Jingyi Luan

Plasmonic Biofoam: A Versatile Optically Active Material

Owing to their ability to confine and manipulate light at the nanoscale, plasmonic nanostructures are highly attractive for a broad range of applications. While tremendous progress has been made in the synthesis of size- and shape-controlled plasmonic nanostructures, their integration with other materials and application in solid-state is primarily through their assembly on rigid two-dimensional (2D) substrates, which limits the plasmonically active space to a few nanometers above the substrate. In this work, we demonstrate a simple method to create plasmonically active three-dimensional biofoams by integrating plasmonic nanostructures with highly porous biomaterial aerogels. We demonstrate that plasmonic biofoam is a versatile optically active platform that can be harnessed for numerous applications including (i) ultrasensitive chemical detection using surface-enhanced Raman scattering; (ii) highly efficient energy harvesting and steam generation through plasmonic photothermal heating; and (iii) optical control of enzymatic activity by triggered release of biomolecules encapsulated within the aerogel. Our results demonstrate that 3D plasmonic biofoam exhibits significantly higher sensing, photothermal, and loading efficiency compared to conventional 2D counterparts. The design principles and processing methodology of plasmonic aerogels demonstrated here can be broadly applied in the fabrication of other functional foams.

Metal-Organic Framework as a Protective Coating for Biodiagnostic Chips

Zeolitic imidazolate framework-8 (ZIF-8) grown around antibodies anchored to plasmonic nanostructures serves as a protective layer to preserve the biorecognition ability of antibodies stored at room and elevated temperatures for several days. The biofunctionality of the ZIF-8-protected biochip can be restored by a simple water-rinsing step, making it highly convenient for use in point-of-care and resource-limited settings.

PEGylated Artificial Antibodies: Plasmonic Biosensors with Improved Selectivity.

Molecular imprinting, which involves the formation of artificial recognition elements or cavities with complementary shape and chemical functionality to the target species, is a powerful method to overcome a number of limitations associated with natural antibodies. An important but often overlooked consideration in the design of artificial biorecognition elements based on molecular imprinting is the nonspecific binding of interfering species to noncavity regions of the imprinted polymer. Here, we demonstrate a universal method, namely, PEGylation of the noncavity regions of the imprinted polymer, to minimize the nonspecific binding and significantly enhance the selectivity of the molecular imprinted polymer for the target biomolecules. The nonspecific binding, as quantified by the localized surface plasmon resonance shift of imprinted plasmonic nanorattles upon exposure to common interfering proteins, was found to be more than 10 times lower compared to the non-PEGylated counterparts. The method demonstrated here can be broadly applied to a wide variety of functional monomers employed for molecular imprinting. The significantly higher selectivity of PEGylated molecular imprints takes biosensors based on these artificial biorecognition elements closer to real-world applications.

Add-on plasmonic patch as a universal fluorescence enhancer

Fluorescence-based techniques are the cornerstone of modern biomedical optics, with applications ranging from bioimaging at various scales (organelle to organism) to detection and quantification of a wide variety of biological species of interest. However, the weakness of the fluorescence signal remains a persistent challenge in meeting the ever-increasing demand to image, detect, and quantify biological species with low abundance. Here, we report a simple and universal method based on a flexible and conformal elastomeric film with adsorbed plasmonic nanostructures, which we term a “plasmonic patch,” that provides large (up to 100-fold) and uniform fluorescence enhancement on a variety of surfaces through simple transfer of the plasmonic patch to the surface. We demonstrate the applications of the plasmonic patch in improving the sensitivity and limit of detection (by more than 100 times) of fluorescence-based immunoassays implemented in microtiter plates and in microarray format. The novel fluorescence enhancement approach presented here represents a disease, biomarker, and application agnostic ubiquitously applicable fundamental and enabling technology to immediately improve the sensitivity of existing analytical methodologies in an easy-to-handle and cost-effective manner, without changing the original procedures of the existing techniques.Fluorescence: Stick-on patch fixes weak bio-signalsAdding a stretchy, nanoparticle-embedded elastomer onto standard fluorescence-based immunoassays raises biomarker signal intensities by two orders of magnitude. Nanomaterials such as gold nanorods have strong surface electromagnetic fields that can couple to the emission of a biomolecule’s fluorescent labels and enhance them, but only at certain distances apart. Srikanth Singamaneni, Rajesh Naik, and co-workers at the Washington University in St. Louis, U.S.A. have now put these nanoparticles into thin polydimethylsiloxane sheet to achieve optimal, atom-level contact for plasmonic enhancement on a variety of substrates. Because the patch is attached to immunoassays after analytical steps including antigen capture and fluorescent labeling have occurred, it avoids interfering with well-established technology. As an example, the team showed that biomarkers for kidney injury and disease could be detected at exceptionally low femtogram concentrations in urine samples.

Photothermally Active Reduced Graphene Oxide/Bacterial Nanocellulose Composites as Biofouling-Resistant Ultrafiltration Membranes

Biofouling poses one of the most serious challenges to membrane technologies by severely decreasing water flux and driving up operational costs. Here, we introduce a novel anti-biofouling ultrafiltration membrane based on reduced graphene oxide (RGO) and bacterial nanocellulose (BNC), which incoporates GO flakes into BNC in situ during its growth. In contrast to previously reported GO-based membranes for water treatment, the RGO/BNC membrane exhibited excellent aqueous stability under environmentally relevant pH conditions, vigorous mechanical agitation/sonication, and even high pressure. Importantly, due to its excellent photothermal property, under light illumination, the membrane exhibited effective bactericidal activity, obviating the need for any treatment of the feedwater or external energy. The novel design and in situ incorporation of the membranes developed in this study present a proof-of-concept for realizing new, highly efficient, and environmental-friendly anti-biofouling membranes for water purification.

Environmental Stability of Plasmonic Biosensors Based on Natural versus Artificial Antibody

Plasmonic biosensors based on the refractive index sensitivity of localized surface plasmon resonance (LSPR) are considered to be highly promising for on-chip and point-of-care biodiagnostics. However, most of the current plasmonic biosensors employ natural antibodies as biorecognition elements, which can easily lose their biorecognition ability upon exposure to environmental stressors (e.g., temperature and humidity). Plasmonic biosensors relying on molecular imprints as recognition elements (artificial antibodies) are hypothesized to be an attractive alternative for applications in resource-limited settings due to their excellent thermal, chemical, and environmental stability. In this work, we provide a comprehensive comparison of the stability of plasmonic biosensors based on natural and artificial antibodies. Although the natural antibody-based plasmonic biosensors exhibit superior sensitivity, their stability (temporal, thermal, and chemical) was found to be vastly inferior to those based on artificial antibodies. Our results convincingly demonstrate that these novel classes of artificial antibody-based plasmonic biosensors are highly attractive for point-of-care and resource-limited conditions where tight control over transport, storage, and handling conditions is not possible.