Chinese medicine and is expected to be popularized.

Web-above-a-Ring (WAR) and Web-above-a-Lens (WAL): Nanostructures for Highly Engineered Plasmonic-Field Tuning and SERS Enhancement.

Synthetic strategies of web-above-a-ring (WAR) and web-above-a-lens (WAL) nanostructures are reported. The WAR has a controllable gap between the nanoring core and a nanoweb with nanopores for the effective confinement of electromagnetic field in the nanogap and subsequent surface-enhanced Raman scattering (SERS) of Raman dyes inside the gap with high signal reproducibility, which are attributed to the generation of circular 3D hot zones along the rim of Pt@Au nanorings with wrapping nanoweb architecture. More specifically, Pt@Au nanorings are adopted as a plasmonic core for structural rigidity and built porous nanowebs above them through a controlled combination of galvanic exchange and the Kirkendall effect. Both nanoweb and nanolens structures are also formed on Pt@Au nanoring, which is WAL. structure. Remarkably, plasmonic hot zone, nanopores, and hot lens are formed inside a single WAL nanostructure, and these structural components are orchestrated to generate stronger SERS signals.