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Ultrasensitive SERS-Based Plasmonic Sensor with Analyte Enrichment System Produced by Direct Laser Writing
摘要： We report an easy-to-implement device for surface-enhanced Raman scattering (SERS)-based detection of various analytes dissolved in water droplets at trace concentrations. The device combines an analyte-enrichment system and SERS-active sensor site, both produced via inexpensive and high-performance direct femtosecond (fs)-laser printing. Fabricated on a surface of water-repellent polytetrafluoroethylene substrate as an arrangement of micropillars, the analyte-enrichment system supports evaporating water droplet in the Cassie–Baxter superhydrophobic state, thus ensuring delivery of the dissolved analyte molecules towards the hydrophilic SERS-active site. The efficient pre-concentration of the analyte onto the sensor site based on densely arranged spiky plasmonic nanotextures results in its subsequent label-free identification by means of SERS spectroscopy. Using the proposed device, we demonstrate reliable SERS-based fingerprinting of various analytes, including common organic dyes and medical drugs at ppb concentrations. The proposed device is believed to find applications in various areas, including label-free environmental monitoring, medical diagnostics, and forensics.
关键词： SERS,direct laser processing,femtosecond laser pulses,medical drugs,superhydrophobic textures,plasmonic nanostructures,analyte enrichment
更新于2025-09-16 10:30:52
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Addressing K/L-edge overlap in elemental analysis from micro-X-ray fluorescence: bioimaging of tungsten and zinc in bone tissue using synchrotron radiation and laser ablation inductively coupled plasma mass spectrometry
摘要： Synchrotron radiation micro-X-ray fluorescence (SR-μXRF) is a powerful elemental mapping technique that has been used to map tungsten and zinc distribution in bone tissue. However, the heterogeneity of the bone samples along with overlap of the tungsten L-edge with the zinc K-edge signals complicates SR-μXRF data analysis, introduces minor artefacts into the resulting element maps, and decreases image sensitivity and resolution. To confirm and more carefully delineate these SR-μXRF results, we have employed laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) to untangle the problem created by the K/L-edge overlap of the tungsten/zinc pair. While the overall elemental distribution results are consistent between the two techniques, LA-ICP-MS provides significantly higher sensitivity and image resolution compared with SR-μXRF measurements in bone. These improvements reveal tissue-specific distribution patterns of tungsten and zinc in bone, not observed using SR-μXRF. We conclude that probing elemental distribution in bone is best achieved using LA-ICP-MS, though SR-μXRF retains the advantage of being a non-destructive method with the capability of being paired with X-ray techniques, which determine speciation in situ. Since tungsten is an emerging contaminant recently found to accumulate in bone, accurately determining its distribution and speciation in situ is essential for directing toxicological studies and informing treatment regimes.
关键词： LA-ICP-MS,Overlap,X-ray spectroscopy (XPS | XRF | EDX),Analyte,Zinc,Tungsten
更新于2025-09-12 10:27:22
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Analyte transport to micro- and nano-plasmonic structures
摘要： The study of optical affinity biosensors based on plasmonic nanostructures has received significant attention in recent years. The sensing surfaces of these biosensors have complex architectures, often composed of localized regions of high sensitivity (electromagnetic hot spots) dispersed along a dielectric substrate having little to no sensitivity. Under conditions such that the sensitive regions are selectively functionalized and the remaining regions passivated, the rate of analyte capture (and thus the sensing performance) will have a strong dependence on the nanoplasmonic architecture. Outside of a few recent studies, there has been little discussion on how changes to a nanoplasmonic architecture will affect the rate of analyte transport. We recently proposed an analytical model to predict transport to such complex architectures; however, those results were based on numerical simulation and to date, have only been partially verified. In this study we measure the characteristics of analyte transport across a wide range of plasmonic structures, varying both in the composition of their base plasmonic element (microwires, nanodisks, and nanorods) and the packing density of such elements. We functionalized each structure with nucleic acid-based bioreceptors, where for each structure we used analyte/receptor sequences as to maintain a Damk?hler number close to unity. This method allows to extract both kinetic (in the form of association and dissociation constants) and analyte transport parameters (in the form of a mass transfer coefficient) from sensorgrams taken from each substrate. We show that, despite having large differences in optical characteristics, measured rates of analyte transport for all plasmonic structures match very well to predictions using our previously proposed model. These results highlight that, along with optical characteristics, analyte transport plays a large role in the overall sensing performance of a nanoplasmonic biosensor.
关键词： mass transfer coefficient,analyte transport,plasmonic nanostructures,nanoplasmonic architecture,optical affinity biosensors
更新于2025-09-12 10:27:22
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Quasi-D-Shaped Fiber Optic Plasmonic Biosensor for High-Index Analyte Detection
摘要： In this paper, we propose a highly sensitive quasi-D-shaped fiber optic biosensor for detection of high refractive index (RI) liquid analytes via surface plasmon resonance. The main mechanism of sensing is interplay between photonic crystal fiber fundamental mode and plasmonic mode which leads to formation of different resonance peaks depending on the analyte RI. We numerically analyze the structure sensitivity to design parameters and demonstrate the sensing performance of the proposed biosensor using both spectral sensitivity and amplitude sensitivity methods. The proposed biosensor has a RI detection range of 0.15 refractive index unit (RIU) from 1.45 to 1.6. The sensor exhibits linear sensing performance with a RI spectral sensitivity of 9300 nm/RIU for analyte RI ranging from 1.45 to 1.525, 1176 nm/RIU for analyte RI ranging from 1.525 to 1.6 and in particular, 11800 nm/RIU for analyte RI between 1.475 and 1.5. Furthermore, an average RI sensitivity of 4800 nm/RIU for analyte RI ranging from 1.45 to 1.6 is demonstrated. We also study the amplitude sensitivities of the proposed sensor which show promising maximum values of 183.6 RIU-1 for 785 nm excitation and 820 RIU-1 for 1050 nm excitation. Due to the simple structure of the proposed biosensor, large detection range, high sensitivity and promising linear sensing performance, the proposed biosensor can be a promising candidate for detecting various high RI chemical and biochemical samples.
关键词： plasmonic biosensor,photonic crystal fiber,high index analyte detection,Fiber optic sensor,refractive index sensing
更新于2025-09-11 14:15:04
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Designing surface-enhanced Raman scattering (SERS) platforms beyond hotspot engineering: emerging opportunities in analyte manipulations and hybrid materials
摘要： Surface-enhanced Raman scattering (SERS) is a molecule-specific spectroscopic technique with diverse applications in (bio)chemistry, clinical diagnosis and toxin sensing. While hotspot engineering has expedited SERS development, it is still challenging to detect molecules with no specific affinity to plasmonic surfaces. With the aim of improving detection performances, we venture beyond hotspot engineering in this tutorial review and focus on emerging material design strategies to capture and confine analytes near SERS-active surfaces as well as various promising hybrid SERS platforms. We outline five major approaches to enhance SERS performance: (1) enlarging Raman scattering cross-sections of non-resonant molecules via chemical coupling reactions; (2) targeted chemical capturing of analytes through surface-grafted agents to localize them on plasmonic surfaces; (3) physically confining liquid analytes on non-wetting SERS-active surfaces and (4) confining gaseous analytes using porous materials over SERS hotspots; (5) synergizing conventional metal-based SERS platforms with functional materials such as graphene, semiconducting materials, and piezoelectric polymers. These approaches can be integrated with engineered hotspots as a multifaceted strategy to further boost SERS sensitivities that are unachievable using hotspot engineering alone. Finally, we highlight current challenges in this research area and suggest new research directions towards efficient SERS designs critical for real-world applications.
关键词： non-wetting surfaces,porous materials,Surface-enhanced Raman scattering,SERS,plasmonic surfaces,chemical coupling,hotspot engineering,semiconductors,piezoelectric polymers,analyte manipulation,hybrid materials,graphene
更新于2025-09-04 15:30:14